“Size-Induced Switching of Nanowire Growth Direction: a New Approach Toward Kinked Nanostructures”. Shen Y, Lebedev OI, Turner S, Van Tendeloo G, Song X, Yu X, Wang Q, Chen H, Dayeh SA, Wu T, Advanced functional materials 26, 3687 (2016). http://doi.org/10.1002/ADFM.201600142
Abstract: Exploring self-assembled nanostructures with controllable architectures has been a central theme in nanoscience and nanotechnology because of the tantalizing perspective of directly integrating such bottom-up nanostructures into functional devices. Here, the growth of kinked single-crystal In2O3 nanostructures consisting of a nanocone base and a nanowire tip with an epitaxial and defect-free transition is demonstrated for the first time. By tailoring the growth conditions, a reliable switching of the growth direction from [111] to [110] or [112] is observed when the Au catalyst nanoparticles at the apexes of the nanocones shrink below approximate to 100 nm. The natural formation of kinked nanoarchitectures at constant growth pressures is related to the size-dependent free energy that changes for different orientations of the nanowires. The results suggest that the mechanism of forming such kinked nanocone-nanowire nanostructures in well-controlled growth environment may be universal for a wide range of functional materials.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 12.124
Times cited: 2
DOI: 10.1002/ADFM.201600142
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“Encapsulation of Noble Metal Nanoparticles through Seeded Emulsion Polymerization as Highly Stable Plasmonic Systems”. Scarabelli L, Schumacher M, Jimenez de Aberasturi D, Merkl J‐P, Henriksen‐Lacey M, Milagres de Oliveira T, Janschel M, Schmidtke C, Bals S, Weller H, Liz‐Marzán LM, Advanced functional materials 29, 1809071 (2019). http://doi.org/10.1002/adfm.201809071
Abstract: The implementation of plasmonic nanoparticles in vivo remains hindered by important limitations such as biocompatibility, solubility in biological fluids, and physiological stability. A general and versatile protocol is presented, based on seeded emulsion polymerization, for the controlled encapsulation of gold and silver nanoparticles. This procedure enables the encapsulation of single nanoparticles as well as nanoparticle clusters inside a protecting polymer shell. Specifically, the efficient coating of nanoparticles of both metals is demonstrated, with final dimensions ranging between 50 and 200 nm, i.e., sizes of interest for bio-applications. Such hybrid nanocomposites display extraordinary stability in high ionic strength and oxidizing environments, along with high cellular uptake, and low cytotoxicity. Overall, the prepared nanostructures are promising candidates for plasmonic applications under biologically relevant conditions.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 12.124
Times cited: 19
DOI: 10.1002/adfm.201809071
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“Self‐Assembly of Atomically Thin Chiral Copper Heterostructures Templated by Black Phosphorus”. Nerl HC, Pokle A, Jones L, Müller‐Caspary K, Bos KHW, Downing C, McCarthy EK, Gauquelin N, Ramasse QM, Lobato I, Daly D, Idrobo JC, Van Aert S, Van Tendeloo G, Sanvito S, Coleman JN, Cucinotta CS, Nicolosi V, Advanced functional materials 29, 1903120 (2019). http://doi.org/10.1002/adfm.201903120
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 12.124
Times cited: 1
DOI: 10.1002/adfm.201903120
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“Thickness dependent properties in oxide heterostructures driven by structurally induced metal-oxygen hybridization variations”. Liao Z, Gauquelin N, Green RJ, Macke S, Gonnissen J, Thomas S, Zhong Z, Li L, Si L, Van Aert S, Hansmann P, Held K, Xia J, Verbeeck J, Van Tendeloo G, Sawatzky GA, Koster G, Huijben M, Rijnders G, Advanced functional materials 27, 1606717 (2017). http://doi.org/10.1002/ADFM.201606717
Abstract: Thickness-driven electronic phase transitions are broadly observed in different types of functional perovskite heterostructures. However, uncertainty remains whether these effects are solely due to spatial confinement, broken symmetry, or rather to a change of structure with varying film thickness. Here, this study presents direct evidence for the relaxation of oxygen-2p and Mn-3d orbital (p-d) hybridization coupled to the layer-dependent octahedral tilts within a La2/3Sr1/3MnO3 film driven by interfacial octahedral coupling. An enhanced Curie temperature is achieved by reducing the octahedral tilting via interface structure engineering. Atomically resolved lattice, electronic, and magnetic structures together with X-ray absorption spectroscopy demonstrate the central role of thickness-dependent p-d hybridization in the widely observed dimensionality effects present in correlated oxide heterostructures.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 12.124
Times cited: 55
DOI: 10.1002/ADFM.201606717
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“Combined use of synchrotron-radiation-based imaging techniques for the characterization of structured catalysts”. Basile F, Benito P, Bugani S, de Nolf W, Fornasari G, Janssens K, Morselli L, Scavetta E, Tonelli D, Vaccari A, Advanced functional materials 20, 4117 (2010). http://doi.org/10.1002/ADFM.201001004
Abstract: Active-phase-coated metallic supports as structured catalysts are gaining attention in endothermic and exothermic processes because they improve heat transfer. The deposition of a well-adhered and stable catalyst layer on the metallic support constitutes an important feature for the successful application of the final material. In this work, coating of FeCrAlY foams is performed by a one-step electrosynthesis-deposition of hydrotalcite-type compounds, precursors of catalysts active in endothermic steam methane reforming. The catalysts are studied at different length scales by using, for the first time, a combination of several techniques: SEM/EDS and X-ray fluorescence, X-ray powder diffraction and absorption-tomography experiments on the micro- and nanoscales at a synchrotron facility. The results show that the morphology of the coating depends on the synthesis conditions and that the catalyst may be described as Ni metal crystallites dispersed on γ-Al2O3, homogeneously coating the FeCrAlY foam.
