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Title: Tunable intrinsic strain in two-dimensional transition metal electrocatalysts

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 10 5atmospheres 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.

Authors:
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [3]; ORCiD logo [2]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [4]; ORCiD logo [1]; ORCiD logo [2]
  1. Johns Hopkins Univ., Baltimore, MD (United States). Dept. of Chemical and Biomolecular Engineering
  2. Purdue Univ., West Lafayette, IN (United States). Davidson School of Chemical Engineering
  3. Univ. of California, Irvine, CA (United States). Dept. of Chemical Engineering and Materials Science
  4. Univ. of California, Irvine, CA (United States). Dept. of Chemical Engineering and Materials Science; Univ. of California, Irvine, CA (United States). Dept. of Physics and Astronomy
Publication Date:
Research Org.:
Lawrence Berkeley National Laboratory-National Energy Research Scientific Computing Center (NERSC)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1542463
DOE Contract Number:  
SC0010379; AC02-06CH11357; EE0007270
Resource Type:
Journal Article
Journal Name:
Science
Additional Journal Information:
Journal Volume: 363; Journal Issue: 6429; Journal ID: ISSN 0036-8075
Country of Publication:
United States
Language:
English

Citation Formats

Wang, Lei, Zeng, Zhenhua, Gao, Wenpei, Maxson, Tristan, Raciti, David, Giroux, Michael, Pan, Xiaoqing, Wang, Chao, and Greeley, Jeffrey. Tunable intrinsic strain in two-dimensional transition metal electrocatalysts. United States: N. p., 2019. Web. doi:10.1126/science.aat8051.
Wang, Lei, Zeng, Zhenhua, Gao, Wenpei, Maxson, Tristan, Raciti, David, Giroux, Michael, Pan, Xiaoqing, Wang, Chao, & Greeley, Jeffrey. Tunable intrinsic strain in two-dimensional transition metal electrocatalysts. United States. doi:10.1126/science.aat8051.
Wang, Lei, Zeng, Zhenhua, Gao, Wenpei, Maxson, Tristan, Raciti, David, Giroux, Michael, Pan, Xiaoqing, Wang, Chao, and Greeley, Jeffrey. Thu . "Tunable intrinsic strain in two-dimensional transition metal electrocatalysts". United States. doi:10.1126/science.aat8051.
@article{osti_1542463,
title = {Tunable intrinsic strain in two-dimensional transition metal electrocatalysts},
author = {Wang, Lei and Zeng, Zhenhua and Gao, Wenpei and Maxson, Tristan and Raciti, David and Giroux, Michael and Pan, Xiaoqing and Wang, Chao and Greeley, Jeffrey},
abstractNote = {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 105atmospheres 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.},
doi = {10.1126/science.aat8051},
journal = {Science},
issn = {0036-8075},
number = 6429,
volume = 363,
place = {United States},
year = {2019},
month = {2}
}

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