Unraveling the mechanism for paired electrocatalysis of organics with water as a feedstock.
basic_science · Level V
Where this comes from
- Record sourced from PubMed, PMID 35668075.
- Also identified by DOI 10.1038/s41467-022-30495-1 and PMC identifier 9170728.
- Licence recorded as CC BY.
- The licence permits redistribution, so the abstract is shown in full and the full text is available from the publisher.
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<sup>-2</sup>, faradaic efficiency of ≥99%, and remarkable cycle stability. This work provides a guide for sustainable synthesis of various value-added chemicals via paired electrocatalysis.