Keywords: A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation)
Impact Factor: 12.124
Times cited: 24
DOI: 10.1002/ADFM.201001004
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“Nonlayered CdSe flakes homojunctions”. Jin B, Liang F, Hu Z-Y, Wei P, Liu K, Hu X, Van Tendeloo G, Lin Z, Li H, Zhou X, Xiong Q, Zhai T, Advanced Functional Materials 30, 1908902 (2020). http://doi.org/10.1002/ADFM.201908902
Abstract: 2D homojunctions have stimulated extensive attention because of their perfect thermal and lattice matches, as well as their tunable band structures in 2D morphology, which provide fascinating opportunities for novel electronics and optoelectronics. Recently, 2D nonlayered materials have attracted the attention of researchers owing to their superior functional applications and diverse portfolio of the 2D family. Therefore, 2D nonlayered homojunctions would open the door to a rich spectrum of exotic 2D materials. However, they are not investigated due to their extremely difficult synthesis methods. Herein, nonlayered CdSe flakes homojunctions are obtained via self-limited growth with InCl3 as a passivation agent. Interestingly, two pieces of vertical wurtzite-zinc blende (WZ-ZB) homojunctions epitaxially integrate into WZ/ZB lateral junctions. These homojunctions show a divergent second-harmonic generation intensity, strongly correlated to the multiple twinned ZB phase, as identified by aberration-corrected scanning transmission electron microscopy and theoretical calculations. Impressively, the photodetector based on this WZ/ZB CdSe homojunction shows excellent performances, integrating a high photoswitching ratio (3.4 x 10(5)) and photoresponsivity (3.7 x 10(3) A W-1), suggesting promising potential for applications in electronics and optoelectronics.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 19
Times cited: 8
DOI: 10.1002/ADFM.201908902
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“Tailoring vanadium dioxide film orientation using nanosheets : a combined microscopy, diffraction, transport, and soft X-ray in transmission study”. Tran Phong Le P, Hofhuis K, Rana A, Huijben M, Hilgenkamp H, Rijnders GAJHM, ten Elshof JE, Koster G, Gauquelin N, Lumbeeck G, Schuessler-Langeheine C, Popescu H, Fortuna F, Smit S, Verbeek XH, Araizi-Kanoutas G, Mishra S, Vaskivskyi I, Duerr HA, Golden MS, Advanced Functional Materials 30, 1900028 (2020). http://doi.org/10.1002/ADFM.201900028
Abstract: Vanadium dioxide (VO2) is a much-discussed material for oxide electronics and neuromorphic computing applications. Here, heteroepitaxy of VO2 is realized on top of oxide nanosheets that cover either the amorphous silicon dioxide surfaces of Si substrates or X-ray transparent silicon nitride membranes. The out-of-plane orientation of the VO2 thin films is controlled at will between (011)(M1)/(110)(R) and (-402)(M1)/(002)(R) by coating the bulk substrates with Ti0.87O2 and NbWO6 nanosheets, respectively, prior to VO2 growth. Temperature-dependent X-ray diffraction and automated crystal orientation mapping in microprobe transmission electron microscope mode (ACOM-TEM) characterize the high phase purity, the crystallographic and orientational properties of the VO2 films. Transport measurements and soft X-ray absorption in transmission are used to probe the VO2 metal-insulator transition, showing results of a quality equal to those from epitaxial films on bulk single-crystal substrates. Successful local manipulation of two different VO2 orientations on a single substrate is demonstrated using VO2 grown on lithographically patterned lines of Ti0.87O2 and NbWO6 nanosheets investigated by electron backscatter diffraction. Finally, the excellent suitability of these nanosheet-templated VO2 films for advanced lensless imaging of the metal-insulator transition using coherent soft X-rays is discussed.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 19
Times cited: 1
DOI: 10.1002/ADFM.201900028
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“Circumventing Wear and Tear of Adaptive Porous Materials”. Canossa S, Ji Z, Wuttke S, Advanced Functional Materials , 1908547 (2020). http://doi.org/10.1002/adfm.201908547
Abstract: The assessment of the architectural stability of molecular porous materials is not yet a common practice, but critical to their understanding and development. The conformational adaptation of porous materials to guest binding and other chemical dynamics poses a risk of architectural damage, leading to performance deterioration during their prolonged usage. The deformation of the framework backbone and the disconnection of building units are driven by chemical, mechanical, and thermal perturbations, and can be quantitatively described by the term connection completeness. Analytical means that can be used to measure this parameter are presented in order to provide a standard, practical protocol for evaluating architectural damage made to framework materials. Preventive and remedial strategies are proposed for enhancing the architectural integrity of frameworks without compromising their functional mechanisms, paving the way to the design of robust yet adaptive materials. In this way, the discussion on architectural stability is initiated, and readers are encouraged to carefully characterize molecular porous materials for a better understanding of their structure-property relationship.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 19
