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“Highly active, selective, and stable Pd single-atom catalyst anchored on N-doped hollow carbon sphere for electrochemical H₂O₂, synthesis under acidic conditions”. Xi J, Yang S, Silvioli L, Cao S, Liu P, Chen Q, Zhao Y, Sun H, Hansen JN, Haraldsted J-PB, Kibsgaard J, Rossmeisl J, Bals S, Wang S, Chorkendorff I, Journal Of Catalysis 393, 313 (2021). http://doi.org/10.1016/J.JCAT.2020.11.020
Abstract: Single-atom catalysts (SACs) have recently attracted broad scientific interests due to their unique structural feature, the single-atom dispersion. Optimized electronic structure as well as high stability are required for single-atom catalysts to enable efficient electrochemical production of H2O2. Herein, we report a facile synthesis method that stabilizes atomic Pd species on the reduced graphene oxide/Ndoped carbon hollow carbon nanospheres (Pd1/N-C). Pd1/N-C exhibited remarkable electrochemical H2O2 production rate with high faradaic efficiency, reaching 80%. The single-atom structure and its high H2O2 production rate were maintained even after 10,000 cycle stability test. The existence of single-atom Pd as well as its coordination with N species is responsible for its high activity, selectivity, and stability. The N coordination number and substrate doping around Pd atoms are found to be critical for an optimized adsorption energy of intermediate *OOH, resulting in efficient electrochemical H2O2 production. (C) 2020 Elsevier Inc. All rights reserved.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 6.844
Times cited: 40
DOI: 10.1016/J.JCAT.2020.11.020
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“Inverse heavy-atom effect in near infrared photoluminescent gold nanoclusters”. Pramanik G, Kvakova K, Thottappali MA, Rais D, Pfleger J, Greben M, El-Zoka A, Bals S, Dracinsky M, Valenta J, Cigler P, Nanoscale 12, 10462 (2021). http://doi.org/10.1039/D1NR90138A
Abstract: Fluorophores functionalized with heavy elements show enhanced intersystem crossing due to increased spin-orbit coupling, which in turn shortens the fluorescence decay lifetime (tau(PL)). This phenomenon is known as the heavy-atom effect (HAE). Here, we report the observation of increased tau(PL) upon functionalisation of near-infrared photoluminescent gold nanoclusters with iodine. The heavy atom-mediated increase in tau(PL) is in striking contrast with the HAE and referred to as inverse HAE. Femtosecond and nanosecond transient absorption spectroscopy revealed overcompensation of a slight decrease in lifetime of the transition associated with the Au core (ps) by a large increase in the long-lived triplet state lifetime associated with the Au shell, which contributed to the observed inverse HAE. This unique observation of inverse HAE in gold nanoclusters provides the means to enhance the triplet excited state lifetime.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 7.367
Times cited: 1
DOI: 10.1039/D1NR90138A
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“Correlating structure and detection properties in HgTe nanocrystal films”. Chee S-S, Greboval C, Vale Magalhaes D, Ramade J, Chu A, Qu J, Rastogi P, Khalili A, Dang TH, Dabard C, Prado Y, Patriarche G, Chaste J, Rosticher M, Bals S, Delerue C, Lhuillier E, Nano Letters 21, 4145 (2021). http://doi.org/10.1021/ACS.NANOLETT.0C04346
Abstract: HgTe nanocrystals (NCs) enable broadly tunable infrared absorption, now commonly used to design light sensors. This material tends to grow under multipodic shapes and does not present well-defined size distributions. Such point generates traps and reduces the particle packing, leading to a reduced mobility. It is thus highly desirable to comprehensively explore the effect of the shape on their performance. Here, we show, using a combination of electron tomography and tight binding simulations, that the charge dissociation is strong within HgTe NCs, but poorly shape dependent. Then, we design a dual-gate field-effect-transistor made of tripod HgTe NCs and use it to generate a planar p-n junction, offering more tunability than its vertical geometry counterpart. Interestingly, the performance of the tripods is higher than sphere ones, and this can be correlated with a stronger Te excess in the case of sphere shapes which is responsible for a higher hole trap density.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 12.712
Times cited: 20
DOI: 10.1021/ACS.NANOLETT.0C04346
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“Gold and silver-catalyzed reductive amination of aromatic carboxylic acids to benzylic amines”. Coeck R, Meeprasert J, Li G, Altantzis T, Bals S, Pidko EA, De Vos DE, Acs Catalysis 11, 7672 (2021). http://doi.org/10.1021/ACSCATAL.1C01693
Abstract: The reductive amination of benzoic acid and its derivatives would be an effective addition to current synthesis methods for benzylamine. However, with current technology it is very difficult to keep the aromaticity intact when starting from benzoic acid, and salt wastes are often generated in the process. Here, we report a heterogeneous catalytic system for such a reductive amination, requiring solely H-2 and NH3 as the reactants. The Ag/TiO2 or Au/TiO2 catalysts can be used multiple times, and very little noble metal is required, only 0.025 mol % Au. The catalysts are bifunctional: the support catalyzes the dehydration of both the ammonium carboxylate to the amide and of the amide to the nitrile, while the sites at the metal-support interface promote the hydrogenation of the in situ generated nitrile. Yields of up to 92% benzylamine were obtained.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT)
Impact Factor: 10.614
Times cited: 16
DOI: 10.1021/ACSCATAL.1C01693
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“Mapping composition–selectivity relationships of supported sub-10 nm Cu–Ag nanocrystals for high-rate CO₂, electroreduction”. Choukroun D, Pacquets L, Li C, Hoekx S, Arnouts S, Baert K, Hauffman T, Bals S, Breugelmans T, Acs Nano 15, 14858 (2021). http://doi.org/10.1021/ACSNANO.1C04943
