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Title: Uncovering the Effect of Lattice Strain and Oxygen Deficiency on Electrocatalytic Activity of Perovskite Cobaltite Thin Films

Abstract

Developing cost effective electrocatalysts with high oxygen evolution reaction (OER) activity is essential for large-scale application of many electrochemical energy systems. Although the impacts of either lattice strain or oxygen defects on the OER performance of oxide catalysts have been extensively investigated, the effects of both factors are normally treated separately. In this work, the coupled effects of both strain and oxygen deficiency on the electrocatalytic activity of La 0.7Sr 0.3CoO 3-δ (LSC) thin films grown on single crystal substrates (LaAlO3 (LAO) and SrTiO3 (STO)) are investigated. Electrochemical tests show that the OER activities of LSC films are higher under compression than under tension, and are diminished as oxygen vacancies are introduced by vacuum annealing. Both experimental and computational results indicate that the LSC films under tension (e.g., LSC/STO) have larger oxygen deficiency than the films under compression (e.g., LSC/LAO), which attribute to smaller oxygen vacancy formation energy. Such strain-induced excessive oxygen vacancies in the LSC/STO increases the e g state occupancy and enlarges the energy gap between the O 2p and Co 3d band, resulting in lower OER activity. Understanding the critical role of strain–defect coupling is important for achieving the rational design of highly active and durable catalystsmore » for energy devices.« less

Authors:
ORCiD logo [1]; ORCiD logo [2];  [3];  [4];  [5];  [5];  [5];  [5];  [3];  [4];  [5]; ORCiD logo [5]; ORCiD logo [2]
  1. South China Univ. of Technology Guangzhou, Guangdong (China)
  2. Georgia Inst. of Technology, Atlanta, GA (United States)
  3. Tsinghua Univ., Beijing (China)
  4. Peking Univ., Beijing (China)
  5. South China Univ. of Technology Guangzhou, Guangdong (China)
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1493070
Alternate Identifier(s):
OSTI ID: 1493071; OSTI ID: 1530194
Grant/Contract Number:  
AC02‐05CH11231
Resource Type:
Journal Article: Published Article
Journal Name:
Advanced Science
Additional Journal Information:
Journal Volume: 6; Journal Issue: 6; Journal ID: ISSN 2198-3844
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 30 DIRECT ENERGY CONVERSION

Citation Formats

Liu, Xi, Zhang, Lei, Zheng, Yun, Guo, Zheng, Zhu, Yunmin, Chen, Huijun, Li, Fei, Liu, Peipei, Yu, Bo, Wang, Xinwei, Liu, Jiang, Chen, Yan, and Liu, Meilin. Uncovering the Effect of Lattice Strain and Oxygen Deficiency on Electrocatalytic Activity of Perovskite Cobaltite Thin Films. United States: N. p., 2019. Web. doi:10.1002/advs.201801898.
Liu, Xi, Zhang, Lei, Zheng, Yun, Guo, Zheng, Zhu, Yunmin, Chen, Huijun, Li, Fei, Liu, Peipei, Yu, Bo, Wang, Xinwei, Liu, Jiang, Chen, Yan, & Liu, Meilin. Uncovering the Effect of Lattice Strain and Oxygen Deficiency on Electrocatalytic Activity of Perovskite Cobaltite Thin Films. United States. doi:10.1002/advs.201801898.
Liu, Xi, Zhang, Lei, Zheng, Yun, Guo, Zheng, Zhu, Yunmin, Chen, Huijun, Li, Fei, Liu, Peipei, Yu, Bo, Wang, Xinwei, Liu, Jiang, Chen, Yan, and Liu, Meilin. Wed . "Uncovering the Effect of Lattice Strain and Oxygen Deficiency on Electrocatalytic Activity of Perovskite Cobaltite Thin Films". United States. doi:10.1002/advs.201801898.
@article{osti_1493070,
title = {Uncovering the Effect of Lattice Strain and Oxygen Deficiency on Electrocatalytic Activity of Perovskite Cobaltite Thin Films},
author = {Liu, Xi and Zhang, Lei and Zheng, Yun and Guo, Zheng and Zhu, Yunmin and Chen, Huijun and Li, Fei and Liu, Peipei and Yu, Bo and Wang, Xinwei and Liu, Jiang and Chen, Yan and Liu, Meilin},
abstractNote = {Developing cost effective electrocatalysts with high oxygen evolution reaction (OER) activity is essential for large-scale application of many electrochemical energy systems. Although the impacts of either lattice strain or oxygen defects on the OER performance of oxide catalysts have been extensively investigated, the effects of both factors are normally treated separately. In this work, the coupled effects of both strain and oxygen deficiency on the electrocatalytic activity of La0.7Sr0.3CoO3-δ (LSC) thin films grown on single crystal substrates (LaAlO3 (LAO) and SrTiO3 (STO)) are investigated. Electrochemical tests show that the OER activities of LSC films are higher under compression than under tension, and are diminished as oxygen vacancies are introduced by vacuum annealing. Both experimental and computational results indicate that the LSC films under tension (e.g., LSC/STO) have larger oxygen deficiency than the films under compression (e.g., LSC/LAO), which attribute to smaller oxygen vacancy formation energy. Such strain-induced excessive oxygen vacancies in the LSC/STO increases the eg state occupancy and enlarges the energy gap between the O 2p and Co 3d band, resulting in lower OER activity. Understanding the critical role of strain–defect coupling is important for achieving the rational design of highly active and durable catalysts for energy devices.},
doi = {10.1002/advs.201801898},
journal = {Advanced Science},
issn = {2198-3844},
number = 6,
volume = 6,
place = {United States},
year = {2019},
month = {1}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record at 10.1002/advs.201801898

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Cited by: 2 works
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Figures / Tables:

Figure 1 Figure 1: a) Illustration of sample preparation process for LSC thin film electrode. A gold pattern was embedded into the thin film to serve as the current collector for electrochemical measurement; b) illustration of the OER measurement sets up with the film as the WE. c,d) AFM images of LSCmore » model thin films grown on LAO (c) and STO (b) substrates. The surface roughness is less than 1 nm.« less

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Works referenced in this record:

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    Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.