DOI: 10.1002/adfm.201908547
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“Pore Chemistry of Metal–Organic Frameworks”. Ji Z, Wang H, Canossa S, Wuttke S, Yaghi OM, Advanced Functional Materials 30, 2000238 (2020). http://doi.org/10.1002/adfm.202000238
Abstract: The pores in metal–organic frameworks (MOFs) can be functionalized by placing chemical entities along the backbone and within the backbone. This chemistry is enabled by the architectural, thermal, and chemical robustness of the frameworks and the ability to characterize them by many diffraction and spectroscopic techniques. The pore chemistry of MOFs is articulated in terms of site isolation, coupling, and cooperation and relate that to their functions in guest recognition, catalysis, ion and electron transport, energy transfer, pore‐dynamic modulation, and interface construction. It is envisioned that the ultimate control of pore chemistry requires arranging functionalities into defined sequences and developing techniques for reading and writing such sequences within the pores.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 19
DOI: 10.1002/adfm.202000238
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“Excellent excitonic photovoltaic effect in 2D CsPbBr₃/CdS heterostructures”. Jin B, Zuo N, Hu Z-Y, Cui W, Wang R, Van Tendeloo G, Zhou X, Zhai T, Advanced Functional Materials , 2006166 (2020). http://doi.org/10.1002/ADFM.202006166
Abstract: P-n photovoltaic junctions are essential building blocks for optoelectronic devices for energy conversion. However, this photovoltaic efficiency has almost reached its theoretical limit. Here, a brand-new excitonic photovoltaic effect in 2D CsPbBr3/CdS heterostructures is revealed. These heterostructures, synthesized by epitaxial growth, display a clean interface and a strong interlayer coupling. The excitonic photovoltaic effect is a function of both the built-in equilibrium electrical potential energy and the chemical potential energy, which is generated by the significant concentration gradient of electrons and holes at the heterojunction interface. Excitingly, this novel photovoltaic effect results in a large open-circuit voltage of 0.76 V and a high power conversion efficiency of 17.5%. In addition, high photodetection performance, including a high photoswitch ratio (I-light/I-dark) of 10(5)and a fast response rate of 23 mu s are obtained. These findings provide a new platform for photovoltaic applications.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 19
Times cited: 1
DOI: 10.1002/ADFM.202006166
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“Injectable Plasma‐Treated Alginate Hydrogel for Oxidative Stress Delivery to Induce Immunogenic Cell Death in Osteosarcoma”. Živanić, M, Espona‐Noguera A, Verswyvel H, Smits E, Bogaerts A, Lin A, Canal C, Advanced functional materials (2023). http://doi.org/10.1002/adfm.202312005
Abstract: Cold atmospheric plasma (CAP) is a source of cell‐damaging oxidant molecules that may be used as low‐cost cancer treatment with minimal side effects. Liquids treated with cold plasma and enriched with oxidants are a modality for non‐invasive treatment of internal tumors with cold plasma via injection. However, liquids are easily diluted with body fluids which impedes high and localized delivery of oxidants to the target. As an alternative, plasma‐treated hydrogels (PTH) emerge as vehicles for the precise delivery of oxidants. This study reports an optimal protocol for the preparation of injectable alginate PTH that ensures the preservation of plasma‐generated oxidants. The generation, storage, and release of oxidants from the PTH are assessed. The efficacy of the alginate PTH in cancer treatment is demonstrated in the context of cancer cell cytotoxicity and immunogenicity–release of danger signals and phagocytosis by immature dendritic cells, up to now unexplored for PTH. These are shown in osteosarcoma, a hard‐to‐treat cancer. The study aims to consolidate PTH as a novel cold plasma treatment modality for non‐invasive or postoperative tumor treatment. The results offer a rationale for further exploration of alginate‐based PTHs as a versatile platform in biomedical engineering.
