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Author | Imran, M.; Ramade, J.; Di Stasio, F.; De Franco, M.; Buha, J.; Van Aert, S.; Goldoni, L.; Lauciello, S.; Prato, M.; Infante, I.; Bals, S.; Manna, L. | ||||
Title | Alloy CsCdxPb1–xBr3Perovskite Nanocrystals: The Role of Surface Passivation in Preserving Composition and Blue Emission | Type | A1 Journal article | ||
Year | 2020 | Publication ![]() |
Chemistry Of Materials | Abbreviated Journal | Chem Mater |
Volume | 32 | Issue | Pages | acs.chemmater.0c03825 | |
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
Abstract | Various strategies have been proposed to engineer the band gap of metal halide perovskite nanocrystals (NCs) while preserving their structure and composition and thus ensuring spectral stability of the emission color. An aspect that has only been marginally investigated is how the type of surface passivation influences the structural/color stability of AMX3 perovskite NCs composed of two different M2+ cations. Here, we report the synthesis of blue-emitting Cs-oleate capped CsCdxPb1–xBr3 NCs, which exhibit a cubic perovskite phase containing Cd-rich domains of Ruddlesden–Popper phases (RP phases). The RP domains spontaneously transform into pure orthorhombic perovskite ones upon NC aging, and the emission color of the NCs shifts from blue to green over days. On the other hand, postsynthesis ligand exchange with various Cs-carboxylate or ammonium bromide salts, right after NC synthesis, provides monocrystalline NCs with cubic phase, highlighting the metastability of RP domains. When NCs are treated with Cs-carboxylates (including Cs-oleate), most of the Cd2+ ions are expelled from NCs upon aging, and the NCs phase evolves from cubic to orthorhombic and their emission color changes from blue to green. Instead, when NCs are coated with ammonium bromides, the loss of Cd2+ ions is suppressed and the NCs tend to retain their blue emission (both in colloidal dispersions and in electroluminescent devices), as well as their cubic phase, over time. The improved compositional and structural stability in the latter cases is ascribed to the saturation of surface vacancies, which may act as channels for the expulsion of Cd2+ ions from NCs. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | 000603288800034 | Publication Date | 2020-12-04 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0897-4756 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 8.6 | Times cited | 44 | Open Access | OpenAccess |
Notes | European Commission; Fonds Wetenschappelijk Onderzoek, G.0267.18N ; H2020 European Research Council, 770887 815128 851794 ; We acknowledge funding from the FLAG-ERA JTC2019 project PeroGas. S.B., and S.V.A. acknowledges funding from the European Research Council under the European Union’s Horizon 2020 research and innovation program (ERC Consolidator Grants #815128REALNANO and #770887PICOMETRICS) and from the Research Foundation Flanders (FWO, Belgium) through project funding G.0267.18N. F.D.S. acknowledges the funding from ERC starting grant NANOLED (851794). The computational work was carried out on the Dutch National e-infrastructure with the support of the SURF Cooperative; sygma | Approved | Most recent IF: 8.6; 2020 IF: 9.466 | ||
Call Number | EMAT @ emat @c:irua:174004 | Serial | 6659 | ||
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Author | Xia, C.; Pedrazo-Tardajos, A.; Wang, D.; Meeldijk, J.D.; Gerritsen, H.C.; Bals, S.; de Donega, C.M. | ||||
Title | Seeded growth combined with cation exchange for the synthesis of anisotropic Cu2-xS/ZnS, Cu2-xS, and CuInS2 nanorods | Type | A1 Journal article | ||
Year | 2021 | Publication ![]() |
Chemistry of materials | Abbreviated Journal | |
Volume | 33 | Issue | 1 | Pages | 102-116 |
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
Abstract | Colloidal copper(I) sulfide (Cu2-xS) nanocrystals (NCs) have attracted much attention for a wide range of applications because of their unique optoelectronic properties, driving scientists to explore the potential of using Cu2-xS NCs as seeds in the synthesis of heteronanocrystals to achieve new multifunctional materials. Herein, we developed a multistep synthesis strategy toward Cu2-xS/ZnS heteronanorods. The Janus-type Cu2-xS/ZnS heteronanorods are obtained by the injection of hexagonal high-chalcocite Cu2-xS seed NCs in a hot zinc oleate solution in the presence of suitable surfactants, 20 s after the injection of sulfur precursors. The Cu2-xS seed NCs undergo rapid aggregation and coalescence in the first few seconds after the injection, forming larger NCs that act as the effective seeds for heteronucleation and growth of ZnS. The ZnS heteronucleation occurs on a single (100) facet of the Cu2-xS seed NCs and is followed by fast anisotropic growth along a direction that is perpendicular to the c-axis, thus leading to Cu2-xS/ZnS Janus-type heteronanorods with a sharp heterointerface. Interestingly, the high-chalcocite crystal structure of the injected Cu2-xS seed NCs is preserved in the Cu2-xS segments of the heteronanorods because of the highthermodynamic stability of this Cu2-xS phase. The Cu2-xS/ZnS heteronanorods are subsequently converted into single-component Cu2-xS and CuInS2 nanorods by postsynthetic topotactic cation exchange. This work expands the possibilities for the rational synthesis of colloidal multicomponent heteronanorods by allowing the design principles of postsynthetic heteroepitaxial seeded growth and nanoscale cation exchange to be combined, yielding access to a plethora of multicomponent heteronanorods with diameters in the quantum confinement regime. | ||||
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Corporate Author | Thesis | ||||
Publisher | Place of Publication | Editor | |||
Language | Wos | 000610984700009 | Publication Date | 2020-12-28 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | ||
Impact Factor | Times cited | 10 | Open Access | OpenAccess | |
Notes | C.X. acknowledges China Scholarship Council (CSC) for the financial support (grant number 201406330055). C.d.M.D. acknowledges funding from the European Commission for access to the EMAT facilities (grant number EUSMI E180900184). D.W. acknowledges an Individual Fellowship funded by the Marie Sklodowska-Curie Actions (MSCA) in Horizon 2020 program (grant 894254 SuprAtom). S.B. acknowledges support by means of the ERC Consolidator grant no. 815128 REALNANO. The authors thank Donglong Fu for XRD measurements.; sygma | Approved | Most recent IF: NA | ||
Call Number | UA @ admin @ c:irua:176587 | Serial | 6732 | ||
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Author | Feng, H.L.; Kang, C.-J.; Manuel, P.; Orlandi, F.; Su, Y.; Chen, J.; Tsujimoto, Y.; Hadermann, J.; Kotliar, G.; Yamaura, K.; McCabe, E.E.; Greenblatt, M. | ||||
Title | Antiferromagnetic order breaks inversion symmetry in a metallic double perovskite, Pb₂NiOsO₆ | Type | A1 Journal article | ||
Year | 2021 | Publication ![]() |
Chemistry Of Materials | Abbreviated Journal | Chem Mater |
Volume | 33 | Issue | 11 | Pages | 4188-4195 |
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
Abstract | A polycrystalline sample of Pb2NiOsO6 was synthesized under high-pressure (6 GPa) and high-temperature (1575 K) conditions. Pb2NiOsO6 crystallizes in a monoclinic double perovskite structure with a centrosymmetric space group P2(1)/n at room temperature. Pb2NiOsO6 is metallic down to 2 K and shows a single antiferromagnetic (AFM) transition at T-N = 58 K. Pb2NiOsO6 is a new example of a metallic and AFM oxide with three-dimensional connectivity. Neutron powder diffraction and first-principles calculation studies indicate that both Ni and Os moments are ordered below T-N and the AFM magnetic order breaks inversion symmetry. This loss of inversion symmetry driven by AFM order is unusual in metallic systems, and the 3d-Sd double-perovskite oxides represent a new class of noncentrosymmetric AFM metallic oxides. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | 000661521800032 | Publication Date | 2021-05-26 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0897-4756; 1520-5002 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 9.466 | Times cited | Open Access | OpenAccess | |
Notes | Approved | Most recent IF: 9.466 | |||
Call Number | UA @ admin @ c:irua:179679 | Serial | 6854 | ||
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Author | Li, W.; Tong, W.; Yadav, A.; Bladt, E.; Bals, S.; Funston, A.M.; Etheridge, J. | ||||
Title | Shape control beyond the seeds in gold nanoparticles | Type | A1 Journal article | ||
Year | 2021 | Publication ![]() |
Chemistry Of Materials | Abbreviated Journal | Chem Mater |
Volume | 33 | Issue | 23 | Pages | 9152-9164 |
