Unraveling the mechanism for paired electrocatalysis of organics with water as a feedstock

Production of value-added chemicals by using renewable energy and cheap water attract great interest. Herein, the authors design a paired electrocatalytic system to produce 4-aminobenzyl alcohol at cathode and 2,5-furandicarboxylic acid at anode. 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(-2), faradaic efficiency of >= 99%, and remarkable cycle stability. This work provides a guide for sustainable synthesis of various value-added chemicals via paired electrocatalysis.

Automated summary

The production of value-added chemicals using renewable energy and cost-effective water has attracted significant interest. In this study, the authors developed a paired electrocatalytic system to produce 4-aminobenzyl alcohol and 2,5-furandicarboxylic acid. The electroreduction and electrooxidation of organics with water as a feedstock show promising potential for the production of value-added chemicals. Through comprehensive investigations, the researchers gained insights into the reaction mechanism and proposed explicit reaction pathways. The paired electrolyzer, powered by a solar cell, exhibited excellent performance with low voltage, high faradaic efficiency, and remarkable cycle stability. This work provides valuable guidance for the sustainable synthesis of various value-added chemicals through paired electrocatalysis.