Tunable intrinsic strain in two-dimensional transition metal electrocatalysts

Science
Lei WangJeffrey Greeley

Abstract

Tuning surface strain is a powerful strategy for tailoring the reactivity of metal catalysts. Traditionally, surface strain is imposed by external stress from a heterogeneous substrate, but the effect is often obscured by interfacial reconstructions and nanocatalyst geometries. Here, we report on a strategy to resolve these problems by exploiting intrinsic surface stresses in two-dimensional transition metal nanosheets. Density functional theory calculations indicate that attractive interactions between surface atoms lead to tensile surface stresses that exert a pressure on the order of 105 atmospheres on the surface atoms and impart up to 10% compressive strain, with the exact magnitude inversely proportional to the nanosheet thickness. Atomic-level control of thickness thus enables generation and fine-tuning of intrinsic strain to optimize catalytic reactivity, which was confirmed experimentally on Pd(110) nanosheets for the oxygen reduction and hydrogen evolution reactions, with activity enhancements that were more than an order of magnitude greater than those of their nanoparticle counterparts.

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Citations

May 23, 2019·Dalton Transactions : an International Journal of Inorganic Chemistry·Ailing YanRenzhi Ma
Jan 16, 2020·Physical Chemistry Chemical Physics : PCCP·Xiaoping GaoZhemin Shen
Mar 7, 2020·Chemical Society Reviews·Jiajia SongZhichuan J Xu
Apr 21, 2020·Chemical Society Reviews·Leigang LiXiaoqing Huang
Nov 16, 2019·Proceedings of the National Academy of Sciences of the United States of America·Yao YangHéctor D Abruña
Jul 22, 2020·Nature Materials·Pietro P LopesVojislav R Stamenkovic
Nov 7, 2019·Scientific Reports·Eric E BensonDrazenka Svedruzic
Feb 7, 2020·Nanoscale·Farhat NosheenWenping Hu
Sep 21, 2019·Physical Chemistry Chemical Physics : PCCP·P S MiedemaM Beye
Oct 28, 2019·Nature Communications·Geng WuYadong Li
Oct 28, 2019·Physical Chemistry Chemical Physics : PCCP·Z W ChenQ Jiang
Oct 25, 2020·Nature Communications·Shaoyun HaoXingwang Zhang
Nov 17, 2020·Physical Chemistry Chemical Physics : PCCP·Huan LouGuochun Yang
Dec 11, 2019·Nano Letters·Zheng XiXiaohu Xia
Nov 15, 2020·Chemical Communications : Chem Comm·Zhiyuan WeiXiaohu Xia
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May 19, 2021·Chemical Society Reviews·Shao-Hai LiYi-Jun Xu
Mar 3, 2020·Chemical Science·M Alexander ArdaghPaul J Dauenhauer

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