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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 5 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.

Authors:
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Publication Date:
Sponsoring Org.:
USDOE
OSTI Identifier:
1547726
Grant/Contract Number:  
SC0010379; EE0007270; E-AC02-06CH11357
Resource Type:
Published Article
Journal Name:
Science
Additional Journal Information:
Journal Name: Science Journal Volume: 363 Journal Issue: 6429; Journal ID: ISSN 0036-8075
Publisher:
American Association for the Advancement of Science (AAAS)
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_1547726,
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 10 5 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.},
doi = {10.1126/science.aat8051},
journal = {Science},
number = 6429,
volume = 363,
place = {United States},
year = {2019},
month = {2}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
DOI: 10.1126/science.aat8051

Citation Metrics:
Cited by: 5 works
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Works referenced in this record:

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