Abstract: Colloidal Cu–Ag nanocrystals measuring less than 10 nm across are promising candidates for integration in hybrid CO2 reduction reaction (CO2RR) interfaces, especially in the context of tandem catalysis and selective multicarbon (C2–C3) product formation. In this work, we vary the synthetic-ligand/copper molar ratio from 0.1 to 1.0 and the silver/copper atomic ratio from 0 to 0.7 and study the variations in the nanocrystals’ size distribution, morphology and reactivity at rates of ≥100 mA cm–2 in a gas-fed recycle electrolyzer operating under neutral to mildly basic conditions (0.1–1.0 M KHCO3). High-resolution electron microscopy and spectroscopy are used in order to characterize the morphology of sub-10 nm Cu–Ag nanodimers and core–shells and to elucidate trends in Ag coverage and surface composition. It is shown that Cu–Ag nanocrystals can be densely dispersed onto a carbon black support without the need for immediate ligand removal or binder addition, which considerably facilitates their application. Although CO2RR product distribution remains an intricate function of time, (kinetic) overpotential and processing conditions, we nevertheless conclude that the ratio of oxygenates to hydrocarbons (which depends primarily on the initial dispersion of the nanocrystals and their composition) rises 3-fold at moderate Ag atom % relative to Cu NCs-based electrodes. Finally, the merits of this particular Cu–Ag/C system and the recycling reactor employed are utilized to obtain maximum C2–C3 partial current densities of 92–140 mA cm–2 at −1.15 VRHE and liquid product concentrations in excess of 0.05 wt % in 1 M KHCO3 after short electrolysis periods.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT)
Impact Factor: 13.942
Times cited: 25
DOI: 10.1021/ACSNANO.1C04943
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“State of the art and prospects for Halide Perovskite Nanocrystals”. Dey A, Ye J, De A, Debroye E, Ha SK, Bladt E, Kshirsagar AS, Wang Z, Yin J, Wang Y, Quan LN, Yan F, Gao M, Li X, Shamsi J, Debnath T, Cao M, Scheel MA, Kumar S, Steele JA, Gerhard M, Chouhan L, Xu K, Wu X-gang, Li Y, Zhang Y, Dutta A, Han C, Vincon I, Rogach AL, Nag A, Samanta A, Korgel BA, Shih C-J, Gamelin DR, Son DH, Zeng H, Zhong H, Sun H, Demir HV, Scheblykin IG, Mora-Sero I, Stolarczyk JK, Zhang JZ, Feldmann J, Hofkens J, Luther JM, Perez-Prieto J, Li L, Manna L, Bodnarchuk M I, Kovalenko M V, Roeffaers MBJ, Pradhan N, Mohammed OF, Bakr OM, Yang P, Muller-Buschbaum P, Kamat P V, Bao Q, Zhang Q, Krahne R, Galian RE, Stranks SD, Bals S, Biju V, Tisdale WA, Yan Y, Hoye RLZ, Polavarapu L, Acs Nano 15, 10775 (2021). http://doi.org/10.1021/ACSNANO.0C08903
Abstract: Metal-halide perovskites have rapidly emerged as one of the most promising materials of the 21st century, with many exciting properties and great potential for a broad range of applications, from photovoltaics to optoelectronics and photocatalysis. The ease with which metal-halide perovskites can be synthesized in the form of brightly luminescent colloidal nanocrystals, as well as their tunable and intriguing optical and electronic properties, has attracted researchers from different disciplines of science and technology. In the last few years, there has been a significant progress in the shape-controlled synthesis of perovskite nanocrystals and understanding of their properties and applications. In this comprehensive review, researchers having expertise in different fields (chemistry, physics, and device engineering) of metal-halide perovskite nanocrystals have joined together to provide a state of the art overview and future prospects of metal-halide perovskite nanocrystal research.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 13.942
Times cited: 538
DOI: 10.1021/ACSNANO.0C08903
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“Grain boundaries as a diffusion-limiting factor in lithium-rich NMC cathodes for high-energy lithium-ion batteries”. Abakumov AM, Li C, Boev A, Aksyonov DA, Savina AA, Abakumova TA, Van Tendeloo G, Bals S, ACS applied energy materials 4, 6777 (2021). http://doi.org/10.1021/ACSAEM.1C00872
Abstract: High-energy lithium-rich layered transition metal oxides are capable of delivering record electrochemical capacity and energy density as positive electrodes for Li-ion batteries. Their electrochemical behavior is extremely complex due to sophisticated interplay between crystal structure, electronic structure, and defect structure. Here we unravel an extra level of this complexity by revealing that the most typical representative Li1.2Ni0.13Mn0.54Co0.13O2 material, prepared by a conventional coprecipitation technique with Na2CO3 as a precipitating agent, contains abundant coherent (001) grain boundaries with a Na-enriched P2-structured block due to segregation of the residual sodium traces. The trigonal prismatic oxygen coordination of Na triggers multiple nanoscale twinning, giving rise to incoherent (104) boundaries. The cationic layers at the (001) grain boundaries are filled with transition metal cations being Mn-depleted and Co-enriched; this makes them virtually not permeable for the Li+ cations, and therefore they negatively influence the Li diffusion in and out of the spherical agglomerates. These results demonstrate that besides the mechanisms intrinsic to the crystal and electronic structure of Li-rich cathodes, their rate capability might also be depreciated by peculiar microstructural aspects. Dedicated engineering of grain boundaries opens a way for improving inherently sluggish kinetics of these materials.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Times cited: 4
DOI: 10.1021/ACSAEM.1C00872
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Skorikov A, Heyvaert W, Albrecht W, Pelt DM, Bals S (2021) EMAT Simulated 3D Nanoparticle Structures Dataset
Abstract: This dataset contains 1000 simulated nanoparticle-like 3D structures and noisy EDX-like elemental maps based on them. These data are intended to be used for quantitative analysis of data processing methods in (EDX) tomography of nanoparticles and training the data-driven approaches for these tasks. The dataset is structured as follows: voxel_data/clean 3D voxel grid representation of the simulated nanoparticles. Voxel intensities are adjusted so that the total intensity equals 103. All 3D structures have unique identifiers in 0..999 range. The data derived from a 3D structure preserves this unique identifier. sinograms/clean Tilt series of projection images obtained from the corresponding 3D structures over an angular range of -75..75 degrees with a tilt step of 10 degrees to simulate a typical tilt series used in EDX tomography. Total intensity in each projection image equals 103. sinograms/noisy Tilt series of projection images corrupted with Poisson noise and an additional spatially uniform background noise. projections/clean Projection images extracted from the clean tilt series at 0 degrees tilt angle. projections/noisy Projection images extracted from the noisy tilt series at 0 degrees tilt angle. images/clean Visualizations of the clean projections as PNG images with the intensity range adjusted to 0..255 images/noisy Visualizations of the noisy projections as PNG images with the intensity range adjusted to 0..255