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
Abstract | In typical seed-mediated syntheses of metal nanocrystals, the shape of the nanocrystal is determined largely by the seed nucleation environment and subsequent growth environment (where “environment” refers to the chemical environment, including the surfactant and additives). In this approach, crystallinity is typically determined by the seeds, and surfaces are controlled by the environment(s). However, surface energies, and crystallinity, are both influenced by the choice of environment(s). This limits the permutations of crystallinity and surface facets that can be mixed and matched to generate new nanocrystal morphologies. Here, we control post-seed growth to deliberately incorporate twin planes during the growth stage to deliver new final morphologies, including twinned cubes and bipyramids from single-crystal seeds. The nature and number of twin planes, together with surfactant control of facet growth, define the final nanoparticle morphology. Moreover, by breaking symmetry, the twin planes introduce new facet orientations. This additional mechanism opens new routes for the synthesis of different morphologies and facet orientations. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | 000753956100012 | Publication Date | 0000-00-00 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0897-4756; 1520-5002 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 9.466 | Times cited | 3 | Open Access | Not_Open_Access |
Notes | This work was supported by the Australian Research Council (ARC) Grants DP160104679 and CE170100026 and used microscopes at the Monash Centre for Electron Microscopy funded by ARC Grants LE0454166, LE110100223, and LE140100104. W.L. thanks the support of the Australian Government Research Training Program (RTP) scholarship. W.T. thanks the Australian Department of Education and Monash University for the IPRS and APA scholarships. E.B. acknowledges financial support and a post-doctoral grant from the Research Foundation Flanders (FWO, Belgium). The authors thank Dr. Matthew Weyland and Dr. Tim Peterson for helpful discussions. A.Y. thanks the support from Post Graduation Publication Award (PPA) scholarship from Monash University. | Approved | Most recent IF: 9.466 | ||
Call Number | UA @ admin @ c:irua:187229 | Serial | 7065 | ||
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Author | Hao, Y.; Velpula, G.; Kaltenegger, M.; Bodlos, W.R.; Vibert, F.; Mali, K.S.; De Feyter, S.; Resel, R.; Geerts, Y.H.; Van Aert, S.; Beljonne, D.; Lazzaroni, R. | ||||
Title | From 2D to 3D : bridging self-assembled monolayers to a substrate-induced polymorph in a molecular semiconductor | Type | A1 Journal article | ||
Year | 2022 | Publication ![]() |
Chemistry of materials | Abbreviated Journal | Chem Mater |
Volume | 34 | Issue | 5 | Pages | 2238-2248 |
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
Abstract | In this study, a new bottom-up approach is proposed to predict the crystal structure of the substrate-induced polymorph (SIP) of an archetypal molecular semiconductor. In spite of intense efforts, the formation mechanism of SIPs is still not fully understood, and predicting their crystal structure is a very delicate task. Here, we selected lead phthalocyanine (PbPc) as a prototypical molecular material because it is a highly symmetrical yet nonplanar molecule and we demonstrate that the growth and crystal structure of the PbPc SIPs can be templated by the corresponding physisorbed self-assembled molecular networks (SAMNs). Starting from SAMNs of PbPc formed at the solution/graphite interface, the structural and energetic aspects of the assembly were studied by a combination of in situ scanning tunneling microscopy and multiscale computational chemistry approach. Then, the growth of a PbPc SIP on top of the physisorbed monolayer was modeled without prior experimental knowledge, from which the crystal structure of the SIP was predicted. The theoretical prediction of the SIP was verified by determining the crystal structure of PbPc thin films using X-ray diffraction techniques, revealing the formation of a new polymorph of PbPc on the graphite substrate. This study clearly illustrates the correlation between the SAMNs and SIPs, which are traditionally considered as two separate but conceptually connected research areas. This approach is applicable to molecular materials in general to predict the crystal structure of their SIPs. | ||||
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Corporate Author | Thesis | ||||
Publisher | Place of Publication | Editor | |||
Language | Wos | 000812125800001 | Publication Date | 2022-02-17 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0897-4756; 1520-5002 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 8.6 | Times cited | Open Access | Not_Open_Access | |
Notes | Approved | Most recent IF: 8.6 | |||
Call Number | UA @ admin @ c:irua:189086 | Serial | 7084 | ||
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Author | van der Sluijs, M.M.; Salzmann, B.B.V.; Arenas Esteban, D.; Li, C.; Jannis, D.; Brafine, L.C.; Laning, T.D.; Reinders, J.W.C.; Hijmans, N.S.A.; Moes, J.R.; Verbeeck, J.; Bals, S.; Vanmaekelbergh, D. | ||||
Title | Study of the Mechanism and Increasing Crystallinity in the Self-Templated Growth of Ultrathin PbS Nanosheets | Type | A1 Journal article | ||
Year | 2023 | Publication ![]() |
Chemistry of materials | Abbreviated Journal | |
Volume | Issue | Pages | |||
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
Abstract | Colloidal 2D semiconductor nanocrystals, the analogue of solid-state quantum wells, have attracted strong interest in material science and physics. Molar quantities of suspended quantum objects with spectrally pure absorption and emission can be synthesized. For the visible region, CdSe nanoplatelets with atomically precise thickness and tailorable emission have been (almost) perfected. For the near-infrared region, PbS nanosheets (NSs) hold strong promise, but the photoluminescence quantum yield is low and many questions on the crystallinity, atomic structure, intriguing rectangular shape, and formation mechanism remain to be answered. Here, we report on a detailed investigation of the PbS NSs prepared with a lead thiocyanate single source precursor. Atomically resolved HAADF-STEM imaging reveals the presence of defects and small cubic domains in the deformed orthorhombic PbS crystal lattice. Moreover, variations in thickness are observed in the NSs, but only in steps of 2 PbS monolayers. To study the reaction mechanism, a synthesis at a lower temperature allowed for the study of reaction intermediates. Specifically, we studied the evolution of pseudo-crystalline templates towards mature, crystalline PbS NSs. We propose a self-induced templating mechanism based on an oleylamine-lead-thiocyanate (OLAM-Pb-SCN) complex with two Pb-SCN units as a building block; the interactions between the long-chain ligands regulate the crystal structure and possibly the lateral dimensions. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | 000959572100001 | Publication Date | 2023-03-25 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0897-4756 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 8.6 | Times cited | 2 | Open Access | OpenAccess |
Notes | H2020 Research Infrastructures, 731019 ; H2020 European Research Council, 692691 815128 ; Nederlandse Organisatie voor Wetenschappelijk Onderzoek, 715.016.002 ; | Approved | Most recent IF: 8.6; 2023 IF: 9.466 | ||
Call Number | EMAT @ emat @c:irua:195894 | Serial | 7255 | ||
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Author | Zankowski, S.P.; Van Hoecke, L.; Mattelaer, F.; de Raedt, M.; Richard, O.; Detavernier, C.; Vereecken, P.M. | ||||
Title | Redox layer deposition of thin films of MnO2 on nanostructured substrates from aqueous solutions | Type | A1 Journal article | ||
Year | 2019 | Publication ![]() |
Chemistry of materials | Abbreviated Journal | |
Volume | 31 | Issue | 13 | Pages | 4805-4816 |
Keywords | A1 Journal article; Sustainable Energy, Air and Water Technology (DuEL) | ||||
