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| Author | Kirkwood, N.; De Backer, A.; Altantzis, T.; Winckelmans, N.; Longo, A.; Antolinez, F.V.; Rabouw, F.T.; De Trizio, L.; Geuchies, J.J.; Mulder, J.T.; Renaud, N.; Bals, S.; Manna, L.; Houtepen, A.J. | ||||
| Title | Locating and controlling the Zn content in In(Zn)P quantum dots | Type | A1 Journal article | ||
| Year | 2019 | Publication | Chemistry of materials | Abbreviated Journal | Chem Mater |
| Volume | 32 | Issue | 32 | Pages | 557-565 |
| Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
| Abstract | Zinc is routinely employed in the synthesis of InP quantum dots (QDs) to improve the photoluminescence efficiency and carrier mobility of the resulting In(Zn)P alloy nanostructures. The exact location of Zn in the final structures and the mechanism by which it enhances the optoelectronic properties of the QDs is debated. We use synchrotron X-ray absorbance spectroscopy to show that the majority of Zn in In(Zn)P QDs is located at their surface as Zn-carboxylates. However, a small amount of Zn is present inside the bulk of the QDs with the consequent contraction of their lattice, as confirmed by combining high resolution high-angle annular dark-field imaging scanning transmission electron microscopy (HAADF-STEM) with statistical parameter estimation theory. We further demonstrate that the Zn content and its incorporation into the QDs can be tuned by the ligation of commonly employed Zn carboxylate precursors: the use of highly reactive Zn-acetate leads to the formation of undesired Zn3P2 and the final nanostructures being characterized by broad optical features, whereas Zn-carboxylates with longer carbon chains lead to InP crystals with much lower zinc content and narrow optical features. These results can explain the differences between structural and optical properties of In(Zn)P samples reported across the literature, and provide a rational method to tune the amount of Zn in InP nanocrystals and to drive the incorporation of Zn either as surface Zn-carboxylate, as a substitutional dopant inside the InP crystal lattice, or even predominantly as Zn3P2. | ||||
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| Language | Wos | 000507721600056 | Publication Date | 2019-12-13 | |
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ISSN  |
0897-4756 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
| Impact Factor | 9.466 | Times cited | 39 | Open Access | OpenAccess |
| Notes | A.J.H. acknowledges support from the European Research Council Horizon 2020 ERC Grant Agreement No. 678004 (Doping on Demand). This research is supported by the Dutch Technology Foundation TTW, which is part of The Netherlands Organization for Scientific Research (NWO), and which is partly funded by Ministry of Economic Affairs. SB acknowledges funding from the European Research Council (grant 815128 REALNANO). The authors gratefully acknowledge funding from the Research Foundation Flanders (FWO, Belgium) through project funding G.0381.16N and a postdoctoral grant to A.D.B. AJH, LM and JM acknowledge support from the H2020 Collaborative Project TEQ (Grant No. 766900).; sygma | Approved | Most recent IF: 9.466 | ||
| Call Number | EMAT @ emat @c:irua:165234 | Serial | 5438 | ||
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| Author | Minjauw, M.M.; Solano, E.; Sree, S.P.; Asapu, R.; Van Daele, M.; Ramachandran, R.K.; Heremans, G.; Verbruggen, S.W.; Lenaerts, S.; Martens, J.A.; Detavernier, C.; Dendooven, J. | ||||
| Title | Plasma-enhanced atomic layer deposition of silver using Ag(fod)(PEt3) and NH3-plasma | Type | A1 Journal article | ||
| Year | 2017 | Publication | Chemistry of materials | Abbreviated Journal | Chem Mater |
| Volume | 29 | Issue | 17 | Pages | 7114-7121 |
| Keywords | A1 Journal article; Sustainable Energy, Air and Water Technology (DuEL) | ||||
| Abstract | A plasma-enhanced atomic layer deposition (ALD) process using the Ag(fod)(PEt3) precursor [(triethylphosphine)(6,6,7,7,8,8,8-heptafluoro-2,2-dimethy1-3,5-octanedionate)silver(I)] in combination with NH3-plasma is reported. The steady growth rate of the reported process (0.24 +/- 0.03 nm/cycle) was found to be 6 times larger than that of the previously reported Ag ALD process based on the same precursor in combination with H-2-plasma (0.04 +/- 0.02 nm/cycle). The ALD characteristics of the H-2-plasma and NH3-plasma processes were verified. The deposited Ag films were polycrystalline face-centered cubic Ag for both processes. The film morphology was investigated by ex situ scanning electron microscopy and grazing-incidence small-angle X-ray scattering, and it was found that films grown with the NH3-plasma process exhibit a much higher particle areal density and smaller particle sizes on oxide substrates compared to those deposited using the H-2-plasma process. This control over morphology of the deposited Ag is important for applications in catalysis and plasmonics. While films grown with the H-2-plasma process had oxygen impurities (similar to 9 atom %) in the bulk, the main impurity for the NH3-plasma process was nitrogen (similar to 7 atom %). In situ Fourier transform infrared spectroscopy experiments suggest that these nitrogen impurities are derived from NH surface groups generated during the NH3-plasma, which interact with the precursor molecules during the precursor pulse. We propose that the reaction of these surface groups with the precursor leads to additional deposition of Ag atoms during the precursor pulse compared to the H-2-plasma process, which explains the enhanced growth rate of the NH3-plasma process. | ||||
