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Multi-step nucleation of nanocrystals in aqueous solution
Duane Loh,Soumyo Sen,Michael Bosman,Shu Fen Tan,Jun Zhong,Christian A. Nijhuis,Petr Král,Paul Matsudaira,Utkur Mirsaidov +8 more
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TLDR
In situ electron microscopy is used to show how gold and silver nanocrystals nucleate from supersaturated aqueous solutions in three distinct steps: spinodal decomposition into solute-rich andsolute-poor liquid phases, nucleation of amorphous nanoclusters within the metal-rich liquid phase, followed by crystallization of theseAmorphous clusters.Abstract:
Nucleation and growth of solids from solutions impacts many natural processes and are fundamental to applications in materials engineering and medicine. For a crystalline solid, the nucleus is a nanoscale cluster of ordered atoms, which forms through mechanisms that are still poorly understood. These mechanisms have important consequences on the morphology and nucleation rates of the resultant crystals but it is unclear whether a nucleus forms spontaneously from solution in a single step or through multiple steps. Using in-situ electron microscopy, we observe and quantify how gold and silver nanocrystals nucleate from a supersaturated aqueous gold and silver solution in three distinct steps: (I) spinodal decomposition into solute-rich and solute-poor liquid phases, (II) nucleation of amorphous gold nanoclusters within the gold-rich liquid phase, followed by (III) crystallization of these amorphous clusters. Our ab-initio calculations on gold nucleation suggest that these steps might be associated with strong gold-gold atom coupling and water-mediated metastable gold complexes. The understanding of intermediate steps in nuclei formation has important implications for the formation and growth of both crystalline and amorphous materials.read more
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Observation of Single Colloidal Platinum Nanocrystal Growth Trajectories
TL;DR: In this article, the authors used in situ transmission electron microscopy to show that platinum nanocrystals can grow either by monomer attachment from solution onto the existing particles or by coalescence between the particles.
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Iced photochemical reduction to synthesize atomically dispersed metals by suppressing nanocrystal growth
Hehe Wei,Kai Huang,Da Wang,Ruoyu Zhang,Binghui Ge,Jingyuan Ma,Bo Wen,Shuai Zhang,Qunyang Li,Ming Lei,Cheng Zhang,Joshua Irawan,Li-Min Liu,Hui Wu +13 more
TL;DR: A facile approach is demonstrated to generate atomically dispersed platinum via photochemical reduction of frozen chloroplatinic acid solution using ultraviolet light to obtain atomically-dispersed platinum catalysts with high electrocatalytic performance.
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Noble-Metal Nanocrystals with Controlled Shapes for Catalytic and Electrocatalytic Applications.
TL;DR: This review article provides a comprehensive account of recent progress in the development of noble-metal nanocrystals with controlled shapes, in addition to their remarkable performance in a large number of catalytic and electrocatalytic reactions.
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Understanding active species in catalytic transformations: From molecular catalysis to nanoparticles, leaching, “Cocktails” of catalysts and dynamic systems
TL;DR: In this paper, the role of catalyst evolution and the mechanistic picture of cocktail-type systems are considered from the perspective of the development of a new generation of efficient, selective and re-usable catalysts for synthetic applications.
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Particle mesh Ewald: An N⋅log(N) method for Ewald sums in large systems
TL;DR: An N⋅log(N) method for evaluating electrostatic energies and forces of large periodic systems is presented based on interpolation of the reciprocal space Ewald sums and evaluation of the resulting convolutions using fast Fourier transforms.
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All-atom empirical potential for molecular modeling and dynamics studies of proteins.
Alexander D. MacKerell,D. Bashford,M. Bellott,Roland L. Dunbrack,Jeffrey D. Evanseck,Martin J. Field,Stefan Fischer,Jiali Gao,H. Guo,S. Ha,Diane Joseph-McCarthy,L. Kuchnir,K. Kuczera,F. T. K. Lau,C. Mattos,Stephen W. Michnick,Thien H. Ngo,D. T. Nguyen,B. Prodhom,W. E. Reiher,Benoît Roux,M. Schlenkrich,Jeremy C. Smith,Roland H. Stote,John E. Straub,Masakatsu Watanabe,J. Wiórkiewicz-Kuczera,D. Yin,Martin Karplus +28 more
TL;DR: The results demonstrate that use of ab initio structural and energetic data by themselves are not sufficient to obtain an adequate backbone representation for peptides and proteins in solution and in crystals.