Artificially steering electrocatalytic oxygen evolution reaction mechanism by regulating oxygen defect contents in perovskites

Min Lu; Yao Zheng; Yang Hu; Bolong Huang; Deguang Ji; Mingzi Sun; Jianyi Li; Yong Peng; Rui Si; Pinxian Xi; Chun-Hua Yan

doi:10.1126/sciadv.abq3563

Artificially steering electrocatalytic oxygen evolution reaction mechanism by regulating oxygen defect contents in perovskites

Min Lu (Co-first Author)
, Yao Zheng (Co-first Author)
, Yang Hu (Co-first Author)
, Bolong Huang^*
, Deguang Ji
, Mingzi Sun
, Jianyi Li
, Yong Peng
, Rui Si
, Pinxian Xi^*
, Chun-Hua Yan

^*Corresponding author for this work

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

203 Citations (Scopus)

100 Downloads (CityUHK Scholars)

Abstract

The regulation of mechanism on the electrocatalysis process with multiple reaction pathways is more efficient and essential than conventional material engineering for the enhancement of catalyst performance. Here, by using oxygen evolution reaction (OER) as a model, which has an adsorbate evolution mechanism (AEM) and a lattice oxygen oxidation mechanism (LOM), we demonstrate a general strategy for steering the two mechanisms on various La_xSr_1-xCoO_3-δ. By delicately controlling the oxygen defect contents, the dominant OER mechanism on La_xSr_1-xCoO_3-δ can be arbitrarily transformed between AEM-LOM-AEM accompanied by a volcano-type activity variation trend. Experimental and computational evidence explicitly reveal that the phenomenon is due to the fact that the increased oxygen defects alter the lattice oxygen activity with a volcano-type trend and preserve the Co⁰ state for preferably OER. Therefore, we achieve the co-optimization between the activity and stability of catalysts by altering the mechanism rather than a specific design of catalysts. Copyright © 2022 The Authors, some rights reserved.

Original language	English
Article number	eabq3563
Journal	Science Advances
Volume	8
Issue number	30
Online published	29 Jul 2022
DOIs	https://doi.org/10.1126/sciadv.abq3563
Publication status	Published - Jul 2022
Externally published	Yes

Funding

This work was funded by the National Key R&D Program of China (2021YFA1501101), the National Natural Science Foundation of China (NSFC; nos. 21922105 and 21931001), the Special Fund Project of Guiding Scientific and Technological Innovation Development of Gansu Province (2019ZX-04), and the 111 Project (B20027). We also acknowledge support by the Fundamental Research Funds for the Central Universities (lzujbky-2021-pd04, lzujbky-2021-it12, and lzujbky-2021-37). B.H. acknowledges the support of the NSFC (no. 21771156), the NSFC/RGC Joint Research Scheme (N_PolyU502/21), and the funding for Projects of Strategic Importance of The Hong Kong Polytechnic University (project code: 1-ZE2V). Y.Z. acknowledges funding from the Australian Research Council (DP190103472 and FT200100062).

Publisher's Copyright Statement

This full text is made available under CC-BY-NC 4.0. https://creativecommons.org/licenses/by-nc/4.0/

RGC Funding Information

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title = "Artificially steering electrocatalytic oxygen evolution reaction mechanism by regulating oxygen defect contents in perovskites",

abstract = "The regulation of mechanism on the electrocatalysis process with multiple reaction pathways is more efficient and essential than conventional material engineering for the enhancement of catalyst performance. Here, by using oxygen evolution reaction (OER) as a model, which has an adsorbate evolution mechanism (AEM) and a lattice oxygen oxidation mechanism (LOM), we demonstrate a general strategy for steering the two mechanisms on various LaxSr1-xCoO3-δ. By delicately controlling the oxygen defect contents, the dominant OER mechanism on LaxSr1-xCoO3-δ can be arbitrarily transformed between AEM-LOM-AEM accompanied by a volcano-type activity variation trend. Experimental and computational evidence explicitly reveal that the phenomenon is due to the fact that the increased oxygen defects alter the lattice oxygen activity with a volcano-type trend and preserve the Co0 state for preferably OER. Therefore, we achieve the co-optimization between the activity and stability of catalysts by altering the mechanism rather than a specific design of catalysts. Copyright {\textcopyright} 2022 The Authors, some rights reserved.",

