Fe2+/Fe3+ Cycling for Coupling Self-Powered Hydrogen Evolution and Preparation of Electrode Catalysts

Angewandte Chemie Pub Date : 2022-05-30 DOI:10.1002/ange.202207226

Chang Chen, Zhengqian Fu, Fenggang Qi, Yafeng Chen, Ge Meng, Ziwei Chang, Fantao Kong, Libo Zhu, Han Tian, Prof. Haitao Huang, Prof. Xiangzhi Cui, Prof. Jianlin Shi

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Abstract

A novel Zn−Fe flow battery featuring an Fe³⁺ reduction reaction (Fe³⁺RR)-coupled zinc oxidation, and an Fe²⁺ oxidation reaction (Fe²⁺OR)-coupled hydrogen evolution reaction (HER) system as well, was established. This battery is capable of driving two Fe²⁺OR-coupled HER systems in series based on the above Fe²⁺/Fe³⁺ cycling, for efficient self-powered hydrogen evolution. Meanwhile, this Fe²⁺/Fe³⁺ cycling enables the preparation of a multifunctional catalyst, Pt-3@SXNS (siloxene nanosheet), by the Fe²⁺OR-promoted dispersion of Pt nanoparticles on SXNS; alternatively, this support could be obtained by Fe³⁺RR-assisted exfoliation using Fe³⁺ from the anolyte of Fe²⁺OR-coupled HER. The Pt-3@SXNS catalyst exhibits excellent catalytic activities toward Fe³⁺RR in the Zn−Fe flow battery, HER, and Fe²⁺OR in the electrolyzer, which is attributed to the strong electronic interaction between Pt and Si. This work offers a new strategy for energy storage and low-cost hydrogen production from acidic wastewater.

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Fe2+/Fe3+循环耦合自供能析氢及电极催化剂制备

建立了一种具有Fe3+还原反应(Fe3+RR)耦合锌氧化和Fe2+氧化反应(Fe2+OR)耦合析氢反应(HER)体系的新型Zn - Fe液流电池。该电池能够基于上述Fe2+/Fe3+循环驱动两个Fe2+ or耦合HER系统串联，实现高效的自供能析氢。同时，这种Fe2+/Fe3+循环可以通过Fe2+ or促进Pt纳米粒子在SXNS上的分散制备多功能催化剂Pt-3@SXNS(硅氧烷纳米片);也可以通过Fe2+ or - HER阳极液中的Fe3+进行Fe3+ r辅助剥离来获得这种支持。Pt-3@SXNS催化剂在Zn−Fe液流电池、HER和电解槽中的Fe2+OR中表现出优异的催化活性，这是由于Pt和Si之间的强电子相互作用所致。这项工作为酸性废水的储能和低成本制氢提供了一种新的策略。

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