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Recent Advances in the Understanding of the Surface Reconstruction of Oxygen Evolution Electrocatalysts and Materials Development

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Abstract

The electrochemical oxygen evolution reaction (OER) plays an important role in many clean electrochemical energy storage and conversion systems, such as electrochemical water splitting, rechargeable metal–air batteries, and electrochemical CO2 reduction. However, the OER involves a complex four-electron process and suffers from intrinsically sluggish kinetics, which greatly impairs the efficiency of electrochemical systems. In addition, state-of-the-art RuO2-based OER electrocatalysts are too expensive and scarce for practical applications. The development of highly active, cost-effective, and durable electrocatalysts that can improve OER performance (activity and durability) is of significant importance in realizing the widespread application of these advanced technologies. To date, considerable progress has been made in the development of alternative, noble metal-free OER electrocatalysts. Among these alternative catalysts, transition metal compounds have received particular attention and have shown activities comparable to or even higher than those of their precious metal counterparts. In contrast to many other electrocatalysts, such as carbon-based materials, transition metal compounds often exhibit a surface reconstruction phenomenon that is accompanied by the transformation of valence states during electrochemical OER processes. This surface reconstruction results in changes to the true active sites and an improvement or reduction in OER catalytic performance. Therefore, understanding the self-reconstruction process and precisely identifying the true active sites on electrocatalyst surfaces will help us to finely tune the properties and activities of OER catalysts. This review provides a comprehensive summary of recent progress made in understanding the surface reconstruction phenomena of various transition metal-based OER electrocatalysts, focusing on uncovering the correlations among structure, surface reconstruction and intrinsic activity. Recent advances in OER electrocatalysts that exhibit a surface self-reconstruction capability are also discussed. We identify possible challenges and perspectives for the development of OER electrocatalysts based on surface reconstruction. We hope this review will provide readers with some guidance on the rational design of catalysts for various electrochemical reactions.

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Fig. 1
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Reproduced with permission from Ref. [13]. Copyright 2017, Royal Society of Chemistry

Fig. 4

Reproduced with permission from Ref. [17]. Copyright 2018, Science China Press

Fig. 5

Reproduced with permission from Ref. [38]. Copyright 2019, Elsevier

Fig. 6
Fig. 7
Fig. 8

Reproduced with permission from Ref. [114]. Copyright 2019, Springer Nature. b The setup scheme for in situ XAS of electrocatalysts. Reproduced with permission from Ref. [115]. Copyright 2018, Springer Nature

Fig. 9

Reproduced with permission from Ref. [118]. Copyright 2016, Wiley–VCH. b Schematic diagram of the in situ Raman setup combined with electrochemical measurements. Reproduced with permission from Ref. [119]. Copyright 2019, Elsevier

Fig. 10

Reproduced with permission from Ref. [125]. Copyright 2017, Royal Society of Chemistry

Fig. 11

Reproduced with permission from Ref. [131]. Copyright 2016, Elsevier. b In situ FTIR spectra of metal sulfides during the OER. Reproduced with permission from Ref. [42]. Copyright 2018, American Chemistry Society

Fig. 12

Reproduced with permission from Ref. [137]. Copyright 2017, Elsevier. b Co 2p, c P 2p, d O 1s XPS spectra. Reproduced with permission from Ref. [43]. Copyright 2018, American Chemistry Society

Fig. 13

Reproduced with permission from Ref. [145]. Copyright 2019, Royal Society of Chemistry

Fig. 14
Fig. 15

Reproduced with permission from Ref. [146]. Copyright 2020, American Chemistry Society. b Schematic diagram of Fe replacing Al to activate CoAl2O4 surface reconstruction and form active CoOOH. Reproduced with permission from Ref. [46]. Copyright 2019, Springer Nature. c Schematic diagram of the adsorbate evolution mechanism (x  =  0, 0.2 and 0.4) and the mechanism underlying the evolution of participating lattice oxygen (x = 0.6 and 0.8) in ZnCo2−xNixO4. Reproduced with permission from Ref. [48]. Copyright 2019, Wiley–VCH

Fig. 16

Reproduced with permission from Ref. [49]. Copyright 2017, Springer Nature. b Schematic illustration of the formation of (Co/Fe)O(OH) from LaCo0.8Fe0.2O3−δ. Reproduced with permission from Ref. [52]. Copyright 2018, Royal Society of Chemistry. c Schematic diagram of the surface reconstruction of perovskite LaCo0.8Fe0.2O3−δ induced by doping with Sr. Reproduced with permission from Ref. [53]. Copyright 2020, Elsevier. d High resolution transmission electron microscopy (HRTEM) images of perovskite LaCo0.8Fe0.2O3−δ before (left) and after (right) the OER process [(1) and (2) show LCFs without Sr doping; (3) and (4) show LSCFs with Sr doping]. Reproduced with permission from Ref. [53]. Copyright 2020, Elsevier

Fig. 17

Reproduced with permission from Ref. [80]. Copyright 2020, Cell Press

Fig. 18

Reproduced with permission from Ref. [55]. Copyright 2019, Wiley–VCH. b Schematic illustration of the formation of E-CoOx/CF from Co-WO3/CF. Reproduced with permission from Ref. [56]. Copyright 2019, Elsevier. c Thermal stability (left) and corrosion resistance (right) tests for DR-OOH. Reproduced with permission from Ref. [57]. Copyright 2019, American Chemistry Society. d Schematic illustration of CoOOH exposure by in situ self-reconstruction in the OER process. Reproduced with permission from Ref. [58]. Copyright 2020, Wiley–VCH

