New Undisputed Evidence and Strategy for Enhanced Lattice-Oxygen Participation of Perovskite Electrocatalyst through Cation Deficiency Manipulation

Oxygen evolution reaction (OER) is a key half-reaction in many electrochemical transformations, and efficient electrocatalysts are critical to improve its kinetics which is typically sluggish due to its multielectron-transfer nature. Perovskite oxides are a popular category of OER catalysts, while t...

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Main Authors: Xu, Xiaomin, Pan, Y., Zhong, Yijun, Shi, C., Guan, D., Ge, L., Hu, Z., Chin, Y.Y., Lin, H.J., Chen, C.T., Wang, H., Jiang, San Ping, Shao, Zongping
Format: Journal Article
Language:English
Published: WILEY 2022
Subjects:
Online Access:http://purl.org/au-research/grants/arc/DP200103315
http://hdl.handle.net/20.500.11937/90614
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author Xu, Xiaomin
Pan, Y.
Zhong, Yijun
Shi, C.
Guan, D.
Ge, L.
Hu, Z.
Chin, Y.Y.
Lin, H.J.
Chen, C.T.
Wang, H.
Jiang, San Ping
Shao, Zongping
author_facet Xu, Xiaomin
Pan, Y.
Zhong, Yijun
Shi, C.
Guan, D.
Ge, L.
Hu, Z.
Chin, Y.Y.
Lin, H.J.
Chen, C.T.
Wang, H.
Jiang, San Ping
Shao, Zongping
author_sort Xu, Xiaomin
building Curtin Institutional Repository
collection Online Access
description Oxygen evolution reaction (OER) is a key half-reaction in many electrochemical transformations, and efficient electrocatalysts are critical to improve its kinetics which is typically sluggish due to its multielectron-transfer nature. Perovskite oxides are a popular category of OER catalysts, while their activity remains insufficient under the conventional adsorbate evolution reaction scheme where scaling relations limit activity enhancement. The lattice oxygen-mediated mechanism (LOM) has been recently reported to overcome such scaling relations and boost the OER catalysis over several doped perovskite catalysts. However, direct evidence supporting the LOM participation is still very little because the doping strategy applied would introduce additional active sites that may mask the real reaction mechanism. Herein, a dopant-free, cation deficiency manipulation strategy to tailor the bulk diffusion properties of perovskites without affecting their surface properties is reported, providing a perfect platform for studying the contribution of LOM to OER catalysis. Further optimizing the A-site deficiency achieves a perovskite candidate with excellent intrinsic OER activity, which also demonstrates outstanding performance in rechargeable Zn–air batteries and water electrolyzers. These findings not only corroborate the key role of LOM in OER electrocatalysis, but also provide an effective way for the rational design of better catalyst materials for clean energy technologies.
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spelling curtin-20.500.11937-906142023-03-27T02:42:10Z New Undisputed Evidence and Strategy for Enhanced Lattice-Oxygen Participation of Perovskite Electrocatalyst through Cation Deficiency Manipulation Xu, Xiaomin Pan, Y. Zhong, Yijun Shi, C. Guan, D. Ge, L. Hu, Z. Chin, Y.Y. Lin, H.J. Chen, C.T. Wang, H. Jiang, San Ping Shao, Zongping Science & Technology Physical Sciences Technology Chemistry, Multidisciplinary Nanoscience & Nanotechnology Materials Science, Multidisciplinary Chemistry Science & Technology - Other Topics Materials Science cation deficiency lattice-oxygen participation oxygen evolution reaction perovskites water splitting Zn-air batteries A-SITE DEFICIENCY OXIDE CATALYSTS EVOLUTION CHARGE RECONSTRUCTION PERFORMANCE REDUCTION CELLS STATE ION Oxygen evolution reaction (OER) is a key half-reaction in many electrochemical transformations, and efficient electrocatalysts are critical to improve its kinetics which is typically sluggish due to its