Abstract | In this work, we report a new method for depositing thin films of MnO2 on planar and complex nanostructured surfaces, with high precision and conformality. The method is based on repeating cycles of adsorption of an unsaturated alcohol on a surface, followed by its oxidation with aqueous KMnO4 and formation of thin, solid MnO2. The amount of manganese oxide formed in each cycle is limited by the quantity of the adsorbed alcohol; thus, the growth exhibits the self-limiting characteristics of atomic layer deposition (ALD). Contrary to the typical ALD, however, the new redox layer deposition is performed in air, at room temperature, using common chemicals and simple laboratory glassware, which greatly reduces its cost and complexity. We also demonstrate application of the method for the fabrication of a nanostructured MnO2/Ni electrode, which was not possible with thermal ALD because of the rapid decomposition of the gaseous precursor on the high surface-area substrate. Thanks to its simplicity, the conformal deposition of MnO2 can be easily upscaled and thus exploited for its numerous (electro)chemical applications. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | 000475408400021 | Publication Date | 2019-06-12 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0897-4756; 1520-5002 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | Times cited | Open Access | |||
Notes | Approved | no | |||
Call Number | UA @ admin @ c:irua:161225 | Serial | 8465 | ||
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Author | Sa, J.; Hu, N.; Heyvaert, W.; Van Gordon, K.; Li, H.; Wang, L.; Bals, S.; Liz-Marzán, L.M.; Ni, W. | ||||
Title | Spontaneous Chirality Evolved at the Au–Ag Interface in Plasmonic Nanorods | Type | A1 Journal article | ||
Year | 2023 | Publication ![]() |
Chemistry of materials | Abbreviated Journal | Chem. Mater. |
Volume | Issue | Pages | |||
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
Abstract | Chiral ligands are considered a required ingredient during the synthesis of dissymmetric plasmonic metal nanocrystals. The mechanism behind the generation of chiral structures involves the formation of high Miller index chiral facets, induced by the adsorption of such chiral ligands. We found however that, chirality can also evolve spontaneously, without the involvement of any chiral ligands, during the co-deposition of Au and Ag on Au nanorods. When using a specific Au/Ag ratio, phase segregation of the two metals leads to an interface within the obtained AuAg shell, which can be exposed by removing the Ag component via oxidative etching. Although a close-to-racemic mixture of chiral Au nanorods with right and left handedness is found in solution, electron tomography analysis evidences left- and righthanded helicities, both at the Au-Ag interface and at the exposed surface of Au NRs after Ag etching. The helicity profile of the NRs indicates dominating inclination angles in a range from 30° to 60°. Single-particle optical characterization also reveals random handedness in the plasmonic response of individual nanorods. We hypothesize that, the origin of chirality is related with symmetry breaking during the co-deposition of Au and Ag, through an initial perturbation in a small region on the Au-Ag interface that eventually leads to chiral segregation throughout the nanocrystal. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | 001052093300001 | Publication Date | 2023-08-21 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0897-4756 | ISBN | Additional Links | UA library record; WoS full record | |
Impact Factor | 8.6 | Times cited | Open Access | OpenAccess | |
Notes | The authors acknowledge the financial support from the National Natural Science Foundation of China (grant 22074102). LMLM acknowledges funding from 26 MCIN/AEI/10.13039/501100011033 and “ESF Investing in your future” (Grant PID2020- 117779RB-I00). This project has received funding from the European Union’s Horizon 2020 research and innovation programme under grant agreement No 823717 – ESTEEM3.; Ministerio de Ciencia e Innovaci?n, PID2020-117779RB-I00 ; H2020 Research Infrastructures, 823717 ; European Social Fund, PID2020-117779RB-I00 ; National Natural Science Foundation of China, 22074102 ; | Approved | Most recent IF: 8.6; 2023 IF: 9.466 | ||
Call Number | EMAT @ emat @c:irua:198151 | Serial | 8810 | ||
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Author | Mulder, J.T.T.; Jenkinson, K.; Toso, S.; Prato, M.; Evers, W.H.H.; Bals, S.; Manna, L.; Houtepen, A.J.J. | ||||
Title | Nucleation and growth of bipyramidal Yb:LiYF₄ nanocrystals : growing up in a hot environment | Type | A1 Journal article | ||
Year | 2023 | Publication ![]() |
Chemistry of materials | Abbreviated Journal | |
Volume | 35 | Issue | 14 | Pages | 5311-5321 |
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
Abstract | Lanthanide-doped LiYF4 (Ln:YLF) is commonlyused fora broad variety of optical applications, such as lasing, photon upconversionand optical refrigeration. When synthesized as nanocrystals (NCs),this material is also of interest for biological applications andfundamental physical studies. Until now, it was unclear how Ln:YLFNCs grow from their ionic precursors into tetragonal NCs with a well-defined,bipyramidal shape and uniform dopant distribution. Here, we studythe nucleation and growth of ytterbium-doped LiYF4 (Yb:YLF),as a template for general Ln:YLF NC syntheses. We show that the formationof bipyramidal Yb:YLF NCs is a multistep process starting with theformation of amorphous Yb:YLF spheres. Over time, these spheres growvia Ostwald ripening and crystallize, resulting in bipyramidal Yb:YLFNCs. We further show that prolonged heating of the NCs results inthe degradation of the NCs, observed by the presence of large LiFcubes and small, irregular Yb:YLF NCs. Due to the similarity in chemicalnature of all lanthanide ions our work sheds light on the formationstages of Ln:YLF NCs in general. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | 001021474500001 | Publication Date | 2023-07-03 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0897-4756; 1520-5002 | ISBN | Additional Links | UA library record; WoS full record | |
Impact Factor | 8.6 | Times cited | Open Access | OpenAccess | |
Notes | This project has received funding from the European Union's Horizon 2020 research and innovation program under Grant Agreement No. 766900 (Testing the large-scale limit of quantum mechanics). The authors thank Niranjan Saikumar for proof reading the manuscript. | Approved | Most recent IF: 8.6; 2023 IF: 9.466 | ||
Call Number | UA @ admin @ c:irua:197787 | Serial | 8907 | ||
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Author | Filez, M.; Feng, J.-Y.; Minjauw, M.M.; Solano, E.; Poonkottil, N.; Van Daele, M.; Ramachandran, R.K.; Li, C.; Bals, S.; Poelman, H.; Detavernier, C.; Dendooven, J.; Filez, M.; Minjauw, M.; Solano, E.; Poonkottil, N.; Li, C.; Bals, S.; Dendooven, J. | ||||
Title | Shuffling atomic layer deposition gas sequences to modulate bimetallic thin films and nanoparticle properties | Type | A1 Journal article | ||
Year | 2022 | Publication ![]() |
Chemistry of materials | Abbreviated Journal | |
Volume | Issue | Pages | |||
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
Abstract | Atomic layer deposition (ALD) typically employs metal precursors and co-reactant pulses to deposit thin films in a layer-by-layer fashion. While conventional ABAB-type ALD sequences implement only two functionalities, namely, a metal source and ligand exchange agent, additional functionalities have emerged, including etching and reduction agents. Herein, we construct gas-phase sequences-coined as ALD+-with complex-ities reaching beyond the classic ABAB-type ALD by freely combining multiple functionalities within irregular pulse schemes, e.g., ABCADC. The possibilities of such combinations are explored as a smart strategy to tailor bimetallic thin films and nanoparticle (NP) properties. By doing so, we demonstrate that bimetallic thin films can be tailored with target thickness and through the full compositional range, while the morphology can be flexibly modulated from thin films to NPs by shuI 1ing the pulse sequence. These complex pulse schemes are expected to be broadly applicable but are here explored for Pd-Ru bimetallic thin films and NPs. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | 000823205700001 | Publication Date | 2022-06-29 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0897-4756; 1520-5002 | ISBN | Additional Links | UA library record; WoS full record | |
Impact Factor | Times cited | 2 | Open Access | OpenAccess | |
Notes | This research was funded by the Research Foundation, Flanders (FWO) , and the Special Research Fund BOF of Ghent University (GOA 01G01019) . M.F. and M.M.M. acknowledge the FWO for a postdoctoral research fellowship (1280621N) . N.P. acknowledges the European Union's Horizon 2020 research and innovation program under the Marie Skiodowska-Curie grant agreement no. 765378. For the GISAXS measurements, the author s received funding from the European Community's Transnational Access Program CALIPSOplus. E.S. acknowledges the Spanish project RTI2018-093996-B-C32 MICINN/FEDER funds. Air Liquide is acknowledged for supporting this research. The authors acknowledge SOLEIL for the provision of synchrotron radiation facilities and would like to thank Dr. Alessandro Coati for assistance in using beamline SiXS. The GIWAXS experiments were performed at NCD-SWEET beamline at ALBA Synchrotron with the collaboration of ALBA staff . | Approved | no | ||