Fig. 19

Reproduced with permission from Ref. [59]. Copyright 2019, American Chemistry Society. b SEM (left) and HAAD-STEM (right) images of NiFe-OH-F-SR. Reproduced with permission from Ref. [59]. Copyright 2019, American Chemistry Society. c Comparison of the formation energy for α-Ni(OH)2 and γ-NiOOH with different VNi concentrations. Reproduced with permission from Ref. [60]. Copyright 2018, American Chemistry Society. d Schematic representation of the reconstruction process of NiCoHxOy to NiOOH-h-CoO2. Reproduced with permission from Ref. [61]. Copyright 2018, American Chemistry Society. e Raman spectra of CoHxOy (left) and Ni-doped CoHxOy (right). Reproduced with permission from Ref. [61]. Copyright 2018, American Chemistry Society

Fig. 20

Reproduced with permission from Ref. [63]. Copyright 2018, American Chemistry Society. b Schematic of the formation process for the Ru-RuPx-CoxP polyhedron. Reproduced with permission from Ref. [64]. Copyright 2018, Elsevier. c ABF-STEM image of CoMoP2 after surface reconstruction. Reproduced with permission from Ref. [65]. Copyright 2020, Royal Society of Chemistry. d Schematic diagram of the conversion of Ni–Fe-P/PO3 into Fe-γ-NiOOH. Reproduced with permission from Ref. [66]. Copyright 2019, Royal Society of Chemistry. e Timing potential curves for Ni1−xFex-P/PO3 with different Fe doping rates. Reproduced with permission from Ref. [66]. Copyright 2019, Royal Society of Chemistry. f HRTEM images of NiPS3 nanosheets after the OER test. Reproduced with permission from Ref. [67]. Copyright 2019, Elsevier. g Raman spectra of NiPS3 nanosheets before and after the OER test. Reproduced with permission from Ref. [67]. Copyright 2019, Elsevier

Fig. 21

Reproduced with permission from Ref. [42]. Copyright 2018, American Chemistry Society. b Timing potential curve for CoSx during the OER process. Reproduced with permission from Ref. [42]. Copyright 2018, American Chemistry Society. c XPS spectra of the pristine and post-OER Ni3S2 catalysts. Reproduced with permission from Ref. [69]. Copyright 2020, Royal Society of Chemistry. d Schematic diagram of the energy change associated with the Co–Cl bond cleavage in the Co2(OH)3Cl catalyst. Reproduced with permission from Ref. [70]. Copyright 2019, Wiley–VCH. e Schematic diagram of the reconstruction of the NiSe2 catalyst. Reproduced with permission from Ref. [71]. Copyright 2019, Elsevier. f Schematic representation of O-CoSe2-O-UNs reconstructed from cobalt diselenide via an Ar/O2 plasma. Reproduced with permission from Ref. [73]. Copyright 2018, Wiley–VCH

Fig. 22

Reproduced with permission from Ref. [74]. Copyright 2019, Springer Nature. b Schematic diagram of the reconstruction of Co3C. Reproduced with permission from Ref. [76]. Copyright 2018, American Chemistry Society. c Trend in OER overpotential as a function of the number of electrochemical sweeps, where red is based on the geometric electrode surface area and blue is based on the electrochemically active surface area. Reproduced with permission from Ref. [76]. Copyright 2018, American Chemistry Society. d ECSA curve as a function of the number of sweeps. Reproduced with permission from Ref. [76]. Copyright 2018, American Chemistry Society

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Acknowledgements

The authors would like to thank the National Natural Science Foundation of China (21975292, 21978331, 21905311, 92061124), the Guangzhou Science and Technology Project (201707010079), the Guangdong Province Nature Science Foundation (2020A1515010343), the Tip-top Scientific and Technical Innovative Youth Talents of Guangdong Special Support Program (No. 2016TQ03N322), and the Fundamental Research Funds for Central Universities (No19lgpy136, 19lgpy116) for financial support. Prof. Tongwen Yu would like to give special thanks to the support of the startup grant provided by the “Hundred Talents Program” at Sun Yat-sen University (No. 76110-18841219).

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  1. The Key Lab of Low-Carbon Chemistry & Energy Conservation of Guangdong Province, PCFM Lab, School of Chemical Engineering and Technology, School of Materials Science and Engineering, Sun Yat-sen University, Guangzhou, 510275, Guangdong, China

    Junwei Chen, Haixin Chen, Tongwen Yu, Ruchun Li, Yi Wang & Shuqin Song

  2. Jiangsu National Synergetic Innovation Center for Advanced Materials, State Key Laboratory of Materials-Oriented Chemical Engineering, College of Chemical Engineering, Nanjing Tech University, Nanjing, 210009, Jiangsu, China

    Zongping Shao

  3. WA School of Mines: Minerals, Energy and Chemical Engineering, Curtin University, Perth, WA, 6102, Australia

    Zongping Shao

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  1. Junwei Chen
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  2. Haixin Chen
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  3. Tongwen Yu
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Correspondence to Zongping Shao.

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Chen, J., Chen, H., Yu, T. et al. Recent Advances in the Understanding of the Surface Reconstruction of Oxygen Evolution Electrocatalysts and Materials Development. Electrochem. Energ. Rev. 4, 566–600 (2021). https://doi.org/10.1007/s41918-021-00104-8

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