Unraveling the Mechanism for Paired Electrocatalysis of Organics with Water As a Feedstock

Overview

Journal Nat Commun

Specialty Biology

Date 2022 Jun 6

PMID 35668075

Authors

Ganceng Yang

Yanqing Jiao

Haijing Yan

Ying Xie

Chungui Tian

Aiping Wu

Yu Wang

Honggang Fu

Affiliations

Soon will be listed here.

Abstract

Paired electroreduction and electrooxidation of organics with water as a feedstock to produce value-added chemicals is meaningful. A comprehensive understanding of reaction mechanism is critical for the catalyst design and relative area development. Here, we have systematically studied the mechanism of the paired electroreduction and electrooxidation of organics on Fe-Mo-based phosphide heterojunctions. It is shown that active H* species for organic electroreduction originate from water. As for organic electrooxidation, among various oxygen species (OH*, OOH*, and O*), OH* free radicals derived from the first step of water dissociation are identified as active species. Furthermore, explicit reaction pathways and their paired advantages are proposed based on theoretical calculations. The paired electrolyzer powered by a solar cell shows a low voltage of 1.594 V at 100 mA cm, faradaic efficiency of ≥99%, and remarkable cycle stability. This work provides a guide for sustainable synthesis of various value-added chemicals via paired electrocatalysis.

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