Redox-mediated decoupled seawater direct splitting for H2 production

Tao Liu (), Cheng Lan (), Min Tang, Mengxin Li, Yitao Xu, Hangrui Yang, Qingyue Deng, Wenchuan Jiang, Zhiyu Zhao, Yifan Wu () and Heping Xie ()
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Tao Liu: Sichuan University & Shenzhen University
Cheng Lan: Sichuan University & Shenzhen University
Min Tang: Sichuan University-Pittsburgh Institute
Mengxin Li: Sichuan University
Yitao Xu: Sichuan University-Pittsburgh Institute
Hangrui Yang: Sichuan University
Qingyue Deng: Sichuan University-Pittsburgh Institute
Wenchuan Jiang: Sichuan University & Shenzhen University
Zhiyu Zhao: Sichuan University & Shenzhen University
Yifan Wu: Sichuan University & Shenzhen University
Heping Xie: Sichuan University & Shenzhen University

Nature Communications, 2024, vol. 15, issue 1, 1-12

Abstract: Abstract Seawater direct electrolysis (SDE) using renewable energy provides a sustainable pathway to harness abundant oceanic hydrogen resources. However, the side-reaction of the chlorine electro-oxidation reaction (ClOR) severely decreased direct electrolysis efficiency of seawater and gradually corrodes the anode. In this study, a redox-mediated strategy is introduced to suppress the ClOR, and a decoupled seawater direct electrolysis (DSDE) system incorporating a separate O2 evolution reactor is established. Ferricyanide/ferrocyanide ([Fe(CN)6]3−/4−) serves as an electron-mediator between the cell and the reactor, thereby enabling a more dynamically favorable half-reaction to supplant the traditional oxygen evolution reaction (OER). This alteration involves a straightforward, single-electron-transfer anodic reaction without gas precipitation and effectively eliminates the generation of chlorine-containing byproducts. By operating at low voltages (~1.37 V at 10 mA cm−2 and ~1.57 V at 100 mA cm−2) and maintaining stability even in a Cl−-saturated seawater electrolyte, this system has the potential of undergoing decoupled seawater electrolysis with zero chlorine emissions. Further improvements in the high-performance redox-mediators and catalysts can provide enhanced cost-effectiveness and sustainability of the DSDE system.

Date: 2024
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DOI: 10.1038/s41467-024-53335-w

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