Pt/IrO x enables selective electrochemical C-H chlorination at high current

Abstract Employing electrochemistry for the selective functionalization of liquid alkanes allows for sustainable and efficient production of high-value chemicals. However, the large potentials required for C(sp 3)-H bond functionalization and low water solubility of such alkanes make it challenging....

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Main Authors: Bo Wu, Ruihu Lu, Chao Wu, Tenghui Yuan, Bin Liu, Xi Wang, Chenyi Fang, Ziyu Mi, Surani Bin Dolmanan, Weng Weei Tjiu, Mingsheng Zhang, Bingqing Wang, Zainul Aabdin, Sui Zhang, Yi Hou, Bote Zhao, Shibo Xi, Wan Ru Leow, Ziyun Wang, Yanwei Lum
Format: Article
Language:English
Published: Nature Portfolio 2025-01-01
Series:Nature Communications
Online Access:https://doi.org/10.1038/s41467-024-55283-x
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Summary:Abstract Employing electrochemistry for the selective functionalization of liquid alkanes allows for sustainable and efficient production of high-value chemicals. However, the large potentials required for C(sp 3)-H bond functionalization and low water solubility of such alkanes make it challenging. Here we discover that a Pt/IrO x electrocatalyst with optimized Cl binding energy enables selective generation of Cl free radicals for C-H chlorination of alkanes. For instance, we achieve monochlorination of cyclohexane with a current up to 5 A, Faradaic efficiency (FE) up to 95% and stable performance over 100 h in aqueous KCl electrolyte. We further demonstrate that our system can directly utilize concentrated seawater derived from a solar evaporation reverse osmosis process, achieving a FE of 93.8% towards chlorocyclohexane at a current of 1 A. By coupling to a photovoltaic module, we showcase solar-driven production of chlorocyclohexane using concentrated seawater in a membrane electrode assembly cell without any external bias. Our findings constitute a sustainable pathway towards renewable energy driven chemicals manufacture using abundant feedstock at industrially relevant rates.
ISSN:2041-1723