Keywords: A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT); Center for Oncological Research (CORE)
Impact Factor: 19
DOI: 10.1002/adfm.202312005
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“Functionalization chemistry of porous materials”. Canossa S, Wuttke S, Advanced Functional Materials 30, 2003875 (2020). http://doi.org/10.1002/ADFM.202003875
Keywords: Editorial; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 19
Times cited: 1
DOI: 10.1002/ADFM.202003875
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“Intracellular fate of hydrophobic nanocrystal self-assemblies in tumor cells”. Nicolas-Boluda A, Yang Z, Dobryden I, Carn F, Winckelmans N, Pechoux C, Bonville P, Bals S, Claesson PM, Gazeau F, Pileni MP, Advanced Functional Materials 30, 2004274 (2020). http://doi.org/10.1002/ADFM.202004274
Abstract: Control of interactions between nanomaterials and cells remains a biomedical challenge. A strategy is proposed to modulate the intralysosomal distribution of nanoparticles through the design of 3D suprastructures built by hydrophilic nanocrystals (NCs) coated with alkyl chains. The intracellular fate of two water-dispersible architectures of self-assembled hydrophobic magnetic NCs: hollow deformable shells (colloidosomes) or solid fcc particles (supraballs) is compared. These two self-assemblies display increased cellular uptake by tumor cells compared to dispersions of the water-soluble NC building blocks. Moreover, the self-assembly structures increase the NCs density in lysosomes and close to the lysosome membrane. Importantly, the structural organization of NCs in colloidosomes and supraballs are maintained in lysosomes up to 8 days after internalization, whereas initially dispersed hydrophilic NCs are randomly aggregated. Supraballs and colloidosomes are differently sensed by cells due to their different architectures and mechanical properties. Flexible and soft colloidosomes deform and spread along the biological membranes. In contrast, the more rigid supraballs remain spherical. By subjecting the internalized suprastructures to a magnetic field, they both align and form long chains. Overall, it is highlighted that the mechanical and topological properties of the self-assemblies direct their intracellular fate allowing the control intralysosomal density, ordering, and localization of NCs.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 19
Times cited: 11
DOI: 10.1002/ADFM.202004274
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“Phase-transformation-induced giant deformation in thermoelectric Ag₂Se semiconductor”. Liang Q, Yang D, Xia F, Bai H, Peng H, Yu R, Yan Y, He D, Cao S, Van Tendeloo G, Li G, Zhang Q, Tang X, Wu J, Advanced Functional Materials , 2106938 (2021). http://doi.org/10.1002/ADFM.202106938
Abstract: In most semiconducting metal chalcogenides, a large deformation is usually accompanied by a phase transformation, while the deformation mechanism remains largely unexplored. Herein, a phase-transformation-induced deformation in Ag2Se is investigated by in situ transmission electron microscopy, and a new ordered high-temperature phase (named as alpha '-Ag2Se) is identified. The Se-Se bonds are folded when the Ag+-ion vacancies are ordered and become stretched when these vacancies are disordered. Such a stretch/fold of the Se-Se bonds enables a fast and large deformation occurring during the phase transition. Meanwhile, the different Se-Se bonding states in alpha-, alpha '-, beta-Ag2Se phases lead to the formation of a large number of nanoslabs and the high concentration of dislocations at the interface, which flexibly accommodate the strain caused by the phase transformation. This study reveals the atomic mechanism of the deformation in Ag2Se inorganic semiconductors during the phase transition, which also provides inspiration for understanding the phase transition process in other functional materials.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 12.124
DOI: 10.1002/ADFM.202106938
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“The role of SnF₂, additive on interface formation in all lead-free FASnI₃, perovskite solar cells”. Zillner J, Boyen H-G, Schulz P, Hanisch J, Gauquelin N, Verbeeck J, Kueffner J, Desta D, Eisele L, Ahlswede E, Powalla M, Advanced functional materials , 2109649 (2022). http://doi.org/10.1002/ADFM.202109649
Abstract: Tin-based perovskites are promising alternative absorber materials for leadfree perovskite solar cells but need strategies to avoid fast tin (Sn) oxidation. Generally, this reaction can be slowed down by the addition of tin fluoride (SnF2) to the perovskite precursor solution, which also improves the perovskite layer morphology. Here, this work analyzes the spatial distribution of the additive within formamidinium tin triiodide (FASnI(3)) films deposited on top of poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) hole transporting layers. Employing time-of-flight secondary ion mass spectrometry and a combination of hard and soft X-ray photoelectron spectroscopy, it is found that Sn F2 preferably accumulates at the PEDOT:PSS/perovskite interface, accompanied by the formation of an ultrathin SnS interlayer with an effective thickness of approximate to 1.2 nm.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 19
