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Surface-derived phosphate layer on NiFe-layered double hydroxide realizes stable seawater oxidation at the current density of 1 A·cm−2

Show Author's Information Chaoxin Yang1,  Zhengwei Cai1,  Jie Liang2,  Kai Dong1,  Zixiao Li1,2,  Hang Sun3,  Shengjun Sun1,  Dongdong Zheng1,  Hui Zhang1,  Yongsong Luo1,  Yongchao Yao2,  Yan Wang2,  Yuchun Ren2,  Qian Liu4,  Luming Li4,  Wei Chu4,  Xuping Sun1,2( ),  Bo Tang1,5( )
College of Chemistry, Chemical Engineering and Materials Science, Shandong Normal University, Jinan 250014, China
Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu 610054, China
Department of Science and Environmental Studies, Faculty of Liberal Arts and Social Science, the Education University of Hong Kong, Hong Kong 999077, China
Institute for Advanced Study, Chengdu University, Chengdu 610106, China
Laoshan Laboratory, Qingdao 266237, China
Keywords:
layered double hydroxide, seawater oxidation, in situ Raman, electrostatic repulsion, phosphate outer-layer
Topics:
Electrocatalysis
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Yang C, Cai Z, Liang J, et al. Surface-derived phosphate layer on NiFe-layered double hydroxide realizes stable seawater oxidation at the current density of 1 A·cm−2. Nano Research, 2024, https://doi.org/10.1007/s12274-024-6562-z
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Abstract Full text Electronic supplementary material About this article

Seawater electrolysis, especially in coastlines, is widely considered as a sustainable way of making clean and high-purity H2 from renewable energy; however, the practical viability is challenged severely by the limited anode durability resulting from side reactions of chlorine species. Herein, we report an effective Cl− blocking barrier of NiFe-layer double hydroxide (NiFe-LDH) to harmful chlorine chemistry during alkaline seawater oxidation (ASO), a pre-formed surface-derived NiFe-phosphate (Pi) outer-layer. Specifically, the PO43−-enriched outer-layer is capable of physically and electrostatically inhibiting Cl− adsorption, which protects active Ni3+ sites during ASO. The NiFe-LDH with the NiFe-Pi outer-layer (NiFe-LDH@NiFe-Pi) exhibits higher current densities (j) and lower overpotentials to afford 1 A·cm−2 (η1000 of 370 mV versus η1000 of 420 mV) than the NiFe-LDH in 1 M KOH + seawater. Notably, the NiFe-LDH@NiFe-Pi also demonstrates longer-term electrochemical durability than NiFe-LDH, attaining 100-h duration at the j of 1 A·cm−2. Additionally, the importance of surface-derived PO43−-enriched outer-layer in protecting the active centers, γ-NiOOH, is explained by ex situ characterizations and in situ electrochemical spectroscopic studies.


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Abstract
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Electronic supplementary material
About this article

Surface-derived phosphate layer on NiFe-layered double hydroxide realizes stable seawater oxidation at the current density of 1 A·cm−2

Show Author's information Chaoxin Yang1, Zhengwei Cai1, Jie Liang2, Kai Dong1, Zixiao Li1,2, Hang Sun3, Shengjun Sun1, Dongdong Zheng1, Hui Zhang1, Yongsong Luo1, Yongchao Yao2, Yan Wang2, Yuchun Ren2, Qian Liu4, Luming Li4, Wei Chu4, Xuping Sun1,2( ), Bo Tang1,5( )
College of Chemistry, Chemical Engineering and Materials Science, Shandong Normal University, Jinan 250014, China
Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu 610054, China
Department of Science and Environmental Studies, Faculty of Liberal Arts and Social Science, the Education University of Hong Kong, Hong Kong 999077, China
Institute for Advanced Study, Chengdu University, Chengdu 610106, China
Laoshan Laboratory, Qingdao 266237, China

Abstract

Seawater electrolysis, especially in coastlines, is widely considered as a sustainable way of making clean and high-purity H2 from renewable energy; however, the practical viability is challenged severely by the limited anode durability resulting from side reactions of chlorine species. Herein, we report an effective Cl− blocking barrier of NiFe-layer double hydroxide (NiFe-LDH) to harmful chlorine chemistry during alkaline seawater oxidation (ASO), a pre-formed surface-derived NiFe-phosphate (Pi) outer-layer. Specifically, the PO43−-enriched outer-layer is capable of physically and electrostatically inhibiting Cl− adsorption, which protects active Ni3+ sites during ASO. The NiFe-LDH with the NiFe-Pi outer-layer (NiFe-LDH@NiFe-Pi) exhibits higher current densities (j) and lower overpotentials to afford 1 A·cm−2 (η1000 of 370 mV versus η1000 of 420 mV) than the NiFe-LDH in 1 M KOH + seawater. Notably, the NiFe-LDH@NiFe-Pi also demonstrates longer-term electrochemical durability than NiFe-LDH, attaining 100-h duration at the j of 1 A·cm−2. Additionally, the importance of surface-derived PO43−-enriched outer-layer in protecting the active centers, γ-NiOOH, is explained by ex situ characterizations and in situ electrochemical spectroscopic studies.

Keywords: layered double hydroxide, seawater oxidation, in situ Raman, electrostatic repulsion, phosphate outer-layer

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Publication history
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Acknowledgements

Publication history

Received: 09 December 2023
Revised: 29 January 2024
Accepted: 14 February 2024
Published: 15 March 2024

Copyright

© Tsinghua University Press 2024

Acknowledgements

Acknowledgements

This work was supported by the Free Exploration Project of Frontier Technology for Laoshan Laboratory (No. 16-02) and the National Natural Science Foundation of China (Nos. 22072015 and 21927811).

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