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| Language | Wos | 000410868600012 | Publication Date | 2017-08-09 | |
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| ISSN |
0897-4756 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
| Impact Factor | 9.466 | Times cited | 9 | Open Access | |
| Notes | ; M.M.M. and J.D. acknowledge the Fonds Wetenschappelijk Onderzoek Vlaanderen (FWO Vlaanderen) for financial support through a personal research grant. We also acknowledge FWO Vlaanderen for providing project funding for this work. We are grateful to the ESRF staff for smoothly running the synchrotron and beamline facilities. We also thank Olivier Janssens for performing the SEM measurements and Stefaan Broekaert for mechanical assistance. J.A.M. acknowledges the Flemish Government for long-term structural funding (Methusalem). ; | Approved | Most recent IF: 9.466 | ||
| Call Number | UA @ admin @ c:irua:146757 | Serial | 5983 | ||
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| Author | Marchetti, A.; Saniz, R.; Krishnan, D.; Rabbachin, L.; Nuyts, G.; De Meyer, S.; Verbeeck, J.; Janssens, K.; Pelosi, C.; Lamoen, D.; Partoens, B.; De Wael, K. | ||||
| Title | Unraveling the Role of Lattice Substitutions on the Stabilization of the Intrinsically Unstable Pb2Sb2O7Pyrochlore: Explaining the Lightfastness of Lead Pyroantimonate Artists’ Pigments | Type | A1 Journal article | ||
| Year | 2020 | Publication | Chemistry Of Materials | Abbreviated Journal | Chem Mater |
| Volume | 32 | Issue | 7 | Pages | 2863-2873 |
| Keywords | A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation); Electron microscopy for materials research (EMAT); Condensed Matter Theory (CMT) | ||||
| Abstract | The pyroantimonate pigments Naples yellow and lead tin antimonate yellow are recognized as some of the most stable synthetic yellow pigments in the history of art. However, this exceptional lightfastness is in contrast with experimental evidence suggesting that this class of mixed oxides is of semiconducting nature. In this study the electronic structure and light-induced behavior of the lead pyroantimonate pigments were determined by means of a combined multifaceted analytical and computational approach (photoelectrochemical measurements, UV-vis diffuse reflectance spectroscopy, STEM-EDS, STEM-HAADF, and density functional theory calculations). The results demonstrate both the semiconducting nature and the lightfastness of these pigments. Poor optical absorption and minority carrier mobility are the main properties responsible for the observed stability. In addition, novel fundamental insights into the role played by Na atoms in the stabilization of the otherwise intrinsically unstable Pb2Sb2O7 pyrochlore were obtained. | ||||
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| Language | Wos | 000526394000016 | Publication Date | 2020-04-14 | |
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| ISSN |
0897-4756 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
| Impact Factor | 8.6 | Times cited | 8 | Open Access | OpenAccess |
| Notes | Universiteit Antwerpen; Belgian Federal Science Policy Office; | Approved | Most recent IF: 8.6; 2020 IF: 9.466 | ||
| Call Number | EMAT @ emat @c:irua:168819 | Serial | 6363 | ||
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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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| Language | Wos | 000603288800034 | Publication Date | 2020-12-04 | |
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| 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 | 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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| Language | Wos | 000959572100001 | Publication Date | 2023-03-25 | |
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| 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 | 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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| Language | Wos | 001052093300001 | Publication Date | 2023-08-21 | |
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| 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 | 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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| Language | English | Wos | 001174840900001 | Publication Date | 2024-02-20 |
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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 | ||