Call Number | UA @ admin @ c:irua:189541 | Serial | 8928 | ||
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Author | Vandemeulebroucke, D.; Batuk, M.; Hajizadeh, A.; Wastiaux, M.; Roussel, P.; Hadermann, J. | ||||
Title | Incommensurate Modulations and Perovskite Growth in LaxSr2–xMnO4−δAffecting Solid Oxide Fuel Cell Conductivity | Type | A1 Journal Article | ||
Year | 2024 | Publication ![]() |
Chemistry of Materials | Abbreviated Journal | Chem. Mater. |
Volume | Issue | Pages | |||
Keywords | A1 Journal Article; Electron Microscopy for Materials Science (EMAT) ; | ||||
Abstract | Ruddlesden-Popper La????Sr2−????MnO4−???? materials are interesting symmetric solid oxide fuel cell electrodes due to their good redox stability, mixed ionic and electronic conducting behavior and thermal expansion that matches well with common electrolytes. In reducing environments – as at a solid oxide fuel cell anode – the x = 0.5 member, i.e. La0.5Sr1.5MnO4−????, has a much higher total conductivity than compounds with a different La/Sr ratio, although all those compositions have the same K2NiF4-type I4/mmm structure. The origin for this conductivity difference is not yet known in literature. Now, a combination of in-situ and ex-situ 3D electron diffraction, high-resolution imaging, energy-dispersive X-ray analysis and electron energy-loss spectroscopy uncovered clear differences between x=0.25 and x=0.5 in the pristine structure, as well as in the transformations upon high-temperature reduction. In La0.5Sr1.5MnO4−????, Ruddlesden-Popper n=2 layer defects and an amorphous surface layer are present, but not in La0.25Sr1.75MnO4−????. After annealing at 700°C in 5% H2/Ar, La0.25Sr1.75MnO4−???? transforms to a tetragonal 2D incommensurately modulated structure with modulation vectors ⃗????1 = 0.2848(1) · (⃗????* +⃗????*) and ⃗????2 =0.2848(1) · (⃗????* – ⃗????*), whereas La0.5Sr1.5MnO4−???? only partially transforms to an orthorhombic 1D incommensurately modulated structure, with ⃗???? = 0.318(2) · ⃗????*. Perovskite domains grow at the crystal edge at 700°C in 5% H2 or vacuum, due to the higher La concentration on the surface compared to the bulk, which leads to a different thermodynamic equilibrium. Since it is known that a lower degree of oxygen vacancy ordering and a higher amount of perovskite blocks enhance oxygen mobility, those differences in defect structure and structural transformation upon reduction, might all contribute to the higher conductivity of La0.5Sr1.5MnO4−???? in solid oxide fuel cell anode conditions compared to other La/Sr ratios. |
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Address | |||||
Corporate Author | Thesis | ||||
Publisher | Place of Publication | Editor | |||
Language | English | Wos | 001174840900001 | Publication Date | 2024-02-20 |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0897-4756 | ISBN | Additional Links | UA library record; WoS full record | |
Impact Factor | 8.6 | Times cited | Open Access | Not_Open_Access | |
Notes | Universiteit Antwerpen, BOF TOP 38689 ; Fonds Wetenschappelijk Onderzoek, I003218N ; European Commission NanED, 956099 ; | Approved | Most recent IF: 8.6; 2024 IF: 9.466 | ||
Call Number | EMAT @ emat @c:irua:204354 | Serial | 8997 | ||
Permanent link to this record | |||||
Author | Mayda, S.; Monico, L.; Krishnan, D.; De Meyer, S.; Cotte, M.; Garrevoet, J.; Falkenberg, G.; Sandu, I.C.A.; Partoens, B.; Lamoen, D.; Romani, A.; Miliani, C.; Verbeeck, J.; Janssens, K. | ||||
Title | A combined experimental and computational approach to understanding CdS pigment oxidation in a renowned early 20th century painting | Type | A1 Journal article | ||
Year | 2023 | Publication ![]() |
Chemistry of materials | Abbreviated Journal | |
Volume | 35 | Issue | 24 | Pages | 10403-10415 |
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT); Condensed Matter Theory (CMT); Antwerp X-ray Imaging and Spectroscopy (AXIS) | ||||
Abstract | Cadmium sulfide (CdS)-based yellow pigments have been used in a number of early 20th century artworks, including The Scream series painted by Edvard Munch. Some of these unique paintings are threatened by the discoloration of these CdS-based yellow oil paints because of the oxidation of the original sulfides to sulfates. The experimental data obtained here prove that moisture and cadmium chloride compounds play a key role in promoting such oxidation. To clarify how these two factors effectively prompt the process, we studied the band alignment between CdS, CdCl2, and Cd-(OH)Cl as well as the radicals center dot OH and H3O center dot by density functional theory (DFT) methods. Our results show that a stack of several layers of Cd-(OH)Cl creates a pocket of positive holes at the Cl-terminated surface and a pocket of electrons at the OH-terminated surface by leading in a difference in ionization energy at both surfaces. The resulting band alignment indicates that Cd-(OH)Cl can indeed play the role of an oxidative catalyst for CdS in a moist environment, thus providing an explanation for the experimental evidence. | ||||
Address | |||||
Corporate Author | Thesis | ||||
Publisher | Place of Publication | Editor | |||
Language | Wos | 001133000900001 | Publication Date | 2023-12-08 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0897-4756; 1520-5002 | ISBN | Additional Links | UA library record; WoS full record | |
Impact Factor | 8.6 | Times cited | Open Access | ||
Notes | The experimental research on the cadmium yellow powders/paint mock-ups and The Scream (ca. 1910) was financially supported by the European Union, research projects IPERION-CH (H2020-INFRAIA-2014-2015, GA no. 654028) and IPERION-HS (H2020-INFRAIA-2019-1, GA no. 871034) and the project AMIS within the program Dipartimenti di Eccellenza 2018-2022 (funded by MUR and the University of Perugia). For the beamtime grants received, the authors thank the ESRF-ID21 beamline (experiments HG64 and HG95), the DESY-P06 beamline, a member of the Helmholtz Association HGF (experiments I-20130221 EC and I-20160126 EC), and the project CALIPSOplus under the GA no. 730872 from the E.U. Framework Programme for Research and Innovation Horizon 2020. All of the staff of the MUNCH Museum (Conservation Department) is acknowledged for their collaboration. The computational resources and services used in this work were provided by the VSC (Flemish Supercomputer Center) and the HPC infrastructure of the University of Antwerp (CalcUA), both funded by the FWO – Vlaanderen and the Flemish Government, Department EWI. | Approved | Most recent IF: 8.6; 2023 IF: 9.466 | ||
Call Number | UA @ admin @ c:irua:202836 | Serial | 8999 | ||
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Author | Shevchenko, V.A.; Glazkova, I.S.; Novichkov, D.A.; Skvortsova, I.; V. Sobolev, A.; Abakumov, A.M.; Presniakov, I.A.; Drozhzhin, O.A.; V. Antipov, E. | ||||
Title | Competition between the Ni and Fe redox in the O3-NaNi1/3Fe1/3Mn1/3O2 cathode material for Na-ion batteries | Type | A1 Journal article | ||
Year | 2023 | Publication ![]() |
Chemistry of materials | Abbreviated Journal | |
Volume | 35 | Issue | 10 | Pages | 4015-4025 |
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
Abstract | Sodium-ion batteries are attracting great attention due to their low cost and abundance of sodium. The O3-type NaNi1/3Fe1/3Mn1/3O2 layered oxide material is a promising candidate for positive electrodes (cathodes) in Na-ion batteries. However, its stable electrochemical performance is restricted by the upper voltage limit of 4.0 V (vs Na/Na+), which allows for reversibly removing 0.5-0.55 Na+ per formula unit, corresponding to the capacity of 120-130 mAh.g(-1). Further reduction of sodium content inevitably accelerates capacity degradation, and this issue calls for a detailed study of the redox reactions that accompany the electrochemical (de)intercalation of a large amount of sodium. Here, we present operando and ex situ studies using powder X-ray diffraction and X-ray absorption spectroscopy combined with Fe-57 Mossbauer spectroscopy. Our approach reveals the sequence of the redox transitions that occur during the charge and discharge of O3-NaNi1/3Fe1/3Mn1/3O2. Our data show that in addition to nickel and iron cations oxidizing to M+4, a part of iron transforms into the “3 + delta” state owing to the fast electron exchange Fe3+ + Fe4+ <-> Fe4+ + Fe3+. This process freezes upon cooling the material to 35 K, producing Fe4+ cations, some of which occupy tetrahedral positions. | ||||