Times cited: 22
DOI: 10.1002/ADFM.202109649
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“Wearable self‐powered electrochemical devices for continuous health management”. Parrilla M, De Wael K, Advanced Functional Materials 31, 2107042 (2021). http://doi.org/10.1002/ADFM.202107042
Abstract: The wearable revolution is already present in society through numerous gadgets. However, the contest remains in fully deployable wearable (bio)chemical sensing. Its use is constrained by the energy consumption which is provided by miniaturized batteries, limiting the autonomy of the device. Hence, the combination of materials and engineering efforts to develop sustainable energy management is paramount in the next generation of wearable self-powered electrochemical devices (WeSPEDs). In this direction, this review highlights for the first time the incorporation of innovative energy harvesting technologies with top-notch wearable self-powered sensors and low-powered electrochemical sensors toward battery-free and self-sustainable devices for health and wellbeing management. First, current elements such as wearable designs, electrochemical sensors, energy harvesters and storage, and user interfaces that conform WeSPEDs are depicted. Importantly, the bottlenecks in the development of WeSPEDs from an analytical perspective, product side, and power needs are carefully addressed. Subsequently, energy harvesting opportunities to power wearable electrochemical sensors are discussed. Finally, key findings that will enable the next generation of wearable devices are proposed. Overall, this review aims to bring new strategies for an energy-balanced deployment of WeSPEDs for successful monitoring of (bio)chemical parameters of the body toward personalized, predictive, and importantly, preventive healthcare.
Keywords: A1 Journal article; Engineering sciences. Technology; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation); Antwerp Electrochemical and Analytical Sciences Lab (A-Sense Lab)
Impact Factor: 12.124
DOI: 10.1002/ADFM.202107042
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“Atomically deciphering the phase segregation in mixed halide perovskite”. Yang C-Q, Yin Z-W, Li W, Cui W-J, Zhou X-G, Wang L-D, Zhi R, Xu Y-Y, Tao Z-W, Sang X, Cheng Y-B, Van Tendeloo G, Hu Z-Y, Su B-L, Advanced functional materials , 1 (2024). http://doi.org/10.1002/ADFM.202400569
Abstract: Mixed-halide perovskites show promising applications in tandem solar cells owing to their adjustable bandgap. One major obstacle to their commercialization is halide phase segregation, which results in large open-circuit voltage deficiency and J-V hysteresis. However, the ambiguous interplay between structural origin and phase segregation often results in aimless and unspecific optimization strategies for the device's performance and stability. An atomic scale is directly figured out the abundant Ruddlesden-Popper anti-phase boundaries (RP-APBs) within a CsPbIBr2 polycrystalline film and revealed that phase segregation predominantly occurs at RP-APB-enriched interfaces due to the defect-mediated lattice strain. By compensating their structural lead halide, such RP-APBs are eliminated, and the decreasing of strain can be observed, resulting in the suppression of halide phase segregation. The present work provides the deciphering to precisely regulate the perovskite atomic structure for achieving photo-stable mixed halide wide-bandgap perovskites of high-efficiency tandem solar cell commercial applications. The phase segregation in mixed halide perovskite film predominantly occurs at Ruddlesden-Popper anti-phase boundaries (RP-APBs)-enriched interfaces due to the defect-mediated lattice strain. The RP-APBs defects can be eliminated by compensating for their structural lead halide deficiency, resulting in the suppression of halide phase segregation. image
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 19
DOI: 10.1002/ADFM.202400569
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“Mitigated oxygen loss in lithium-rich manganese-based cathode enabled by strong Zr-O affinity”. Wang G, Xie C, Wang H, Li Q, Xia F, Zeng W, Peng H, Van Tendeloo G, Tan G, Tian J, Wu J, Advanced functional materials , 2313672 (2024). http://doi.org/10.1002/ADFM.202313672
