Industrial electrocatalytic C-C coupling reaction of C_(1) liquid molecules for efficient ethanol synthesisOA
Electrochemical conversion of C_(1) feedstocks into ethanol(EtOH)offers a promising pathway for achieving efficient carbon cycling and sustainable fuel production.However,conventional electrocatalytic methods suffer from poor mass transfer and lengthy reaction pathways,hindering the concurrent achievement of high current density and selectivity and thus limiting industrial application.Herein,we propose a novel electrocatalytic C-C coupling pathway for EtOH synthesis from liquid formic acid C_(1) feedstock,achieving high selectivity at high current densities.At 500 mA cm^(-2),the PdCu electrocatalyst achieves an EtOH Faradaic efficiency of 84.68%,with a formation rate of 1970.1μmol h^(-1) cm^(-2),demonstrating significantly superior overall performance compared to conventional gaseous C_(1) feedstock electrocatalytic systems.Theoretical and operando spectroscopic studies elucidate that lattice hydrogen at the in situ-formed PdHx sites on PdH0.45Cu/CNT promotes the conversion of electrophilic^(*)HCOO to nucleophilic^(*)C(OH)_(2),while adjacent Cu promotes asymmetric coupling of^(*)HCOO and^(*)C(OH)_(2).The PdCu electrocatalyst demonstrates outstanding industrial potential,with 120 h of stable operation at 800 mA cm^(-2) in an anion exchange membrane electrolyzer,validated by technical-economic analysis.Moreover,this mechanism is equally applicable to the efficient conversion of formaldehyde into EtOH.This research proposes a novel pathway for the industrial production of electro-synthesized EtOH.
Jiani Han;Yaodong Yu;G.A.Bagliuk;Jianping Lai;Lei Wang
State Key Laboratory Base of Eco-Chemical Engineering,Ministry of Education,International Science and Technology Cooperation Base of Eco-chemical Engineering and Green Manufacturing,College of Chemistry and Molecular Engineering,Qingdao University of Science and Technology,Qingdao 266042,China Shandong Engineering Research Center for Marine Environment Corrosion and Safety Protection,College of Environment and Safety Engineering,Qingdao University of Science and Technology,Qingdao 266042,ChinaState Key Laboratory Base of Eco-Chemical Engineering,Ministry of Education,International Science and Technology Cooperation Base of Eco-chemical Engineering and Green Manufacturing,College of Chemistry and Molecular Engineering,Qingdao University of Science and Technology,Qingdao 266042,ChinaFrantsevich Institute for Problems of Materials Science,National Academy of Sciences of Ukraine,Kyiv 02000,UkraineState Key Laboratory Base of Eco-Chemical Engineering,Ministry of Education,International Science and Technology Cooperation Base of Eco-chemical Engineering and Green Manufacturing,College of Chemistry and Molecular Engineering,Qingdao University of Science and Technology,Qingdao 266042,ChinaState Key Laboratory Base of Eco-Chemical Engineering,Ministry of Education,International Science and Technology Cooperation Base of Eco-chemical Engineering and Green Manufacturing,College of Chemistry and Molecular Engineering,Qingdao University of Science and Technology,Qingdao 266042,China
化学化工
ethanol electrosynthesisliquid C_(1)moleculesC-C couplingformic acid reductionpalladium-copper electrocatalyst
《National Science Review》 2026 (12)
P.138-152,15
supported by the National Natural Science Foundation of China(52272222)Taishan Scholar Young Tal-ent Program(tsqn201909114 and tsqn201909123)the University Youth Innovation Team of Shandong Province(202201010318).
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