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Corporate Author | Thesis | ||||
Publisher | Place of Publication | Editor | |||
Language | Wos | 000985970200001 | Publication Date | 2023-05-04 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0897-4756; 1520-5002 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 8.6 | Times cited | Open Access | ||
Notes | Approved | Most recent IF: 8.6; 2023 IF: 9.466 | |||
Call Number | UA @ admin @ c:irua:197352 | Serial | 9013 | ||
Permanent link to this record | |||||
Author | Hervieu, M.; Martin, C.; Maignan, A.; Van Tendeloo, G.; Jirak, Z.; Hejtmanek, J.; Barnabe, A.; Thopart, D.; Raveau, B. | ||||
Title | Structural and magnetotransport transitions in the electron-doped Pr1-xSrxMnO3(0.85\leq x\leq1) manganites | Type | A1 Journal article | ||
Year | 2000 | Publication ![]() |
Chemistry and materials | Abbreviated Journal | Chem Mater |
Volume | 12 | Issue | 5 | Pages | 1456-1462 |
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
Abstract | The exploration of the Mn4+-rich side of the Pr1-xSrxMnO3 system has allowed the extension of the domain of the cubic perovskite, by using a two-step process, combining synthesis under Ar flow at high temperature and O-2 pressure annealing at lower temperature. We show that these Pr-doped cubic perovskites exhibit a coupled structural (cubic-tetragonal) and magnetic (para-antiferro) transition connected with a resistivity jump at the same temperature. The strong interplay between lattice, charges, and spins for these oxides results from the appearance at low temperature of the distorted C-type antiferromagnetic structure. The Pr1-xSrxMnO3 magnetic phase diagram shows, for 0.9 less than or equal to x less than or equal to 1 (i.e., on the Mn4+-rich side), the existence at low temperature of C- and G-type antiferromagnetism. The absence of ferromagnetic-antiferromagnetic competition explains that magnetoresistante properties are not observed in this system, in contrast to Mn4+-rich Ln(1-x)Ca(x)MnO(3) systems. | ||||
Address | |||||
Corporate Author | Thesis | ||||
Publisher | Place of Publication | Washington, D.C. | Editor | ||
Language | Wos | 000087136800039 | Publication Date | 2002-07-26 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0897-4756;1520-5002; | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 9.466 | Times cited | 24 | Open Access | |
Notes | Approved | Most recent IF: 9.466; 2000 IF: 3.580 | |||
Call Number | UA @ lucian @ c:irua:103454 | Serial | 3198 | ||
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Author | Rossell, M.D.; Abakumov, A.M.; Van Tendeloo, G.; Pardo, J.A.; Santiso, J. | ||||
Title | Structure and microstructure of epitaxial Sr4Fe6O13-\delta films on SrTiO3 | Type | A1 Journal article | ||
Year | 2004 | Publication ![]() |
Chemistry and materials | Abbreviated Journal | Chem Mater |
Volume | 16 | Issue | Pages | 2578-2584 | |
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
Abstract | The crystal structure and the microstructure of epitaxial Sr4Fe6O13+/-delta thin films grown on a single-crystal SrTiO3 substrate by PLD have been investigated. A combination of electron diffraction and high-resolution microscopy allows us to refine the structure and to identify an incommensurate modulation in the Sr4Fe6O13+/-delta films. The incommensurate structure (q = alphaa(m)* approximate to 0.39alpha(m)*, superspace group Xmmm(alpha00)0s0) can be interpreted as an oxygen-deficient modification in the Fe2O2.5 double layers. Moreover, it is shown that the experimentally determined a component of the modulation can be used consistently to estimate the local oxygen content in the Sr4Fe6O13+/-delta films. The compound composition can therefore be described as Sr4Fe6O12+2alpha and the value alpha = 0.39 corresponds to a Sr4Fe6O12.78 composition. The misfit stress along the Sr4Fe6O13+/-delta/SrTiO3 interface is accommodated via both elastic deformation and inelastic mechanisms (misfit dislocations and 90degrees rotation twins). The present results also suggest the existence of SrFeO3 perovskite in the Sr4Fe6O13+/-delta films. | ||||
Address | |||||
Corporate Author | Thesis | ||||
Publisher | Place of Publication | Washington, D.C. | Editor | ||
Language | Wos | 000222252300011 | Publication Date | 2004-06-22 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0897-4756;1520-5002; | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 9.466 | Times cited | 26 | Open Access | |
Notes | Approved | Most recent IF: 9.466; 2004 IF: 4.103 | |||
Call Number | UA @ lucian @ c:irua:54770 | Serial | 3286 | ||
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Author | Rossell, M.D.; Abakumov, A.M.; Van Tendeloo, G.; Lomakov, M.V.; Istomin, S.Y.; Antipov, E.V. | ||||
Title | Transmission electron microscopic study of the defect structure in Sr4Fe6O12+\delta compounds with variable oxygen content | Type | A1 Journal article | ||
Year | 2005 | Publication ![]() |
Chemistry and materials | Abbreviated Journal | Chem Mater |
Volume | 17 | Issue | Pages | 4717-4726 | |
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
Abstract | |||||
Address | |||||
Corporate Author | Thesis | ||||
Publisher | Place of Publication | Editor | |||
Language | Wos | 000231742600024 | Publication Date | 2005-08-30 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0897-4756;1520-5002; | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 9.466 | Times cited | 17 | Open Access | |
Notes | Approved | Most recent IF: 9.466; 2005 IF: 4.818 | |||
Call Number | UA @ lucian @ c:irua:54772 | Serial | 3703 | ||
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Author | Semenov, M.Y.; Khodzher, T.V.; Obolkin, V.A.; Domysheva, V.M.; Golobokova, L.P.; Kobeleva, N.A.; Netsvetaeva, O.G.; Potemkin, V.L.; Van Grieken, R.; Fukuzaki, N. | ||||
Title | Assessing the acidification risk in the Lake Baikal region | Type | A1 Journal article | ||
Year | 2006 | Publication ![]() |
Chemistry and ecology | Abbreviated Journal | |
Volume | 22 | Issue | 1 | Pages | 1-11 |
Keywords | A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation) | ||||
Abstract | |||||
Address | |||||
Corporate Author | Thesis | ||||
Publisher | Place of Publication | Editor | |||
Language | Wos | 000236110800001 | Publication Date | 2006-03-02 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0275-7540 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | Times cited | Open Access | |||
Notes | Approved | no | |||
Call Number | UA @ admin @ c:irua:56510 | Serial | 7496 | ||
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Author | Neyts, E.; Eckert, M.; Bogaerts, A. | ||||
Title | Molecular dynamics simulations of the growth of thin a-C:H films under additional ion bombardment: influence of the growth species and the Ar+ ion kinetic energy | Type | A1 Journal article | ||
Year | 2007 | Publication ![]() |
Chemical vapor deposition | Abbreviated Journal | Chem Vapor Depos |
Volume | 13 | Issue | 6/7 | Pages | 312-318 |
Keywords | A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | |||||
Address | |||||
Corporate Author | Thesis | ||||
Publisher | Place of Publication | Weinheim | Editor | ||
Language | Wos | 000248381800007 | Publication Date | 2007-07-10 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0948-1907;1521-3862; | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 1.333 | Times cited | 14 | Open Access | |
Notes | Approved | Most recent IF: 1.333; 2007 IF: 1.936 | |||
Call Number | UA @ lucian @ c:irua:64532 | Serial | 2176 | ||
Permanent link to this record | |||||
Author | Eckert, M.; Neyts, E.; Bogaerts, A. | ||||
Title | Molecular dynamics simulations of the sticking and etch behavior of various growth species of (ultra)nanocrystalline diamond films | Type | A1 Journal article | ||
Year | 2008 | Publication ![]() |
Chemical vapor deposition | Abbreviated Journal | Chem Vapor Depos |
Volume | 14 | Issue | 7/8 | Pages | 213-223 |
Keywords | A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | The reaction behavior of species that may affect the growth of ultrananocrystal line and nanocrystalline diamond ((U)NCD) films is investigated by means of molecular dynamics simulations. Impacts of CHx (x = 0 – 4), C2Hx (x=0-6), C3Hx (x=0-2), C4Hx (x = 0 – 2), H, and H-2 on clean and hydrogenated diamond (100)2 x 1 and (111) 1 x 1 surfaces at two different substrate temperatures are simulated. We find that the different bonding structures of the two surfaces cause different temperature effects on the sticking efficiency. These results predict a temperature-dependent ratio of diamond (100) and (111) growth. Furthermore, predictions of which are the most important hydrocarbon species for (U)NCD growth are made. | ||||