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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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| Language | Wos | 000610984700009 | Publication Date | 2020-12-28 | |
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| 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 | Jorgensen, M.; Shea, P.T.; Tomich, A.W.; Varley, J.B.; Bercx, M.; Lovera, S.; Cerny, R.; Zhou, W.; Udovic, T.J.; Lavallo, V.; Jensen, T.R.; Wood, B.C.; Stavila, V. | ||||
| Title | Understanding superionic conductivity in lithium and sodium salts of weakly coordinating closo-hexahalocarbaborate anions | Type | A1 Journal article | ||
| Year | 2020 | Publication | Chemistry of materials | Abbreviated Journal | |
| Volume | 32 | Issue | 4 | Pages | 1475-1487 |
| Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
| Abstract | Solid-state ion conductors based on closo-polyborate anions combine high ionic conductivity with a rich array of tunable properties. Cation mobility in these systems is intimately related to the strength of the interaction with the neighboring anionic network and the energy for reorganizing the coordination polyhedra. Here, we explore such factors in solid electrolytes with two anions of the weakest coordinating ability, [HCB11H5Cl6](-) and [HCB11H5Br6](-), and a total of 11 polymorphs are identified for their lithium and sodium salts. Our approach combines ab initio molecular dynamics, synchrotron X-ray powder diffraction, differential scanning calorimetry, and AC impedance measurements to investigate their structures, phase-transition behavior, anion orientational mobilities, and ionic conductivities. We find that M(HCB11H5X6) (M = Li, Na, X = Cl, Br) compounds exhibit order-disorder polymorphic transitions between 203 and 305 degrees C and display Li and Na superionic conductivity in the disordered state. Through detailed analysis, we illustrate how cation disordering in these compounds originates from a competitive interplay among the lattice symmetry, the anion reorientational mobility, the geometric and electronic asymmetry of the anion, and the polarizability of the halogen atoms. These factors are compared to other closo-polyborate-based ion conductors to suggest guidelines for optimizing the cation-anion interaction for fast ion mobility. This study expands the known solid-state poly(carba)borate-based materials capable of liquid-like ionic conductivities, unravels the mechanisms responsible for fast ion transport, and provides insights into the development of practical superionic solid electrolytes. | ||||
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| Language | Wos | 000517351300014 | Publication Date | 2020-01-23 | |
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| Impact Factor | Times cited | 5 | Open Access | OpenAccess | |
| Notes | ; The authors gratefully acknowledge support from the Hydrogen Materials-Advanced Research Consortium (HyMARC), established as part of the Energy Materials Network under the U.S. Department of Energy, Office of Energy Efficiency and Renewable Energy, Fuel Cell Technologies Office, under Contract no. AC04-94AL85000. Sandia National Laboratories is a multimission laboratory managed and operated by National Technology and Engineering Solutions of Sandia, LLC., a wholly owned subsidiary of Honeywell International, Inc., for the U.S. Department of Energy's National Nuclear Security Administration under Contract no. DE-NA-0003525. A portion of this work was performed under the auspices of the U.S. Department of Energy by Lawrence Livermore National Laboratory under Contract no. ACS2-07NA27344. We also gratefully thank Kyoung Kweon for useful discussions. The views and opinions of the authors expressed herein do not necessarily state or reflect those of the United States Government or any agency thereof. Neither the United States Government nor any agency thereof nor any of their employees, makes any warranty, expressed or implied, or assumes any legal liability or responsibility for the accuracy, completeness, or usefulness of any information, apparatus, product, or process disclosed, or represents that its use would not infringe privately owned rights. The Danish council for independent research, technology and production, HyNanoBorN (4181-00462) and SOS-MagBat (9041-00226B) and NordForsk, The Nordic Neutron Science Program, project FunHy (81942), and the Carlsberg Foundation are acknowledged for funding. Affiliation with the Center for Integrated Materials Research (iMAT) at Aarhus University is gratefully acknowledged. V.L. acknowledges the NSF for partial support of this project (DMR-1508537). The authors would like to thank the Swiss-Norwegian beamlines (BM01) at the ESRF, Grenoble, for the help with the data collection, DESY for access to Petra III, at beamline P02.1, and Diamond for access to beamline I11. ; | Approved | Most recent IF: NA | ||
| Call Number | UA @ admin @ c:irua:167754 | Serial | 6645 | ||
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