Multistep nucleation of nanocrystals in aqueous solution
N. Duane Loh,Soumyo Sen,Michel Bosman,Michel Bosman,Shu Fen Tan,Jun Zhong,Christian A. Nijhuis,Petr Král,Paul Matsudaira,Utkur Mirsaidov +9 more
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TLDR
In this paper, the authors used in situ electron microscopy to show how gold and silver nanocrystals nucleate from supersaturated aqueous solutions in three distinct steps: spinodal decomposition into solute-rich and solutepoor liquid phases, nucleation of amorphous nanoclusters within the metal-rich liquid phase, followed by crystallization of these amomorphous clusters.Abstract:
The nucleation and growth of solids from solutions impacts many natural processes and is fundamental to applications in materials engineering and medicine. For a crystalline solid, the nucleus is a nanoscale cluster of ordered atoms that forms through mechanisms still poorly understood. In particular, it is unclear whether a nucleus forms spontaneously from solution via a single- or multiple-step process. Here, using in situ electron microscopy, we show how gold and silver nanocrystals nucleate from supersaturated aqueous solutions in three distinct steps: spinodal decomposition into solute-rich and solute-poor liquid phases, nucleation of amorphous nanoclusters within the metal-rich liquid phase, followed by 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
Citations
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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.
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Understanding active species in catalytic transformations: From molecular catalysis to nanoparticles, leaching, “Cocktails” of catalysts and dynamic systems
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Nanoparticle Characterization: What to Measure?
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Liquid-liquid phase separation during amphiphilic self-assembly.
Alessandro Ianiro,Hanglong Wu,Mark M. J. van Rijt,M. Paula Vena,Arthur D. A. Keizer,A. Catarina C. Esteves,Remco Tuinier,Heiner Friedrich,Nico A. J. M. Sommerdijk,Joseph P. Patterson +9 more
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References
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Free Energy of a Nonuniform System. III. Nucleation in a Two‐Component Incompressible Fluid
John W. Cahn,John E. Hilliard +1 more
TL;DR: In this article, the saddle point in the expression derived in Paper I (see reference 8) for the free energy of a nonuniform system was used to derive the properties of a critical nucleus in a two-component metastable fluid.
Journal ArticleDOI
Crystallization by particle attachment in synthetic, biogenic, and geologic environments
James J. De Yoreo,James J. De Yoreo,Pupa U. P. A. Gilbert,Pupa U. P. A. Gilbert,Nico A. J. M. Sommerdijk,R. Lee Penn,Stephen Whitelam,Derk Joester,Hengzhong Zhang,Jeffrey D. Rimer,Alexandra Navrotsky,Jillian F. Banfield,Adam F. Wallace,F. Marc Michel,Fiona C. Meldrum,Helmut Cölfen,Patricia M. Dove +16 more
TL;DR: The current understanding of CPA is described, some of the nonclassical thermodynamic and dynamic mechanisms known to give rise to experimentally observed pathways are examined, and the challenges to the understanding of these mechanisms are highlighted.
Journal ArticleDOI
Observation of Single Colloidal Platinum Nanocrystal Growth Trajectories
Haimei Zheng,Rachel K. Smith,Young-wook Jun,Young-wook Jun,Christian Kisielowski,Ulrich Dahmen,A. Paul Alivisatos,A. Paul Alivisatos +7 more
TL;DR: Using in situ transmission electron microscopy, it is shown that platinum nanocrystals can grow either by monomer attachment from solution or by particle coalescence, and it is suggested that colloidal nanocrystal take different pathways of growth based on their size- and morphology-dependent internal energies.
Journal ArticleDOI
Nucleation of crystals from solution: classical and two-step models.
TL;DR: The shortcomings of classical nucleation theory are discussed and the applicability of the two-step mechanism to both macromolecules and small organic molecules are demonstrated, suggesting that this mechanism may underlie most crystallization processes from solutions.
Journal ArticleDOI
Dynamic microscopy of nanoscale cluster growth at the solid–liquid interface
TL;DR: This work follows in real time the evolution of individual clusters, and compares their development with simulations incorporating the basic physics of electrodeposition during the early stages of growth, to analyse dynamic observations—recorded in situ using a novel transmission electron microscopy technique—of the nucleation and growth of nanoscale copper clusters during electro Deposition.
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