multielectron-transfer nature. Perovskite oxides are a popular category of OER catalysts, while their activity remains insufficient under the conventional adsorbate evolution reaction scheme where scaling relations limit activity enhancement. The lattice oxygen-mediated mechanism (LOM) has been recently reported to overcome such scaling relations and boost the OER catalysis over several doped perovskite catalysts. However, direct evidence supporting the LOM participation is still very little because the doping strategy applied would introduce additional active sites that may mask the real reaction mechanism. Herein, a dopant-free, cation deficiency manipulation strategy to tailor the bulk diffusion properties of perovskites without affecting their surface properties is reported, providing a perfect platform for studying the contribution of LOM to OER catalysis. Further optimizing the A-site deficiency achieves a perovskite candidate with excellent intrinsic OER activity, which also demonstrates outstanding performance in rechargeable Zn–air batteries and water electrolyzers. These findings not only corroborate the key role of LOM in OER electrocatalysis, but also provide an effective way for the rational design of better catalyst materials for clean energy technologies. 2022 Journal Article http://hdl.handle.net/20.500.11937/90614 10.1002/advs.202200530 English http://purl.org/au-research/grants/arc/DP200103315 http://purl.org/au-research/grants/arc/DP200103332 http://creativecommons.org/licenses/by/4.0/ WILEY fulltext
spellingShingle Science & Technology
Physical Sciences
Technology
Chemistry, Multidisciplinary
Nanoscience & Nanotechnology
Materials Science, Multidisciplinary
Chemistry
Science & Technology - Other Topics
Materials Science
cation deficiency
lattice-oxygen participation
oxygen evolution reaction
perovskites
water splitting
Zn-air batteries
A-SITE DEFICIENCY
OXIDE CATALYSTS
EVOLUTION
CHARGE
RECONSTRUCTION
PERFORMANCE
REDUCTION
CELLS
STATE
ION
Xu, Xiaomin
Pan, Y.
Zhong, Yijun
Shi, C.
Guan, D.
Ge, L.
Hu, Z.
Chin, Y.Y.
Lin, H.J.
Chen, C.T.
Wang, H.
Jiang, San Ping
Shao, Zongping
New Undisputed Evidence and Strategy for Enhanced Lattice-Oxygen Participation of Perovskite Electrocatalyst through Cation Deficiency Manipulation
title New Undisputed Evidence and Strategy for Enhanced Lattice-Oxygen Participation of Perovskite Electrocatalyst through Cation Deficiency Manipulation
title_full New Undisputed Evidence and Strategy for Enhanced Lattice-Oxygen Participation of Perovskite Electrocatalyst through Cation Deficiency Manipulation
title_fullStr New Undisputed Evidence and Strategy for Enhanced Lattice-Oxygen Participation of Perovskite Electrocatalyst through Cation Deficiency Manipulation
title_full_unstemmed New Undisputed Evidence and Strategy for Enhanced Lattice-Oxygen Participation of Perovskite Electrocatalyst through Cation Deficiency Manipulation
title_short New Undisputed Evidence and Strategy for Enhanced Lattice-Oxygen Participation of Perovskite Electrocatalyst through Cation Deficiency Manipulation
title_sort new undisputed evidence and strategy for enhanced lattice-oxygen participation of perovskite electrocatalyst through cation deficiency manipulation
topic Science & Technology
Physical Sciences
Technology
Chemistry, Multidisciplinary
Nanoscience & Nanotechnology
Materials Science, Multidisciplinary
Chemistry
Science & Technology - Other Topics
Materials Science
cation deficiency
lattice-oxygen participation
oxygen evolution reaction
perovskites
water splitting
Zn-air batteries
A-SITE DEFICIENCY
OXIDE CATALYSTS
EVOLUTION
CHARGE
RECONSTRUCTION
PERFORMANCE
REDUCTION
CELLS
STATE
ION
url http://purl.org/au-research/grants/arc/DP200103315
http://purl.org/au-research/grants/arc/DP200103315
http://hdl.handle.net/20.500.11937/90614