Keywords: Dataset; Electron microscopy for materials research (EMAT)
DOI: 10.5281/zenodo.4580545
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“Phase transformation behavior of a two-dimensional zeolite”. Bae J, Cichocka MO, Zhang Y, Bacsik Z, Bals S, Zou X, Willhammar T, Hong SB, Angewandte Chemie: international edition in English 58, 10230 (2019). http://doi.org/10.1002/ANIE.201904825
Abstract: Understanding the molecular-level mechanisms of phase transformation in solids is of fundamental interest for functional materials such as zeolites. Two-dimensional (2D) zeolites, when used as shape-selective catalysts, can offer improved access to the catalytically active sites and a shortened diffusion length in comparison with their 3D analogues. However, few materials are known to maintain both their intralayer microporosity and structure during calcination for organic structure-directing agent (SDA) removal. Herein we report that PST-9, a new 2D zeolite which has been synthesized via the multiple inorganic cation approach and fulfills the requirements for true layered zeolites, can be transformed into the small-pore zeolite EU-12 under its crystallization conditions through the single-layer folding process, but not through the traditional dissolution/recrystallization route. We also show that zeolite crystal growth pathway can differ according to the type of organic SDAs employed.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Times cited: 2
DOI: 10.1002/ANIE.201904825
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“From CdSe nanoplatelets to quantum rings by thermochemical edge reconfiguration”. Salzmann BBV, Vliem JF, Maaskant DN, Post LC, Li C, Bals S, Vanmaekelbergh D, Chemistry Of Materials 33, 6853 (2021). http://doi.org/10.1021/ACS.CHEMMATER.1C01618
Abstract: The variation in the shape of colloidal semiconductor nanocrystals (NCs) remains intriguing. This interest goes beyond crystallography as the shape of the NC determines its energy levels and optoelectronic properties. While thermodynamic arguments point to a few or just a single shape(s), terminated by the most stable crystal facets, a remarkable variation in NC shape has been reported for many different compounds. For instance, for the well-studied case of CdSe, close-to-spherical quantum dots, rods, two-dimensional nanoplatelets, and quantum rings have been reported. Here, we report how two-dimensional CdSe nanoplatelets reshape into quantum rings. We monitor the reshaping in real time by combining atomically resolved structural characterization with optical absorption and photoluminescence spectroscopy. We observe that CdSe units leave the vertical sides of the edges and recrystallize on the top and bottom edges of the nanoplatelets, resulting in a thickening of the rims. The formation of a central hole, rendering the shape into a ring, only occurs at a more elevated temperature.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 9.466
Times cited: 7
DOI: 10.1021/ACS.CHEMMATER.1C01618
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“Quantitative 3D real-space analysis of Laves phase supraparticles”. Wang D, van der Wee EB, Zanaga D, Altantzis T, Wu Y, Dasgupta T, Dijkstra M, Murray CB, Bals S, van Blaaderen A, Nature Communications 12, 3980 (2021). http://doi.org/10.1038/S41467-021-24227-0
Abstract: 3D real-space analysis of thick nanoparticle crystals is non-trivial. Here, the authors demonstrate the structural analysis of a bulk-like Laves phase by imaging an off-stoichiometric binary mixture of hard-sphere-like nanoparticles in spherical confinement by electron tomography, enabling defect analysis on the single-particle level. Assembling binary mixtures of nanoparticles into crystals, gives rise to collective properties depending on the crystal structure and the individual properties of both species. However, quantitative 3D real-space analysis of binary colloidal crystals with a thickness of more than 10 layers of particles has rarely been performed. Here we demonstrate that an excess of one species in the binary nanoparticle mixture suppresses the formation of icosahedral order in the self-assembly in droplets, allowing the study of bulk-like binary crystal structures with a spherical morphology also called supraparticles. As example of the approach, we show single-particle level analysis of over 50 layers of Laves phase binary crystals of hard-sphere-like nanoparticles using electron tomography. We observe a crystalline lattice composed of a random mixture of the Laves phases. The number ratio of the binary species in the crystal lattice matches that of a perfect Laves crystal. Our methodology can be applied to study the structure of a broad range of binary crystals, giving insights into the structure formation mechanisms and structure-property relations of nanomaterials.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT)
Impact Factor: 12.124
Times cited: 10
DOI: 10.1038/S41467-021-24227-0
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“Kinetic regulation of the synthesis of pentatwinned gold nanorods below room temperature”. Sanchez-Iglesias A, Jenkinson K, Bals S, Liz-Marzan LM, Journal Of Physical Chemistry C 125, 23937 (2021). http://doi.org/10.1021/ACS.JPCC.1C07284
