Combining anodic alcohol oxidative coupling for C-C bond formation with cathodic ammonia production

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外文摘要：Electrocatalytic oxidation of alcohols using heterogeneous catalysts is a promising aqueous,energy-efficient and environmentally friendly approach,especially for coupling different alcohols to prolong the carbon chain via co-oxidation.Precisely regulating critical steps to tailor electrode materials and electrolyte composition is key to selectively coupling alcohols for targeted synthesis.However,selectively coupling different alcohols remains challenging due to the lack of effective catalyst and electrolyte design promoting specific pathways.Herein,we demonstrate a paired electrolysis strategy for combining anodic oxidative coupling of ethanol(EtOH)and benzyl alcohol(PhCH2OH)to synthesize cinnamaldehyde(CAL)and cathodic ammonia production.The strategies involve:(ⅰ)utilizing the salt-out effect to balance selective oxidation and coupling rates;(ⅱ)developing platinum-loaded nickel hydroxide electrocatalysts to accelerate intermediate coupling kinetics;(ⅲ)introducing thermodynamically favorable nitrate reduction at the cathode to improve coupling selectivity by avoiding hydrogenation of products while generating valuable ammonia instead of hydrogen.We achieved 85％coupling selectivity and 278 μmol/h NH3 productive rate at 100 mA/cm2 with a low energy input(～1.63 V).The membrane-free,low energy,scalable approach with a wide substrate scope highlights promising applications of this methodology.This work advances heterogeneous electrocatalytic synthesis through rational design principles that integrate anodic oxidative coupling with cathodic nitrate reduction reactions,having synergistic effects on efficiency and selectivity.

外文关键词：

anodic alcohol oxidative couplingC-C bond formationcinnamaldehydecathodic ammonia production

作者：

Leitao Xu、Wei Chen、Cairong Wang、Wenjie Wu、Yelin Yao、Zhifeng Huang、Jingcheng Wu、Ming Yang、Yandong Wu、Dianke Xie、Yuqin Zou、Shuangyin Wang

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作者单位：

State Key Laboratory of Chemo/Bio-Sensing and Chemometrics,College of Chemistry and Chemical Engineering,Advanced Catalytic Engineering Research Center of the Ministry of Education,Hunan University,Changsha 410082,China

基金：

国家重点研发计划国家自然科学基金国家自然科学基金国家自然科学基金湖南省自然科学基金湖南省自然科学基金湖南省自然科学基金湖南省自然科学基金湖南省研究生科研创新项目

项目编号：

2020YFA07100002182520122122901219020472020JJ50452021JJ200242021RC30542022JJ40043CX20220386

出版年：

2024

DOI：

10.1093/nsr/nwae134

国家科学评论(英文版)

CSTPCD

ISSN：

年,卷(期)：2024.11(5)

参考文献量38