Address | |||||
Corporate Author | Thesis | ||||
Publisher | Place of Publication | Weinheim | Editor | ||
Language | Wos | 000259302700008 | Publication Date | 2008-08-18 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0948-1907;1521-3862; | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 1.333 | Times cited | 25 | Open Access | |
Notes | Approved | Most recent IF: 1.333; 2008 IF: 1.483 | |||
Call Number | UA @ lucian @ c:irua:70001 | Serial | 2177 | ||
Permanent link to this record | |||||
Author | Yan, L.; Niu, H.J.; Duong, G.V.; Suchomel, M.R.; Bacsa, J.; Chalker, P.R.; Hadermann, J.; Van Tendeloo, G.; Rosseinsky, M.J. | ||||
Title | Cation ordering within the perovskite block of a six-layer Ruddlesden-Popper oxide from layer-by-layer growth artificial interfaces in complex unit cells | Type | A1 Journal article | ||
Year | 2011 | Publication ![]() |
Chemical science | Abbreviated Journal | Chem Sci |
Volume | 2 | Issue | 2 | Pages | 261-272 |
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
Abstract | The (AO)(ABO3)n Ruddlesden-Popper structure is an archetypal complex oxide consisting of two distinct structural units, an (AO) rock salt layer separating an n-octahedra thick perovskite block. Conventional high-temperature oxide synthesis methods cannot access members with n > 3, but low-temperature layer-by-layer thin film methods allow the preparation of materials with thicker perovskite blocks, exploiting high surface mobility and lattice matching with the substrate. This paper describes the growth of an n = 6 member CaO[(CSMO)2(LCMO)2 (CSMO)2] in which the six unit cell perovskite block is sub-divided into two central La0.67Ca0.33MnO3 (LCMO) and two terminal Ca0.85Sm0.15MnO3 (CSMO) layers to allow stabilization of the rock salt layer and variation of the transition metal charge. | ||||
Address | |||||
Corporate Author | Thesis | ||||
Publisher | Royal Society of Chemistry | Place of Publication | Cambridge | Editor | |
Language | Wos | 000286327600010 | Publication Date | 2010-11-06 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 2041-6520;2041-6539; | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 8.668 | Times cited | 16 | Open Access | |
Notes | Approved | Most recent IF: 8.668; 2011 IF: 7.525 | |||
Call Number | UA @ lucian @ c:irua:88652 | Serial | 300 | ||
Permanent link to this record | |||||
Author | Alaria, J.; Borisov, P.; Dyer, M.S.; Manning, T.D.; Lepadatu, S.; Cain, M.G.; Mishina, E.D.; Sherstyuk, N.E.; Ilyin, N.A.; Hadermann, J.; Lederman, D.; Claridge, J.B.; Rosseinsky, M.J.; | ||||
Title | Engineered spatial inversion symmetry breaking in an oxide heterostructure built from isosymmetric room-temperature magnetically ordered components | Type | A1 Journal article | ||
Year | 2014 | Publication ![]() |
Chemical science | Abbreviated Journal | Chem Sci |
Volume | 5 | Issue | 4 | Pages | 1599-1610 |
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
Abstract | |||||
Address | |||||
Corporate Author | Thesis | ||||
Publisher | Royal Society of Chemistry | Place of Publication | Cambridge | Editor | |
Language | Wos | 000332467400044 | Publication Date | 2014-01-20 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 2041-6520;2041-6539; | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 8.668 | Times cited | 24 | Open Access | |
Notes | Approved | Most recent IF: 8.668; 2014 IF: 9.211 | |||
Call Number | UA @ lucian @ c:irua:117064 | Serial | 1045 | ||
Permanent link to this record | |||||
Author | Lieberman, C.M.; Filatov, A.S.; Wei, Z.; Rogachev, A.Y.; Abakumov, A.M.; Dikarev, E.V. | ||||
Title | Mixed-valent, heteroleptic homometallic diketonates as templates for the design of volatile heterometallic precursors | Type | A1 Journal article | ||
Year | 2015 | Publication ![]() |
Chemical science | Abbreviated Journal | Chem Sci |
Volume | 6 | Issue | 6 | Pages | 2835-2842 |
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
Abstract | A novel series of mixed-valent, heteroleptic transition metal diketonates that can be utilized as prospective single-source precursors for the low-temperature preparation of oxide materials are reported. The first mixed-valent iron beta-diketonates with different Fe-III/Fe-II ratios have been synthesized by applying the mixed-ligand approach. Based on nearly quantitative reaction yields and analysis of iron-oxygen bonds, these compounds were formulated as [Fe-III(acac)(3)][Fe-II(hfac)(2)] (1) and [Fe-II(hfac)(2)][Fe-III(acac)(3)][Fe-II(hfac)(2)] (2). In the above heteroleptic complexes, the Lewis acidic, coordinatively unsaturated Fe-II centers chelated by two hfac (hexafluoroacetylacetonate) ligands with electron-withdrawing substituents maintain bridging interactions with oxygen atoms of electron-donating acac (acetylacetonate) groups that chelate the neighboring Fe-III atoms. Switching the ligands on Fe-III and Fe-II atoms in starting reagents resulted in the instant ligand exchange between iron centers and in yet another polynuclear homometallic diketonate [Fe-II(hfac)(2)][Fe-III(acac)(2)(hfac)][Fe-II(hfac)(2)] (3) that adheres to the same bonding pattern as in complexes 1 and 2. The proposed synthetic methodology has been extended to design heterometallic diketonates with different M : M' ratios. Homometallic parent molecules have been used as templates to obtain heterometallic mixed-valent [Fe-III(acac)(3)][Mn-II(hfac)(2)] (4) and [Ni-II(hfac)(2)] – [Fe-III(acac)(3)][Ni-II(hfac)(2)] (5) complexes. The combination of two different diketonate ligands with electron-donating and electron-withdrawing substituents was found to be crucial for maintaining the above mixed-valent heterometallic assemblies. Theoretical investigation of two possible “isomers”, [Fe-III(acac)(3)][Mn-II(hfac)(2)] (4) and [Mn-III(acac)(3)][Fe-II(hfac)(2)] (40) provided an additional support for the metal site assignment giving a preference of 9.78 kcal mol(-1) for the molecule 4. Heterometallic complexes obtained in the course of this study have been found to act as effective single-source precursors for the synthesis of mixed-transition metal oxide materials MxM2-xO3 and MxMi-xO. The title highly volatile precursors can be used for the low-temperature preparation of both amorphous and crystalline heterometallic oxides in the form of thin films or nanosized particles that are known to operate as efficient catalysts in oxygen evolution reaction. | ||||
Address | |||||
Corporate Author | Thesis | ||||
Publisher | Royal Society of Chemistry | Place of Publication | Cambridge | Editor | |
Language | Wos | 000353223100021 | Publication Date | 2015-02-25 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 2041-6520;2041-6539; | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 8.668 | Times cited | 13 | Open Access | |
Notes | Approved | Most recent IF: 8.668; 2015 IF: 9.211 | |||
Call Number | c:irua:126031 | Serial | 2092 | ||
Permanent link to this record | |||||
Author | Yang, T.; Abakumov, A.M.; Hadermann, J.; Van Tendeloo, G.; Nowik, I.; Stephens, P.W.; Hamberger, J.; Tsirlin, A.A.; Ramanujachary, K.V.; Lofland, S.; Croft, M.; Ignatov, A.; Sun, J.; Greenblatt, M. | ||||
Title | _BiMnFe2O6, a polysynthetically twinned hcp MO structure | Type | A1 Journal article | ||
Year | 2010 | Publication ![]() |
Chemical science | Abbreviated Journal | Chem Sci |
Volume | 1 | Issue | 6 | Pages | 751-762 |
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
Abstract | The most efficient use of spatial volume and the lowest potential energies in the metal oxide structures are based on cubic close packing (ccp) or hexagonal close packing (hcp) of anions with cations occupying the interstices. A promising way to tune the composition of close packed oxides and design new compounds is related to fragmenting the parent structure into modules by periodically spaced planar interfaces, such as twin planes at the unit cell scale. The unique crystal chemistry properties of cations with a lone electron pair, such as Bi3+ or Pb2+, when located at interfaces, enables them to act as chemical scissors, to help relieve configurational strain. With this approach, we synthesized a new oxide, BiMnFe2O6, where fragments of the hypothetical hcp oxygen-based MO structure (the NiAs structure type), for the first time, serve as the building modules in a complex transition metal oxide. Mn3+ and Fe3+ ions are randomly distributed in two crystallographically independent sites (M1 and M2). The structure consists of quasi two-dimensional blocks of the 2H hexagonal close packed MO structure cut along the (114) crystal plane of the hcp lattice and stacked along the c axis. The blocks are related by a mirror operation that allows BiMnFe2O6 to be considered as a polysynthetically twinned 2H hcp MO structure. The transition to an AFM state with an incommensurate spin configuration at [similar] 212 K is established by 57Fe Mössbauer spectroscopy, magnetic susceptibility, specific heat and low temperature powder neutron diffraction. | ||||