Abstract: The synthesis of gold nanorods requires the presence of symmetry-breaking and shape-directing additives, among which bromide ions and quaternary ammonium surfactants have been reported as essential. As a result, hexadecyltrimethylammonium bromide (CTAB) has been selected as the most efficient surfactant to direct anisotropic growth. One of the difficulties arising from this selection is the low solubility of CTAB in water at room temperature, and therefore the seeded growth of gold nanorods is usually performed at 25 degrees C or above, which has restricted so far the analysis of kinetic effects derived from lower temperatures. We report a systematic study of the synthesis of gold nanorods from pentatwinned seeds using hexadecyltrimethylammonium chloride (CTAC) as the principal surfactant and a low concentration of bromide as shape-directing agent. Under these conditions, the synthesis can be performed at temperatures as low as 8 degrees C, and the corresponding kinetic effects can be studied, resulting in temperature-controlled aspect ratio tunability.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 4.536
Times cited: 6
DOI: 10.1021/ACS.JPCC.1C07284
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“Catalytic upcycling of PVC waste-derived phthalate esters into safe, hydrogenated plasticizers”. Windels S, Diefenhardt T, Jain N, Marquez C, Bals S, Schlummer M, De Vos DE, Green chemistry : cutting-edge research for a greener sustainable future 24, 754 (2022). http://doi.org/10.1039/D1GC03864H
Abstract: Recycling of end-of-life polyvinyl chloride (PVC) calls for solutions to deal with the vast amounts of harmful phthalate plasticizers that have historically been incorporated in PVC. Here, we report on the upcycling of such waste-extracted phthalate esters into analogues of the much safer diisononyl 1,2-cyclohexanedicarboxylate plasticizer (DINCH), via a catalytic one-pot (trans)esterification-hydrogenation process. For most of the virgin phthalates, Ru/Al2O3 is a highly effective hydrogenation catalyst, yielding >99% ring-hydrogenated products under mild reaction conditions (0.1 mol% Ru, 80 degrees C, 50 bar H-2). However, applying this reaction to PVC-extracted phthalates proved problematic, (1) as benzyl phthalates are hydrogenolyzed to benzoic acids that inhibit the Ru-catalyst, and (2) because impurities in the plasticizer extract (PVC, sulfur) further retard the hydrogenation. These complications were solved by coupling the hydrogenation to an in situ (trans)esterification with a higher alcohol, and by pretreating the extract with an activated carbon adsorbent. In this way, a real phthalate extract obtained from post-consumer PVC waste was eventually completely (>99%) hydrogenated to phthalate-free, cycloaliphatic plasticizers.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 9.8
Times cited: 8
DOI: 10.1039/D1GC03864H
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“Cyan emission in two-dimensional colloidal Cs2CdCl4:SB3+ Ruddlesden-Popper phase nanoplatelets”. Locardi F, Samoli M, Martinelli A, Erdem O, Vale Magalhaes D, Bals S, Hens Z, Acs Nano 15, 17729 (2021). http://doi.org/10.1021/ACSNANO.1C05684
Abstract: Metal halide perovskites are one of the most investigated materials in optoelectronics, with their lead-based counterparts being renowned for their enhanced optoelectronic performance. The 3D CsPbX3 structure has set the standard with many studies currently attempting to substitute lead with other metals while retaining the properties of this material. This effort has led to the fabrication of metal halides with lower dimensionality, wherein particular 2D layered perovskite structures have captured attention as inspiration for the next generation of colloidal semiconductors. Here we report the synthesis of the Ruddlesden-Popper Cs2CdCl4:Sb3+ phase as colloidal nanoplatelets (NPs) using a facile hot injection approach under atmospheric conditions. Through strict adjustment of the synthesis parameters with emphasis on the ligand ratio, we obtained NPs with a relatively uniform size and good morphological control. The particles were characterized through transmission electron microscopy, synchrotron X-ray diffraction, and pair distribution function analysis. The spectroscopic characterization revealed most strikingly an intense cyan emission under UV excitation with a measured PLQY of similar to 20%. The emission was attributed to the Sb3+-doping within the structure.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 13.942
Times cited: 34
DOI: 10.1021/ACSNANO.1C05684
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“Shape control beyond the seeds in gold nanoparticles”. Li W, Tong W, Yadav A, Bladt E, Bals S, Funston AM, Etheridge J, Chemistry Of Materials 33, 9152 (2021). http://doi.org/10.1021/ACS.CHEMMATER.1C02459
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.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 9.466
Times cited: 3
DOI: 10.1021/ACS.CHEMMATER.1C02459
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“Metal-polymer heterojunction in colloidal-phase plasmonic catalysis”. Rogolino A, Claes N, Cizaurre J, Marauri A, Jumbo-Nogales A, Lawera Z, Kruse J, Sanroman-Iglesias M, Zarketa I, Calvo U, Jimenez-Izal E, Rakovich YP, Bals S, Matxain JM, Grzelczak M, The journal of physical chemistry letters 13, 2264 (2022). http://doi.org/10.1021/ACS.JPCLETT.1C04242
Abstract: Plasmonic catalysis in the colloidal phase requires robust surface ligands that prevent particles from aggregation in adverse chemical environments and allow carrier flow from reagents to nanoparticles. This work describes the use of a water-soluble conjugated polymer comprising a thiophene moiety as a surface ligand for gold nanoparticles to create a hybrid system that, under the action of visible light, drives the conversion of the biorelevant NAD+ to its highly energetic reduced form NADH. A combination of advanced microscopy techniques and numerical simulations revealed that the robust metal-polymer heterojunction, rich in sulfonate functional groups, directs the interaction of electron-donor molecules with the plasmonic photocatalyst. The tight binding of polymer to the gold surface precludes the need for conventional transition-metal surface cocatalysts, which were previously shown to be essential for photocatalytic NAD(+) reduction but are known to hinder the optical properties of plasmonic nanocrystals. Moreover, computational studies indicated that the coating polymer fosters a closer interaction between the sacrificial electron-donor triethanolamine and the nanoparticles, thus enhancing the reactivity.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 5.7
Times cited: 1
DOI: 10.1021/ACS.JPCLETT.1C04242