Abstract: Oxygen loss is a serious problem of lithium-rich layered oxide (LLO) cathodes, as the high capacity of LLO relies on reversible oxygen redox. Oxygen release can occur at the surface leading to the formation of spinel or rock salt structures. Also, the lattice oxygen will usually become unstable after long cycling, which remains a major roadblock in the application of LLO. Here, it is shown that Zr doping is an effective strategy to retain lattice oxygen in LLO due to the high affinity between Zr and O. A simple sol-gel method is used to dope Zr4+ into the LLOs to adjust the local electronic structure and inhibit the diffusion of oxygen anions to the surface during cycling. Compared with untreated LLOs, LLO-Zr cathodes exhibit a higher cycling stability, with 94% capacity retention after 100 cycles at 0.4 C, up to 223 mAh g-1 at 1 C, and 88% capacity retention after 300 cycles. Theoretical calculations show that due to the strong Zr-O covalent bonding, the formation energy of oxygen vacancies has effectively increased and the loss of lattice oxygen under high voltage can be suppressed. This study provides a simple method for developing high-capacity and cyclability Li-rich cathode materials for lithium-ion batteries. Oxygen release can occur at the cathode surface leading to the formation of spinel or rock salt structures. Here, it is shown that Zr doping is an effective strategy to retain lattice oxygen in lithium-rich layered oxides (LLO) due to the high affinity between Zr and O. LLO-Zr exhibit higher cycling stability, with 88% capacity retention after 300 cycles at 1 C. image
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 19
DOI: 10.1002/ADFM.202313672
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“The role of the electrode surface in Na-Air batteries : insights in electrochemical product formation and chemical growth of NaO2”. Lutz L, Corte DAD, Chen Y, Batuk D, Johnson LR, Abakumov A, Yate L, Azaceta E, Bruce PG, Tarascon J-M, Grimaud A, Advanced energy materials 8, 1701581 (2018). http://doi.org/10.1002/AENM.201701581
Abstract: The Na-air battery, because of its high energy density and low charging overpotential, is a promising candidate for low-cost energy storage, hence leading to intensive research. However, to achieve such a battery, the role of the positive electrode material in the discharge process must be understood. This issue is herein addressed by exploring the electrochemical reduction of oxygen, as well as the chemical formation and precipitation of NaO2 using different electrodes. Whereas a minor influence of the electrode surface is demonstrated on the electrochemical formation of NaO2, a strong dependence of the subsequent chemical precipitation of NaO2 is identified. In the origin, this effect stems from the surface energy and O-2/O-2(-) affinity of the electrode. The strong interaction of Au with O-2/O-2(-) increases the nucleation rate and leads to an altered growth process when compared to C surfaces. Consequently, thin (3 mu m) flakes of NaO2 are found on Au, whereas on C large cubes (10 mu m) of NaO2 are formed. This has significant impact on the cell performance and leads to four times higher capacity when C electrodes with low surface energy and O-2/O-2(-) affinity are used. It is hoped that these findings will enable the design of new positive electrode materials with optimized surfaces.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 16.721
Times cited: 13
DOI: 10.1002/AENM.201701581
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“Carbon Incorporation and Anion Dynamics as Synergistic Drivers for Ultrafast Diffusion in Superionic LiCB11H12 and NaCB11H12”. Dimitrievska M, Shea P, Kweon KE, Bercx M, Varley JB, Tang WS, Skripov AV, Stavila V, Udovic TJ, Wood BC, Advanced energy materials 8, 1703422 (2018). http://doi.org/10.1002/AENM.201703422
Abstract: The disordered phases of LiCB11H12 and NaCB11H12 possess superb superionic conductivities that make them suitable as solid electrolytes. In these materials, cation diffusion correlates with high orientational mobilities of the CB11H12- anions; however, the precise relationship has yet to be demonstrated. In this work, ab initio molecular dynamics and quasielastic neutron scattering are combined to probe anion reorientations and their mechanistic connection to cation mobility over a range of timescales and temperatures. It is found that anions do not rotate freely, but rather transition rapidly between orientations defined by the cation sublattice symmetry. The symmetry-breaking carbon atom in CB11H12- also plays a critical role by perturbing the energy landscape along the instantaneous orientation of the anion dipole, which couples fluctuations in the cation probability density directly to the anion motion. Anion reorientation rates exceed 3 x 10(10) s(-1), suggesting the underlying energy landscape fluctuates dynamically on diffusion-relevant timescales. Furthermore, carbon is found to modify the orientational preferences of the anions and aid rotational mobility, creating additional symmetry incompatibilities that inhibit ordering. The results suggest that synergy between the anion reorientational dynamics and the carbon-modified cation-anion interaction accounts for the higher ionic conductivity in CB11H12- salts compared with B12H122-.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 16.721
Times cited: 20
DOI: 10.1002/AENM.201703422
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“Single-layered imine-linked porphyrin-based two-dimensional covalent organic frameworks targeting CO₂, reduction”. Arisnabarreta N, Hao Y, Jin E, Salame A, Muellen K, Robert M, Lazzaroni R, Van Aert S, Mali KS, De Feyter S, Advanced energy materials (2024). http://doi.org/10.1002/AENM.202304371