author = "Min Lu and Yao Zheng and Yang Hu and Bolong Huang and Deguang Ji and Mingzi Sun and Jianyi Li and Yong Peng and Rui Si and Pinxian Xi and Chun-Hua Yan",

year = "2022",

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doi = "10.1126/sciadv.abq3563",

language = "English",

volume = "8",

journal = "Science Advances",

issn = "2375-2548",

publisher = "American Association for the Advancement of Science",

number = "30",

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Artificially steering electrocatalytic oxygen evolution reaction mechanism by regulating oxygen defect contents in perovskites. / Lu, Min (Co-first Author); Zheng, Yao (Co-first Author); Hu, Yang (Co-first Author) et al.
In: Science Advances, Vol. 8, No. 30, eabq3563, 07.2022.

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

TY - JOUR

T1 - Artificially steering electrocatalytic oxygen evolution reaction mechanism by regulating oxygen defect contents in perovskites

AU - Lu, Min

AU - Zheng, Yao

AU - Hu, Yang

AU - Huang, Bolong

AU - Ji, Deguang

AU - Sun, Mingzi

AU - Li, Jianyi

AU - Peng, Yong

AU - Si, Rui

AU - Xi, Pinxian

AU - Yan, Chun-Hua

PY - 2022/7

Y1 - 2022/7

N2 - The regulation of mechanism on the electrocatalysis process with multiple reaction pathways is more efficient and essential than conventional material engineering for the enhancement of catalyst performance. Here, by using oxygen evolution reaction (OER) as a model, which has an adsorbate evolution mechanism (AEM) and a lattice oxygen oxidation mechanism (LOM), we demonstrate a general strategy for steering the two mechanisms on various LaxSr1-xCoO3-δ. By delicately controlling the oxygen defect contents, the dominant OER mechanism on LaxSr1-xCoO3-δ can be arbitrarily transformed between AEM-LOM-AEM accompanied by a volcano-type activity variation trend. Experimental and computational evidence explicitly reveal that the phenomenon is due to the fact that the increased oxygen defects alter the lattice oxygen activity with a volcano-type trend and preserve the Co0 state for preferably OER. Therefore, we achieve the co-optimization between the activity and stability of catalysts by altering the mechanism rather than a specific design of catalysts. Copyright © 2022 The Authors, some rights reserved.

AB - The regulation of mechanism on the electrocatalysis process with multiple reaction pathways is more efficient and essential than conventional material engineering for the enhancement of catalyst performance. Here, by using oxygen evolution reaction (OER) as a model, which has an adsorbate evolution mechanism (AEM) and a lattice oxygen oxidation mechanism (LOM), we demonstrate a general strategy for steering the two mechanisms on various LaxSr1-xCoO3-δ. By delicately controlling the oxygen defect contents, the dominant OER mechanism on LaxSr1-xCoO3-δ can be arbitrarily transformed between AEM-LOM-AEM accompanied by a volcano-type activity variation trend. Experimental and computational evidence explicitly reveal that the phenomenon is due to the fact that the increased oxygen defects alter the lattice oxygen activity with a volcano-type trend and preserve the Co0 state for preferably OER. Therefore, we achieve the co-optimization between the activity and stability of catalysts by altering the mechanism rather than a specific design of catalysts. Copyright © 2022 The Authors, some rights reserved.

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UR - https://www.scopus.com/pages/publications/85135226090#tab=impact

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DO - 10.1126/sciadv.abq3563

M3 - RGC 21 - Publication in refereed journal

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SN - 2375-2548

VL - 8

JO - Science Advances

JF - Science Advances

IS - 30

M1 - eabq3563

ER -

Artificially steering electrocatalytic oxygen evolution reaction mechanism by regulating oxygen defect contents in perovskites

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