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“Chemistry, local molybdenum clustering, and electrochemistry in the Li2+xMo1-xO3 solid solutions”. Savina AA, Saiutina VV, Morozov AV, Boev AO, Aksyonov DA, Dejoie C, Batuk M, Bals S, Hadermann J, Abakumov AM, Inorganic chemistry 61, 5637 (2022). http://doi.org/10.1021/ACS.INORGCHEM.2C00420
Abstract: A broad range of cationic nonstoichiometry has been demonstratedfor the Li-rich layered rock-salt-type oxide Li2MoO3, which has generally been considered as a phase with a well-defined chemical composition. Li2+xMo1-xO3(-0.037 <= x <= 0.124) solid solutions were synthesized via hydrogen reduction ofLi2MoO4in the temperature range of 650-1100 degrees C, withxdecreasing with theincrease of the reduction temperature. The solid solutions adopt a monoclinicallydistorted O3-type layered average structure and demonstrate a robust localordering of the Li cations and Mo3triangular clusters within the mixed Li/Mocationic layers. The local structure was scrutinized in detail by electron diffractionand aberration-corrected scanning transmission electron microcopy (STEM),resulting in an ordering model comprising a uniform distribution of the Mo3clusters compatible with local electroneutrality and chemical composition. The geometry of the triangular clusters with their oxygenenvironment (Mo3O13groups) has been directly visualized using differential phase contrast STEM imaging. The established localstructure was used as input for density functional theory (DFT)-based calculations; they support the proposed atomic arrangementand provide a plausible explanation for the staircase galvanostatic charge profiles upon electrochemical Li+extraction fromLi2+xMo1-xO3in Li cells. According to DFT, all electrochemical capacity in Li2+xMo1-xO3solely originates from the cationic Moredox process, which proceeds via oxidation of the Mo3triangular clusters into bent Mo3chains where the electronic capacity of the clusters depends on the initial chemical composition and Mo oxidation state defining the width of the first charge low-voltageplateau. Further oxidation at the high-voltage plateau proceeds through decomposition of the Mo3chains into Mo2dimers and further into individual Mo6+cations
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 4.6
Times cited: 3
DOI: 10.1021/ACS.INORGCHEM.2C00420
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“Use of nanoscale carbon layers on Ag-based gas diffusion electrodes to promote CO production”. Pacquets L, Van den Hoek J, Arenas Esteban D, Ciocarlan R-G, Cool P, Baert K, Hauffman T, Daems N, Bals S, Breugelmans T, ACS applied nano materials 5, 7723 (2022). http://doi.org/10.1021/ACSANM.2C00473
Abstract: A promising strategy for the inhibition of the hydrogen evolution reaction along with the stabilization of the electrocatalyst in electrochemical CO2 reduction cells involves the application of a nanoscale amorphous carbon layer on top of the active catalyst layer in a gas diffusion electrode. Without modifying the chemical nature of the electrocatalyst itself, these amorphous carbon layers lead to the stabilization of the electrocatalyst, and a significant improvement with respect to the inhibition of the hydrogen evolution reaction was also obtained. The faradaic efficiencies of hydrogen could be reduced from 31.4 to 2.1% after 1 h of electrolysis with a 5 nm thick carbon layer. Furthermore, the impact of the carbon layer thickness (5–30 nm) on this inhibiting effect was investigated. We determined an optimal thickness of 15 nm where the hydrogen evolution reaction was inhibited and a decent stability was obtained. Next, a thickness of 15 nm was selected for durability measurements. Interestingly, these durability measurements revealed the beneficial impact of the carbon layer already after 6 h by suppressing the hydrogen evolution such that an increase of only 37.9% exists compared to 56.9% without the use of an additional carbon layer, which is an improvement of 150%. Since carbon is only applied afterward, it reveals its great potential in terms of electrocatalysis in general.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Laboratory of adsorption and catalysis (LADCA); Applied Electrochemistry & Catalysis (ELCAT)
Impact Factor: 5.9
Times cited: 3
DOI: 10.1021/ACSANM.2C00473
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“Self-assembled ligand-capped plasmonic Au nanoparticle films in the Kretschmann configuration for sensing of volatile organic compounds”. Borah R, Smets J, Ninakanti R, Tietze ML, Ameloot R, Chigrin DN, Bals S, Lenaerts S, Verbruggen SW, ACS applied nano materials 5, acsanm.2c02524 (2022). http://doi.org/10.1021/ACSANM.2C02524
Abstract: Films of close-packed Au nanoparticles are coupled electrodynamically through their collective plasmon resonances. This collective optical response results in enhanced light–matter interactions, which can be exploited in various applications. Here, we demonstrate their application in sensing volatile organic compounds, using methanol as a test case. Ordered films over several cm2 were obtained by interfacial self-assembly of colloidal Au nanoparticles (∼10 nm diameter) through controlled evaporation of the solvent. Even though isolated nanoparticles of this size are inherently nonscattering, when arranged in a close-packed film the plasmonic coupling results in a strong reflectance and absorbance. The in situ tracking of vapor phase methanol concentration through UV–vis transmission measurements of the nanoparticle film is first demonstrated. Next, in situ ellipsometry of the self-assembled films in the Kretschmann (also known as ATR) configuration is shown to yield enhanced sensitivity, especially with phase difference measurements, Δ. Our study shows the excellent agreement between theoretical models of the spectral response of self-assembled films with experimental in situ sensing experiments. At the same time, the theoretical framework provides the basis for the interpretation of the various observed experimental trends. Combining periodic nanoparticle films with ellipsometry in the Kretschmann configuration is a promising strategy toward highly sensitive and selective plasmonic thin-film devices based on colloidal fabrication methods for volatile organic compound (VOC) sensing applications.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Sustainable Energy, Air and Water Technology (DuEL)
Impact Factor: 5.9