Address | |||||
Corporate Author | Thesis | ||||
Publisher | Royal Society of Chemistry | Place of Publication | Cambridge | Editor | |
Language | Wos | 000283939200013 | Publication Date | 2010-10-12 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 2041-6520;2041-6539; | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 8.668 | Times cited | 12 | Open Access | |
Notes | Approved | Most recent IF: 8.668; 2010 IF: NA | |||
Call Number | UA @ lucian @ c:irua:85823 | Serial | 3517 | ||
Permanent link to this record | |||||
Author | Bal, K.M.; Neyts, E.C. | ||||
Title | Direct observation of realistic-temperature fuel combustion mechanisms in atomistic simulations | Type | A1 Journal article | ||
Year | 2016 | Publication ![]() |
Chemical science | Abbreviated Journal | Chem Sci |
Volume | 7 | Issue | 7 | Pages | 5280-5286 |
Keywords | A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | Atomistic simulations can in principle provide an unbiased description of all mechanisms, intermediates, and products of complex chemical processes. However, due to the severe time scale limitation of conventional simulation techniques, unrealistically high simulation temperatures are usually applied, which are a poor approximation of most practically relevant low-temperature applications. In this work, we demonstrate the direct observation at the atomic scale of the pyrolysis and oxidation of n-dodecane at temperatures as low as 700 K through the use of a novel simulation technique, collective variable-driven hyperdynamics (CVHD). A simulated timescale of up to 39 seconds is reached. Product compositions and dominant mechanisms are found to be strongly temperature-dependent, and are consistent with experiments and kinetic models. These simulations provide a first atomic-level look at the full dynamics of the complicated fuel combustion process at industrially relevant temperatures and time scales, unattainable by conventional molecular dynamics simulations. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | 000380893900059 | Publication Date | 2016-05-05 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 2041-6520 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 8.668 | Times cited | 22 | Open Access | |
Notes | K. M. B. is funded as PhD fellow (aspirant) of the FWO-Flanders (Fund for Scientic Research-Flanders), Grant 11V8915N. The computational resources and services used in this work were provided by the VSC (Flemish Supercomputer Center) and the HPC infrastructure of the University of Antwerp (CalcUA), funded by the Hercules Foundation and the Flemish Government – department EWI. The authors would also like to thank S. Banerjee for assisting with the interpretation of the experimental results. | Approved | Most recent IF: 8.668 | ||
Call Number | c:irua:134577 c:irua:135670 | Serial | 4105 | ||
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Author | Aussems, D.U.B.; Bal, K. M.; Morgan, T.W.; van de Sanden, M.C.M.; Neyts, E.C. | ||||
Title | Atomistic simulations of graphite etching at realistic time scales | Type | A1 Journal article | ||
Year | 2017 | Publication ![]() |
Chemical science | Abbreviated Journal | Chem Sci |
Volume | 8 | Issue | 10 | Pages | 7160-7168 |
Keywords | A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | Hydrogen–graphite interactions are relevant to a wide variety of applications, ranging from astrophysics to fusion devices and nano-electronics. In order to shed light on these interactions, atomistic simulation using Molecular Dynamics (MD) has been shown to be an invaluable tool. It suffers, however, from severe timescale limitations. In this work we apply the recently developed Collective Variable-Driven Hyperdynamics (CVHD) method to hydrogen etching of graphite for varying inter-impact times up to a realistic value of 1 ms, which corresponds to a flux of 1020 m2 s1. The results show that the erosion yield, hydrogen surface coverage and species distribution are significantly affected by the time between impacts. This can be explained by the higher probability of C–C bond breaking due to the prolonged exposure to thermal stress and the subsequent transition from ion- to thermal-induced etching. This latter regime of thermal-induced etching – chemical erosion – is here accessed for the first time using atomistic simulations. In conclusion, this study demonstrates that accounting for long time-scales significantly affects ion bombardment simulations and should not be neglected in a wide range of conditions, in contrast to what is typically assumed. |
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Publisher | Place of Publication | Editor | |||
Language | Wos | 000411730500055 | Publication Date | 2017-08-24 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 2041-6520 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 8.668 | Times cited | 3 | Open Access | OpenAccess |
Notes | DIFFER is part of the Netherlands Organisation for Scientic Research (NWO). K. M. B. is funded as a PhD fellow (aspirant) of the FWO-Flanders (Fund for Scientic Research-Flanders), Grant 11V8915N. The computational resources and services used in this work were provided by the VSC (Flemish Supercomputer Center), funded by the Research Foundation – Flanders (FWO) and the Flemish Government – department EWI. | Approved | Most recent IF: 8.668 | ||
Call Number | PLASMANT @ plasmant @c:irua:145519 | Serial | 4707 | ||
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Author | Bueken, B.; Van Velthoven, N.; Willhammar, T.; Stassin, T.; Stassen, I.; Keen, D.A.; Baron, G.V.; Denayer, J.F.M.; Ameloot, R.; Bals, S.; De Vos, D.; Bennett, T.D. | ||||
Title | Gel-based morphological design of zirconium metal-organic frameworks | Type | A1 Journal article | ||
Year | 2017 | Publication ![]() |
Chemical science | Abbreviated Journal | Chem Sci |
Volume | 8 | Issue | 8 | Pages | 3939-3948 |
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
Abstract | The ability of metal-organic frameworks (MOFs) to gelate under specific synthetic conditions opens up new opportunities in the preparation and shaping of hierarchically porous MOF monoliths, which could be directly implemented for catalytic and adsorptive applications. In this work, we present the first examples of xero-or aerogel monoliths consisting solely of nanoparticles of several prototypical Zr4+-based MOFs: UiO-66-X (X – H, NH2, NO2, (OH)(2)), UiO-67, MOF-801, MOF-808 and NU-1000. High reactant and water concentrations during synthesis were observed to induce the formation of gels, which were converted to monolithic materials by drying in air or supercritical CO2. Electron microscopy, combined with N-2 physisorption experiments, was used to show that irregular nanoparticle packing leads to pure MOF monoliths with hierarchical pore systems, featuring both intraparticle micropores and interparticle mesopores. Finally, UiO-66 gels were shaped into monolithic spheres of 600 mm diameter using an oil-drop method, creating promising candidates for packed-bed catalytic or adsorptive applications, where hierarchical pore systems can greatly mitigate mass transfer limitations. | ||||
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Publisher | Royal Society of Chemistry | Place of Publication | Cambridge | Editor | |
Language | Wos | 000400553000077 | Publication Date | 2017-03-23 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 2041-6520 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 8.668 | Times cited | 168 | Open Access | OpenAccess |
Notes | ; B. B., T. S. and I. S. acknowledge the FWO Flanders (doctoral and post-doctoral grants). T. W. acknowledges a post-doctoral grant from the Swedish Research Council. T. D. B. acknowledges the Royal Society (University Research Fellowship) and Trinity Hall (University of Cambridge) for funding. S. B. and D. D. V. are grateful for funding by Belspo (IAP 7/05 P6/27) and by the FWO Flanders. D. D. V. further acknowledges funding from the European Research Council (project H-CCAT). S. B. acknowledges financial support from the European Research Council (ERC Starting Grant #335078-COLOURATOMS). The authors acknowledge Arnau Carne and Shuhei Furukawa for assistance with supercritical CO<INF>2</INF> extraction, and Charles Ghesquiere for assistance in synthesis. ; Ecas_Sara | Approved | Most recent IF: 8.668 | ||
Call Number | UA @ lucian @ c:irua:152643UA @ admin @ c:irua:152643 | Serial | 5143 | ||