Abstract: The reduction of carbon dioxide (CO2) using porphyrin-containing 2D covalent organic frameworks (2D-COFs) catalysts is widely explored nowadays. While these framework materials are normally fabricated as powders followed by their uncontrolled surface heterogenization or directly grown as thin films (thickness >200 nm), very little is known about the performance of substrate-supported single-layered (approximate to 0.5 nm thickness) 2D-COFs films (s2D-COFs) due to its highly challenging synthesis and characterization protocols. In this work, a fast and straightforward fabrication method of porphyrin-containing s2D-COFs is demonstrated, which allows their extensive high-resolution visualization via scanning tunneling microscopy (STM) in liquid conditions with the support of STM simulations. The as-prepared single-layered film is then employed as a cathode for the electrochemical reduction of CO2. Fe porphyrin-containing s2D-COF@graphite used as a single-layered heterogeneous catalyst provided moderate-to-high carbon monoxide selectivity (82%) and partial CO current density (5.1 mA cm(-2)). This work establishes the value of using single-layered films as heterogene ous catalysts and demonstrates the possibility of achieving high performance in CO2 reduction even with extremely low catalyst loadings.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 27.8
DOI: 10.1002/AENM.202304371
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“Nanoscale mapping by electron energy-loss spectroscopy reveals evolution of organic solar cell contact selectivity”. Guerrero A, Pfannmöller M, Kovalenko A, Ripolles TS, Heidari H, Bals S, Kaufmann L-D, Bisquert J, Garcia-Belmonte G, Organic electronics: physics, materials, applications 16, 227 (2015). http://doi.org/10.1016/j.orgel.2014.11.007
Abstract: Organic photovoltaic (OPV) devices are on the verge of commercialization being long-term stability a key challenge. Morphology evolution during lifetime has been suggested to be one of the main pathways accounting for performance degradation. There is however a lack of certainty on how specifically the morphology evolution relates to individual electrical parameters on operating devices. In this work a case study is created based on a thermodynamically unstable organic active layer which is monitored over a period of one year under non-accelerated degradation conditions. The morphology evolution is revealed by compositional analysis of ultrathin cross-sections using nanoscale imaging in scanning transmission electron microscopy (STEM) coupled with electron energy-loss spectroscopy (EELS). Additionally, devices are electrically monitored in real-time using the non-destructive electrical techniques capacitance-voltage (C-V) and Impedance Spectroscopy (IS). By comparison of imaging and electrical techniques the relationship between nanoscale morphology and individual electrical parameters of device operation can be conclusively discerned. It is ultimately observed how the change in the cathode contact properties occurring after the migration of fullerene molecules explains the improvement in the overall device performance. (C) 2014 Elsevier B.V. All rights reserved.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 3.399
Times cited: 24
DOI: 10.1016/j.orgel.2014.11.007
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“A Universal Deposition Protocol for Planar Heterojunction Solar Cells with High Efficiency Based on Hybrid Lead Halide Perovskite Families”. Conings B, Babayigit A, Klug M T, Bai S, Gauquelin N, Sakai N, Wang J T-W, Verbeeck J, Boyen H-G, Advanced materials 28, 10701 (2016). http://doi.org/10.1002/adma.201603747
Abstract: A robust and expedient gas quenching method is developed for the solution deposition of hybrid perovskite thin films. The method offers a reliable standard practice for the fabrication of a non-exhaustive variety of perovskites exhibiting excellent film morphology and commensurate high performance in both regular and inverted structured solar cell architectures.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 19.791
Times cited: 95
DOI: 10.1002/adma.201603747
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“Element Specific Monolayer Depth Profiling”. Macke S, Radi A, Hamann-Borrero JE, Verna A, Bluschke M, Brück S, Goering E, Sutarto R, He F, Cristiani G, Wu M, Benckiser E, Habermeier H-U, Logvenov G, Gauquelin N, Botton GA, Kajdos AP, Stemmer S, Sawatzky GA, Haverkort MW, Keimer B, Hinkov V, Advanced Materials 26, 6554 (2014). http://doi.org/10.1002/adma.201402028
Abstract: The electronic phase behavior and functionality of interfaces and surfaces in complex materials are strongly correlated to chemical composition profiles, stoichiometry and intermixing. Here a novel analysis scheme for resonant X-ray reflectivity maps is introduced to determine such profiles, which is element specific and non-destructive, and which exhibits atomic-layer resolution and a probing depth of hundreds of nanometers.