Times cited: 11
DOI: 10.1021/ACSANM.2C02524
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“Shuffling atomic layer deposition gas sequences to modulate bimetallic thin films and nanoparticle properties”. Filez M, Feng J-Y, Minjauw MM, Solano E, Poonkottil N, Van Daele M, Ramachandran RK, Li C, Bals S, Poelman H, Detavernier C, Dendooven J, Filez M, Minjauw M, Solano E, Poonkottil N, Li C, Bals S, Dendooven J, Chemistry of materials (2022). http://doi.org/10.1021/acs.chemmater.2c01304
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.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Times cited: 2
DOI: 10.1021/acs.chemmater.2c01304
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“Quantitatively linking morphology and optical response of individual silver nanohedra”. Wang Y, Sztranyovszky Z, Zilli A, Albrecht W, Bals S, Borri P, Langbein W, Nanoscale 14, 11028 (2022). http://doi.org/10.1039/D2NR02131E
Abstract: The optical response of metal nanoparticles is governed by plasmonic resonances, which are dictated by the particle morphology. A thorough understanding of the link between morphology and optical response requires quantitatively measuring optical and structural properties of the same particle. Here we present such a study, correlating electron tomography and optical micro-spectroscopy. The optical measurements determine the scattering and absorption cross-section spectra in absolute units, and electron tomography determines the 3D morphology. Numerical simulations of the spectra for the individual particle geometry, and the specific optical set-up used, allow for a quantitative comparison including the cross-section magnitude. Silver nanoparticles produced by photochemically driven colloidal synthesis, including decahedra, tetrahedra and bi-tetrahedra are investigated. A mismatch of measured and simulated spectra is found in some cases when assuming pure silver particles, which is explained by the presence of a few atomic layers of tarnish on the surface, not evident in electron tomography. The presented method tightens the link between particle morphology and optical response, supporting the predictive design of plasmonic nanomaterials.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 6.7
Times cited: 1
DOI: 10.1039/D2NR02131E
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“Multimode electron tomography sheds light on synthesis, structure, and properties of complex metal-based nanoparticles”. Jenkinson K, Liz-Marzan LM, Bals S, Advanced materials 34, 2110394 (2022). http://doi.org/10.1002/ADMA.202110394
Abstract: Electron tomography has become a cornerstone technique for the visualization of nanoparticle morphology in three dimensions. However, to obtain in-depth information about a nanoparticle beyond surface faceting and morphology, different electron microscopy signals must be combined. The most notable examples of these combined signals include annular dark-field scanning transmission electron microscopy (ADF-STEM) with different collection angles and the combination of ADF-STEM with energy-dispersive X-ray or electron energy loss spectroscopies. Here, the experimental and computational development of various multimode tomography techniques in connection to the fundamental materials science challenges that multimode tomography has been instrumental to overcoming are summarized. Although the techniques can be applied to a wide variety of compositions, the study is restricted to metal and metal oxide nanoparticles for the sake of simplicity. Current challenges and future directions of multimode tomography are additionally discussed.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 29.4
Times cited: 10
DOI: 10.1002/ADMA.202110394
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“Fast A-site cation cross-exchange at room temperature : single-to double- and triple-cation halide perovskite nanocrystals”. Otero-Martinez C, Imran M, Schrenker NJ, Ye J, Ji K, Rao A, Stranks SD, Hoye RLZ, Bals S, Manna L, Perez-Juste J, Polavarapu L, Angewandte Chemie: international edition in English 61, e202205617 (2022). http://doi.org/10.1002/ANIE.202205617
Abstract: We report here fast A-site cation cross-exchange between APbX(3) perovskite nanocrystals (NCs) made of different A-cations (Cs (cesium), FA (formamidinium), and MA (methylammonium)) at room temperature. Surprisingly, the A-cation cross-exchange proceeds as fast as the halide (X=Cl, Br, or I) exchange with the help of free A-oleate complexes present in the freshly prepared colloidal perovskite NC solutions. This enabled the preparation of double (MACs, MAFA, CsFA)- and triple (MACsFA)-cation perovskite NCs with an optical band gap that is finely tunable by their A-site composition. The optical spectroscopy together with structural analysis using XRD and atomically resolved high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) and integrated differential phase contrast (iDPC) STEM indicates the homogeneous distribution of different cations in the mixed perovskite NC lattice. Unlike halide ions, the A-cations do not phase-segregate under light illumination.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 16.6
Times cited: 28
DOI: 10.1002/ANIE.202205617
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“Halide perovskites as disposable epitaxial templates for the phase-selective synthesis of lead sulfochloride nanocrystals”. Toso S, Imran M, Mugnaioli E, Moliterni A, Caliandro R, Schrenker NJ, Pianetti A, Zito J, Zaccaria F, Wu Y, Gemmi M, Giannini C, Brovelli S, Infante I, Bals S, Manna L, Nature communications 13, 3976 (2022). http://doi.org/10.1038/S41467-022-31699-1
