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Platinum-based nanocages with subnanometer-thick walls and well-defined, controllable facets

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TLDR
Nanocages of platinum are fabricated by depositing a few atomic layers of platinum as conformal shells on palladium nanocrystals with well-defined facets and then etching away the Pd templates.
Abstract
A cost-effective catalyst should have a high dispersion of the active atoms, together with a controllable surface structure for the optimization of activity, selectivity, or both. We fabricated nanocages by depositing a few atomic layers of platinum (Pt) as conformal shells on palladium (Pd) nanocrystals with well-defined facets and then etching away the Pd templates. Density functional theory calculations suggest that the etching is initiated via a mechanism that involves the formation of vacancies through the removal of Pd atoms incorporated into the outermost layer during the deposition of Pt. With the use of Pd nanoscale cubes and octahedra as templates, we obtained Pt cubic and octahedral nanocages enclosed by {100} and {111} facets, respectively, which exhibited distinctive catalytic activities toward oxygen reduction.

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Combining theory and experiment in electrocatalysis: Insights into materials design

TL;DR: A unified theoretical framework highlights the need for catalyst design strategies that selectively stabilize distinct reaction intermediates relative to each other, and opens up opportunities and approaches to develop higher-performance electrocatalysts for a wide range of reactions.
Journal ArticleDOI

Recent Advances in Electrocatalysts for Oxygen Reduction Reaction

TL;DR: This comprehensive Review focuses on the low- and non-platinum electrocatalysts including advanced platinum alloys, core-shell structures, palladium-based catalysts, metal oxides and chalcogenides, carbon-based non-noble metal catalysts and metal-free catalysts.
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Recent Advances in Electrocatalytic Hydrogen Evolution Using Nanoparticles.

TL;DR: The fundamentals of HER are summarized and the recent state-of-the-art advances in the low-cost and high-performance catalysts based on noble and non-noble metals, as well as metal-free HER electrocatalysts are reviewed.
Journal ArticleDOI

Bimetallic Nanocrystals: Syntheses, Properties, and Applications

TL;DR: A comprehensive review of recent research activities on bimetallic nanocrystals, featuring key examples from the literature that exemplify critical concepts and place a special emphasis on mechanistic understanding.
References
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Journal ArticleDOI

Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set.

TL;DR: An efficient scheme for calculating the Kohn-Sham ground state of metallic systems using pseudopotentials and a plane-wave basis set is presented and the application of Pulay's DIIS method to the iterative diagonalization of large matrices will be discussed.
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Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set

TL;DR: A detailed description and comparison of algorithms for performing ab-initio quantum-mechanical calculations using pseudopotentials and a plane-wave basis set is presented in this article. But this is not a comparison of our algorithm with the one presented in this paper.
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Origin of the Overpotential for Oxygen Reduction at a Fuel-Cell Cathode

TL;DR: In this paper, the stability of reaction intermediates of electrochemical processes on the basis of electronic structure calculations was analyzed and a detailed description of the free energy landscape of the electrochemical oxygen reduction reaction over Pt(111) as a function of applied bias was presented.
Journal ArticleDOI

Formation of hollow nanocrystals through the nanoscale Kirkendall effect

TL;DR: A simple extension of the process yielded platinum–cobalt oxide yolk-shell nanostructures, which may serve as nanoscale reactors in catalytic applications, and provides a general route to the synthesis of hollow nanostructureures of a large number of compounds.
Journal Article

Formation of hollow nanocrystals through the nanoscale kirkendall effect

TL;DR: Alivisatos et al. as mentioned in this paper demonstrate that hollow nanocrystals can be synthesized through a mechanism analogous to the Kirkendall Effect, in which pores form due to the difference in diffusion rates between two components in a diffusion couple.
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