Keywords: A1 Journal Article; Electron Microscopy for Materials Science (EMAT)
Impact Factor: 19.791
Times cited: 34
DOI: 10.1002/adma.201402028
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“A counterion-catalyzed (S0H+)(X-I+) pathway toward heat- and steam-stable mesostructured silica assembled from amines in acidic conditions”. Cassiers K, van der Voort P, Linssen T, Vansant EF, Lebedev O, van Landuyt J, The journal of physical chemistry : B : condensed matter, materials, surfaces, interfaces and biophysical 107, 3690 (2003). http://doi.org/10.1021/jp026696v
Abstract: An alternative pathway to assemble mesoporous molecular sieve silicas is developed using nonionic alkylamines and N,N-dimethylalkylamines (SO) as structure-directing agents in acidic conditions. The synthesized mesostructures possess wormhole-like frameworks with pore sizes and pore volumes in the range of 20-90 Angstrom and 0.5-1.3 cm(3)/g, respectively. The formation of the mesophase is controlled by a counterion-mediated mechanism of the type (S(0)H(+))(X(-)I(+)), where S(0)H(+) are protonated water molecules that are hydrogen bonded to the lone electron pairs on the amine surfactant headgroups (S(0)H(+)), X(-) is the counteranion originating from the acid, and I(+) are the positively charged (protonated) silicate species. We found that the stronger the ion X(-) is bonded to S(0)H(+), the more it catalyzes the silica condensation into (S(0)H(+))(X(-)I(+)). Br(-) is shown to be a strong binding anion and therefore a fast silica polymerization promoter compared to Cl(-) resulting in the formation of a higher quality mesophase for the Br(-) syntheses. We also showed that the polymerization rate of the silica, dictated by the counterion, controls the morphology of the mesostructures from nonuniform agglomerated blocks in the case of Br(-) syntheses to spherical particles for the Cl(-) syntheses. Next to many benefits such as low temperature, short synthesis time, and the use of inexpensive, nontoxic, and easily extractable amine templates, the developed materials have a remarkable higher thermal and hydrothermal stability compared to hexagonal mesoporous silica, which is also prepared with nonionic amines but formed through the S(0)I(0) mechanism.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT); Laboratory of adsorption and catalysis (LADCA)
Impact Factor: 3.177
Times cited: 9
DOI: 10.1021/jp026696v
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“Aluminum incorporation into MCM-48 toward the creation of Brønsted acidity”. Collart O, Cool P, van der Voort P, Meynen V, Vansant EF, Houthoofd KJ, Grobet PJ, Lebedev OI, Van Tendeloo G, The journal of physical chemistry : B : condensed matter, materials, surfaces, interfaces and biophysical 108, 13905 (2004). http://doi.org/10.1021/jp049837x
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT); Laboratory of adsorption and catalysis (LADCA)
Impact Factor: 3.177
Times cited: 13
DOI: 10.1021/jp049837x
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“Hydrothermal synthesis and characterization of nanorods of various titanates and titanium dioxide”. Kolen'ko YV, Kovnir KA, Gavrilov AI, Garshev AV, Frantti J, Lebedev OI, Churagulov BR, Van Tendeloo G, Yoshimura M, The journal of physical chemistry : B : condensed matter, materials, surfaces, interfaces and biophysical 110, 4030 (2006). http://doi.org/10.1021/jp055687u
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 3.177
Times cited: 234
DOI: 10.1021/jp055687u
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“The influence of the alcohol concentration on the structural ordering of mesoporous silica: cosurfactant versus cosolvent”. Liu S, Cool P, Collart O, van der Voort P, Vansant EF, Lebedev OI, Van Tendeloo G, Jiang M, The journal of physical chemistry : B : condensed matter, materials, surfaces, interfaces and biophysical 107, 10405 (2003). http://doi.org/10.1021/jp034410w
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT); Laboratory of adsorption and catalysis (LADCA)
Impact Factor: 3.177
Times cited: 134
DOI: 10.1021/jp034410w
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“Investigation of the morphology of the mesoporous SBA-16 and SBA-15 materials”. Stevens WJJ, Lebeau K, Mertens M, Van Tendeloo G, Cool P, Vansant EF, The journal of physical chemistry : B : condensed matter, materials, surfaces, interfaces and biophysical 110, 9183 (2006). http://doi.org/10.1021/jp0548725
Keywords: A1 Journal article; Laboratory of adsorption and catalysis (LADCA); Electron microscopy for materials research (EMAT)
Impact Factor: 3.177
Times cited: 109
DOI: 10.1021/jp0548725
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“Leached natural saponite as the silicate source in the synthesis of aluminosilicate hexagonal mesoporous materials”. Linssen T, Cool P, Baroudi M, Cassiers K, Vansant EF, Lebedev O, van Landuyt J, The journal of physical chemistry : B : condensed matter, materials, surfaces, interfaces and biophysical 106, 4470 (2002). http://doi.org/10.1021/jp015578p
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT); Laboratory of adsorption and catalysis (LADCA)
Impact Factor: 3.177
Times cited: 23
DOI: 10.1021/jp015578p
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