Abstract: Colloidal chemistry grants access to a wealth of materials through simple and mild reactions. However, even few elements can combine in a variety of stoichiometries and structures, potentially resulting in impurities or even wrong products. Similar issues have been long addressed in organic chemistry by using reaction-directing groups, that are added to a substrate to promote a specific product and are later removed. Inspired by such approach, we demonstrate the use of CsPbCl3 perovskite nanocrystals to drive the phase-selective synthesis of two yet unexplored lead sulfochlorides: Pb3S2Cl2 and Pb4S3Cl2. When homogeneously nucleated in solution, lead sulfochlorides form Pb3S2Cl2 nanocrystals. Conversely, the presence of CsPbCl3 triggers the formation of Pb4S3Cl2/CsPbCl3 epitaxial heterostructures. The phase selectivity is guaranteed by the continuity of the cationic subnetwork across the interface, a condition not met in a hypothetical Pb3S2Cl2/CsPbCl3 heterostructure. The perovskite domain is then etched, delivering phase-pure Pb4S3Cl2 nanocrystals that could not be synthesized directly. Phase-selective approaches, such using reaction-directing groups, are often seen in traditional organic chemistry and catalysis. Here authors use perovskite nanocrystals as disposable templates to drive the phase-selective synthesis of two colloidal nanomaterials, the lead sulfohalides Pb3S2Cl2 and Pb4S3Cl2.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 16.6
Times cited: 15
DOI: 10.1038/S41467-022-31699-1
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“Photochemical production of hydrogen peroxide by digging pro-superoxide radical carbon vacancies in carbon nitride”. Ding Y, Maitra S, Arenas Esteban D, Bals S, Vrielinck H, Barakat T, Roy S, Van Tendeloo G, Liu J, Li Y, Vlad A, Su B-L, Cell reports physical science 3, 100874 (2022). http://doi.org/10.1016/J.XCRP.2022.100874
Abstract: Artificial photosynthesis of H2O2, an environmentally friendly oxidant and a clean fuel, holds great promise. However, improving its efficiency and stability for industrial implementation remains highly challenging. Here, we report the visible-light H2O2 artificial photosynthesis by digging pro-superoxide radical carbon vacancies in three-dimensional hierarchical porous g-C3N4 through a simple hydrolysis-freeze-drying-thermal treatment. A significant electronic structure change is revealed upon the implantation of carbon vacancies, broadening visible-light absorption and facilitating the photogenerated charge separation. The strong electron affinity of the carbon vacancies promotes superoxide radical (O-center dot(2)-) formation, significantly boosting the H2O2 photocatalytic production. The developed photocatalyst shows an H2O2 evolution rate of 6287.5 mM g(-1) h(-1) under visible-light irradiation with a long cycling stability being the best-performing photocatalyst among all reported g-C3N4-based systems. Our work provides fundamental insight into highly active and stable photocatalysts with great potential for safe industrial H2O2 production.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Times cited: 12
DOI: 10.1016/J.XCRP.2022.100874
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“Waste-derived copper-lead electrocatalysts for CO₂, reduction”. Yang S, An H, Anastasiadou D, Xu W, Wu L, Wang H, de Ruiter J, Arnouts S, Figueiredo MC, Bals S, Altantzis T, van der Stam W, Weckhuysen BM, ChemCatChem 14, e202200754 (2022). http://doi.org/10.1002/CCTC.202200754
Abstract: It remains a real challenge to control the selectivity of the electrocatalytic CO2 reduction (eCO(2)R) reaction to valuable chemicals and fuels. Most of the electrocatalysts are made of non-renewable metal resources, which hampers their large-scale implementation. Here, we report the preparation of bimetallic copper-lead (CuPb) electrocatalysts from industrial metallurgical waste. The metal ions were extracted from the metallurgical waste through simple chemical treatment with ammonium chloride, and CuxPby electrocatalysts with tunable compositions were fabricated through electrodeposition at varying cathodic potentials. X-ray spectroscopy techniques showed that the pristine electrocatalysts consist of Cu-0, Cu1+ and Pb2+ domains, and no evidence for alloy formation was found. We found a volcano-shape relationship between eCO(2)R selectivity toward two electron products, such as CO, and the elemental ratio of Cu and Pb. A maximum Faradaic efficiency towards CO was found for Cu9.00Pb1.00, which was four times higher than that of pure Cu, under the same electrocatalytic conditions. In situ Raman spectroscopy revealed that the optimal amount of Pb effectively improved the reducibility of the pristine Cu1+ and Pb2+ domains to metallic Cu and Pb, which boosted the selectivity towards CO by synergistic effects. This work provides a framework of thinking to design and tune the selectivity of bimetallic electrocatalysts for CO2 reduction through valorization of metallurgical waste.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT)
Impact Factor: 4.5
Times cited: 7
DOI: 10.1002/CCTC.202200754
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“Plasmon resonance of gold and silver nanoparticle arrays in the Kretschmann (attenuated total reflectance) vs. direct incidence configuration”. Borah R, Ninakanti R, Bals S, Verbruggen SW, Scientific reports 12, 15738 (2022). http://doi.org/10.1038/S41598-022-20117-7
Abstract: While the behaviour of plasmonic solid thin films in the Kretschmann (also known as Attenuated Total Reflection, ATR) configuration is well-understood, the use of discrete nanoparticle arrays in this optical configuration is not thoroughly explored. It is important to do so, since close packed plasmonic nanoparticle arrays exhibit exceptionally strong light-matter interactions by plasmonic coupling. The present work elucidates the optical properties of plasmonic Au and Ag nanoparticle arrays in both the direct normal incidence and Kretschmann configuration by numerical models, that are validated experimentally. First, hexagonal close packed Au and Ag nanoparticle films/arrays are obtained by air–liquid interfacial assembly. The numerical models for the rigorous solution of the Maxwell’s equations are validated using experimental optical spectra of these films before systematically investigating various parameters. The individual far-field/near-field optical properties, as well as the plasmon relaxation mechanism of the nanoparticles, vary strongly as the packing density of the array increases. In the Kretschmann configuration, the evanescent fields arising from p – and s -polarized (or TM and TE polarized) incidence have different directional components. The local evanescent field intensity and direction depends on the polarization, angle of incidence and the wavelength of incidence. These factors in the Kretschmann configuration give rise to interesting far-field as well as near-field optical properties. Overall, it is shown that plasmonic nanoparticle arrays in the Kretschmann configuration facilitate strong broadband absorptance without transmission losses, and strong near-field enhancement. The results reported herein elucidate the optical properties of self-assembled nanoparticle films, pinpointing the ideal conditions under which the normal and the Kretschmann configuration can be exploited in multiple light-driven applications.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Sustainable Energy, Air and Water Technology (DuEL)
