Surface Anticorrosion Engineering by Polyphosphate Oxyanions for Durable Seawater Oxidation

Author:

Wang Xunlu12,Hu Huashuai3,Song Junnan4,Ma Junqing12,Du Hanxiao12,Wang Jiacheng Jayden12,Wang Min12,Chen Wei5,Zhou Yin6,Wang Jiacheng4ORCID,Yang Minghui3,Zhang Lingxia12

Affiliation:

1. State Key Laboratory of High‐Performance Ceramics and Superfine Microstructure Shanghai Institute of Ceramics Chinese Academy of Sciences Shanghai 200050 China

2. Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of Sciences Beijing 100049 China

3. School of Environmental Science and Technology Dalian University of Technology Dalian Liaoning 11602 China

4. Zhejiang Key Laboratory for Island Green Energy and New Materials Institute of Electrochemistry School of Materials Science and Engineering Taizhou University Taizhou Zhejiang 318000 China

5. Department of Materials Design and Innovation University at Buffalo The State University of New York Buffalo NY 14260 USA

6. School of Mechanical and Electrical Engineering Taizhou University Taizhou Jiangsu 225300 China

Abstract

AbstractElectrolysis of seawater represents great potentials for sustainable hydrogen production. However, both competitive Cl adsorption and catalysts corrosion caused by chlorine oxidation reaction (ClOR) are major challenges in seawater electrolysis. Inspired by the concept of hard and soft acids and bases (HSAB), polyphosphate oxyanions (P3O105−) on Ni(OH)2 surface is coordinated to obtain harder acid Ni sites, which could obtain 160 times stability enhancement compared to pure Ni(OH)2 for oxygen evolution reaction (OER) in alkaline seawater at 800 mA cm−2. Also, the turnover frequency value on Ni(OH)2‐P3O105− is 50 times that on Ni(OH)2, implying higher intrinsic OER activity of Ni(OH)2‐P3O105−. Theoretical and experimental investigations show that P3O105− could facilitate transition of Ni3+ to harder acid Ni>3+, thus preferring adsorption of hard base OH rather than soft base Cl. This could enhance OER selectivity and inhibit undesirable ClOR. Furthermore, molecular dynamics simulations indicate that the Cl concentration near the electrode could be reduced by nearly half due to electrostatic repulsion of Cl by surface P3O105− oxyanions. When assembled into an electrolyzer for alkaline seawater splitting, it could operate at 2.2 V with large current up to 1.4 A for 240 h.

Funder

National Natural Science Foundation of China

Science and Technology Commission of Shanghai Municipality

Program of Shanghai Academic Research Leader

Publisher

Wiley

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