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Author | Van Velthoven, N.; Waitschat, S.; Chavan, S.M.; Liu, P.; Smolders, S.; Vercammen, J.; Bueken, B.; Bals, S.; Lillerud, K.P.; Stock, N.; De Vos, D.E. | ||||
Title | Single-site metal-organic framework catalysts for the oxidative coupling of arenes via C-H/C-H activation | Type | A1 Journal article | ||
Year | 2019 | Publication ![]() |
Chemical science | Abbreviated Journal | Chem Sci |
Volume | 10 | Issue | 10 | Pages | 3616-3622 |
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
Abstract | C-H activation reactions are generally associated with relatively low turnover numbers (TONs) and high catalyst concentrations due to a combination of low catalyst stability and activity, highlighting the need for recyclable heterogeneous catalysts with stable single-atom active sites. In this work, several palladium loaded metal-organic frameworks (MOFs) were tested as single-site catalysts for the oxidative coupling of arenes (e.g. o-xylene) via C-H/C-H activation. Isolation of the palladium active sites on the MOF supports reduced Pd(0) aggregate formation and thus catalyst deactivation, resulting in higher turnover numbers (TONs) compared to the homogeneous benchmark reaction. Notably, a threefold higher TON could be achieved for palladium loaded MOF-808 due to increased catalyst stability and the heterogeneous catalyst could efficiently be reused, resulting in a cumulative TON of 1218 after three runs. Additionally, the palladium single-atom active sites on MOF-808 were successfully identified by Fourier transform infrared (FTIR) and extended X-ray absorption fine structure (EXAFS) spectroscopy. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | 000463759100017 | Publication Date | 2019-02-18 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 2041-6520 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 8.668 | Times cited | 68 | Open Access | OpenAccess |
Notes | ; The research leading to these results has received funding from the NMBP-01-2016 Program of the European Union's Horizon 2020 Framework Program H2020/2014-2020/under grant agreement no. [720996]. N. V. V., S. S., J. V., B. B. and D. E. D. V. thank the FWO for funding (SB, Aspirant and postdoctoral grants). The electron microscopy work was supported by FWO funding G038116. D. E. D. V. is grateful for KU Leuven support in the frame of the CASAS Metusalem project and a C3 type project. The XAS experiments were performed on beamline BM26A at the European Synchrotron Radiation Facility (ESRF), Grenoble, France. We are grateful to D. Banerjee at the ESRF for providing assistance in using beamline BM26A. Johnson Matthey and S. Bennett are gratefully acknowledged for providing Smopex-102. ; | Approved | Most recent IF: 8.668 | ||
Call Number | UA @ admin @ c:irua:159403 | Serial | 5259 | ||
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Author | De Jong, M.; Sleegers, N.; Kim, J.; Van Durme, F.; Samyn, N.; Wang, J.; De Wael, K. | ||||
Title | Electrochemical fingerprint of street samples for fast on-site screening of cocaine in seized drug powders | Type | A1 Journal article | ||
Year | 2016 | Publication ![]() |
Chemical science | Abbreviated Journal | Chem Sci |
Volume | Issue | Pages | 1-7 | ||
Keywords | A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation) | ||||
Abstract | We report on a wearable fingertip sensor for on-the-spot identification of cocaine and its cutting agents in street samples. Traditionally, on-site screening is performed by means of colour tests which are difficult to interpret and lack selectivity. By presenting the distinct voltammetric response of cocaine, cutting agents, binary mixtures of cocaine and street samples in solution and powder street samples, we were able to elucidate the electrochemical fingerprint of all these compounds. The new electrochemical concept holds considerable promise as an on-site screening method. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | 000371021900094 | Publication Date | 2016-01-06 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 2041-6520 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 8.668 | Times cited | 37 | Open Access | |
Notes | ; The authors acknowledge BELSPO for funding the APTADRU project (BR/314/PI/ APTADRU). ; | Approved | Most recent IF: 8.668 | ||
Call Number | UA @ admin @ c:irua:130404 | Serial | 5591 | ||
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Author | Neyts, E.C.; Ostrikov, K.K.; Sunkara, M.K.; Bogaerts, A. | ||||
Title | Plasma Catalysis: Synergistic Effects at the Nanoscale | Type | A1 Journal article | ||
Year | 2015 | Publication ![]() |
Chemical reviews | Abbreviated Journal | Chem Rev |
Volume | 115 | Issue | 115 | Pages | 13408-13446 |
Keywords | A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | Thermal-catalytic gas processing is integral to many current industrial processes. Ever-increasing demands on conversion and energy efficiencies are a strong driving force for the development of alternative approaches. Similarly, synthesis of several functional materials (such as nanowires and nanotubes) demands special processing conditions. Plasma catalysis provides such an alternative, where the catalytic process is complemented by the use of plasmas that activate the source gas. This combination is often observed to result in a synergy between plasma and catalyst. This Review introduces the current state-of-the-art in plasma catalysis, including numerous examples where plasma catalysis has demonstrated its benefits or shows future potential, including CO2 conversion, hydrocarbon reforming, synthesis of nanomaterials, ammonia production, and abatement of toxic waste gases. The underlying mechanisms governing these applications, as resulting from the interaction between the plasma and the catalyst, render the process highly complex, and little is known about the factors leading to the often-observed synergy. This Review critically examines the catalytic mechanisms relevant to each specific application. | ||||
Address | Department of Chemistry, Research Group PLASMANT, Universiteit Antwerpen , Universiteitsplein 1, 2610 Wilrijk-Antwerp, Belgium | ||||
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Publisher | Place of Publication | Editor | |||
Language | English | Wos | 000367563000006 | Publication Date | 2015-11-30 |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0009-2665 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 47.928 | Times cited | 204 | Open Access | |
Notes | ECN and AB gratefully acknowledge financial support from the Fund of Scientific Research Flanders (FWO), Belgium, Grant Number G.0217.14N. KO acknowledges partial support by the Australian Research Council and CSIRO’s OCE Science Leaders Program. MKS acknowledges partial support from US National Science Foundation through grants DMS 1125909 and EPSCoR 1355448 and also PhD students Babajide Ajayi, Apolo Nambo and Maria Carreon for their help. | Approved | Most recent IF: 47.928; 2015 IF: 46.568 | ||
Call Number | c:irua:130001 | Serial | 3993 | ||
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Author | Hoffman, B.M.; Lukoyanov, D.; Yang, Z.-Y.; Dean, D.R.; Seefeldt, L.C. | ||||
Title | Mechanism of Nitrogen Fixation by Nitrogenase: The Next Stage | Type | A1 Journal Article | ||
Year | 2014 | Publication ![]() |
Chemical Reviews | Abbreviated Journal | Chem. Rev. |
Volume | 114 | Issue | 8 | Pages | 4041-4062 |
Keywords | A1 Journal Article; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; | ||||
Abstract | Ammonia is a crucial nutrient used for plant growth and as a building block in pharmaceutical and chemical industry, produced via nitrogen fixation of the ubiquitous atmospheric N2. Current industrial ammonia production relies heavily on fossil resources, but a lot of work is put into developing non-fossil based pathways. Among these is the use of nonequilibrium plasma. In this work, we investigated water vapor as H source for nitrogen fixation into NH3 by non-equilibrium plasma. The highest selectivity towards NH3 was observed with low amounts of added H2O vapor, but the highest production rate was reached at high H2O vapor. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | Publication Date | 2014-04-23 | ||
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Series Volume | Series Issue | Edition | |||
ISSN | 0009-2665 | ISBN | Additional Links | ||
Impact Factor | Times cited | Open Access | |||
Notes | We would like to thank Sylvia Dewilde (Department of Biomedical Sciences) for providing analytical equipment. | Approved | no | ||
Call Number | PLASMANT @ plasmant @ | Serial | 6337 | ||
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