Impact Factor: 4.6
Times cited: 11
DOI: 10.1038/S41598-022-20117-7
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“Structural diversity in three-dimensional self-assembly of nanoplatelets by spherical confinement”. Wang D, Hermes M, Najmr S, Tasios N, Grau-Carbonell A, Liu Y, Bals S, Dijkstra M, Murray CB, van Blaaderen A, Nature communications 13, 6001 (2022). http://doi.org/10.1038/S41467-022-33616-Y
Abstract: Nanoplatelets offer many possibilities to construct advanced materials due to new properties associated with their (semi)two-dimensional shapes. However, precise control of both positional and orientational order of the nanoplatelets in three dimensions, which is required to achieve emerging and collective properties, is challenging to realize. Here, we combine experiments, advanced electron tomography and computer simulations to explore the structure of supraparticles self-assembled from nanoplatelets in slowly drying emulsion droplets. We demonstrate that the rich phase behaviour of nanoplatelets, and its sensitivity to subtle changes in shape and interaction potential can be used to guide the self-assembly into a wide range of different structures, offering precise control over both orientation and position order of the nanoplatelets. Our research is expected to shed light on the design of hierarchically structured metamaterials with distinct shape- and orientation- dependent properties. Nanoplatelets can be used as anisotropic building blocks for constructing novel optoelectronic materials. Here, Wang et al. show a route of assembling nanoplatelets with controllable positional and orientational order in three dimensions facilitated by the surface tension of drying emulsion droplets.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 16.6
Times cited: 7
DOI: 10.1038/S41467-022-33616-Y
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“Color-switchable nanosilicon fluorescent probes”. Chen H, Xu J, Wang Y, Wang D, Ferrer-Espada R, Wang Y, Zhou J, Pedrazo-Tardajos A, Yang M, Tan J-H, Yang X, Zhang L, Sychugov I, Chen S, Bals S, Paulsson J, Yang Z, ACS nano 16, 15450 (2022). http://doi.org/10.1021/ACSNANO.2C07443
Abstract: Fluorescent probes are vital to cell imaging by allowing specific parts of cells to be visualized and quantified. Color-switchable probes (CSPs), with tunable emission wavelength upon contact with specific targets, are particularly powerful because they not only eliminate the need to wash away all unbound probe but also allow for internal controls of probe concentrations, thereby facilitating quantification. Several such CSPs exist and have proven very useful, but not for all key cellular targets. Here we report a pioneering CSP for in situ cell imaging using aldehydefunctionalized silicon nanocrystals (SiNCs) that switch their intrinsic photoluminescence from red to blue quickly when interacting with amino acids in live cells. Though conventional probes often work better in cell-free extracts than in live cells, the SiNCs display the opposite behavior and function well and fast in universal cell lines at 37 ? while requiring much higher temperature in extracts. Furthermore, the SiNCs only disperse in cytoplasm not nucleus, and their fluorescence intensity correlated linearly with the concentration of fed amino acids. We believe these nanosilicon probes will be promising tools to visualize distribution of amino acids and potentially quantify amino acid related processes in live cells.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 17.1
Times cited: 1
DOI: 10.1021/ACSNANO.2C07443
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“Extracting pure circular dichroism from hierarchically structured CdS magic cluster films”. Yao Y, Ugras TJ, Meyer T, Dykes M, Wang D, Arbe A, Bals S, Kahr B, Robinson RD, ACS nano 16, 20457 (2022). http://doi.org/10.1021/ACSNANO.2C06730
Abstract: Chiroptically active, hierarchically structured materials are difficult to accurately characterize due to linear anisotropic contributions (i.e., linear dichroism (LD) and linear birefringence (LB)) and parasitic ellipticities that produce artifactual circular dichroism (CD) signals, in addition to chiral analyte contributions ranging from molecular-scale clusters to micron-sized assemblies. Recently, we have shown that CdS magic-sized clusters (MSC) can self-assemble into ordered films that have a hierarchical structure spanning seven orders of length-scale. These films have a strong CD response, but the chiral origins are obfuscated by the hierarchical architecture and LDLB contributions. Here, we derive and demonstrate a method for extracting the “pure” CD signal (CD generated by structural dissymmetry) from hierarchical MSC films and identified the chiral origin. The theory behind the method is derived using Mueller matrix and Stokes vector conventions and verified experimentally before being applied to hierarchical MSC and nanoparticle films with varying macroscopic orderings. Each film's extracted “true CD” shares a bisignate profile aligned with the exciton peak, indicating the assemblies adopt a chiral arrangement and form an exciton coupled system. Interestingly, the linearly aligned MSC film possesses one of the highest g-factors (0.05) among semiconducting nanostructures reported. Additionally, we find that films with similar electronic transition dipole alignment can possess greatly different g-factors, indicating chirality change rather than anisotropy is the cause of the difference in the CD signal. The difference in g-factor is controllable via film evaporation geometry. This study provides a simple means to measure “true” CD and presents an example of experimentally understanding chiroptic interactions in hierarchical nanostructures.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 17.1
Times cited: 8
DOI: 10.1021/ACSNANO.2C06730
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