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co electroreduction:What can we learn from its parent reaction,co_(2) electroreduction?

eScience 2023年第6期3卷 1-8页

作者： Xue Ding Jie Zhang Yanguang Li Institute of Functional Nano and Soft Materials(FUNSOM) Soochow UniversitySuzhou 215123China Jiangsu Key Laboratory for Advanced Negative Carbon Technologies Soochow UniversitySuzhou 215123China Macao Institute of Materials Science and Engineering(MIMSE) MUST-SUDA Joint Research Center for Advanced Functional MaterialsMacao University of Science and TechnologyMacao999078China

The co electroreduction reaction(coRR)represents an important piece of the decarbonization puzzle and is heavily inspired by research on the co_(2) electroreduction reaction(co_(2)RR).compared to its parent reaction,coRR circumvents the(bi)carbonate issue that plagues co_(2)RR,potentially enabling greater stability and selectivity toward C2þproducts,particularly oxygenates.Despite its unique potential,coRR still suffers from unsatisfactory performance.In this perspective article,we aim to provide a concise and informative overview of coRR and its close connection with co_(2)RR.We start by briefly presenting the two reactions’similarities and differences,then discussing several catalyst design strategies.This is followed by highlights of the latest results on device integration and engineering.Finally,we offer our thoughts about possible future research opportunities that could render this technology a practical reality.

关键词： co electroreduction co_(2)electroreduction Catalysts Devices

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Boosting C–C coupling to multicarbon products via high-pressure co electroreduction

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Journal of Energy Chemistry 2023年第10期85卷 102-107,I0005页

作者： Wenqiang Yang Huan Liu Yutai Qi Yifan Li Yi Cui Liang Yu Xiaoju Cui Dehui Deng State Key Laboratory of Catalysis Collaborative Innovation Center of Chemistry for Energy MaterialsDalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina University of Chinese Academy of Sciences Beijing 100049China Vacuum Interconnected Nanotech Workstation Suzhou Institute of Nano-Tech and Nano-BionicsChinese Academy of SciencesSuzhou 215123JiangsuChina

Electrochemical co reduction reaction(coRR) provides a promising approach for producing valuable multicarbon products(C_(2+)), while the low solubility of co in aqueous solution and high energy barrier of C–C coupling as well as the competing hydrogen evolution reaction(HER) largely limit the efficiency for C_(2+)production in coRR. Here we report an overturn on the Faradaic efficiency of coRR from being HER-dominant to C_(2+)formation-dominant over a wide potential window, accompanied by a significant activity enhancement over a Moss-like Cu catalyst via pressuring co. With the co pressure rising from 1 to 40 atm, the C_(2+)Faradaic efficiency and partial current density remarkably increase from 22.8%and 18.9 mA cm^(-2)to 89.7% and 116.7 mA cm^(-2), respectively. Experimental and theoretical investigations reveal that high pressure-induced high co coverage on metallic Cu surface weakens the Cu–C bond via reducing electron transfer from Cu to adsorbed co and restrains hydrogen adsorption, which significantly facilitates the C–C coupling while suppressing HER on the predominant Cu(111) surface, thereby boosting the co electroreduction to C_(2+)activity.

关键词： co electroreduction High pressure electrochemistry Cu catalyst C–C coupling Multicarbon products

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铜基催化剂用于一氧化碳电还原为多碳产品

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Science China Materials 2024年第6期67卷 1684-1705页

作者：赵雯刘娟王光滔王新天杨传举李剑王鋙葶孙晓莲林日琛左淦丞朱文磊 State Key Laboratory of Pollution control and Resource Reuse Frontiers Science Center for Critical Earth Material CyclingState Key Laboratory of Pollution Control and Resource Reusethe Frontiers Science Center for Critical Earth Material CyclingSchool of the EnvironmentNanjing UniversityNanjing 210023China State Key Laboratory of Analytical Chemistry for Life Science School of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210023China State Key Laboratory of Natural Medicines Key Laboratory of Drug Quality Control and PharmacovigilanceSchool of PharmaceuticsChina Pharmaceutical UniversityNanjing 210009China Key Laboratory of Energy Thermal conversion and control of Ministry of Education School of Energy and EnvironmentSoutheast UniversityNanjing 211189China Jiangsu Engineering Lab of Water and Soil Eco-remediation School of EnvironmentNanjing Normal UniversityNanjing 210023China

电化学二氧化碳还原(Eco_(2)R)是一种将碳和可再生能源的能量储存在多碳产品(C_(2+))的化学键中的有效途径.然而,反应涉及的复杂步骤为co_(2)直接转化为C_(2+)设置了巨大的障碍.一种利用co作为“中转站”,通过串联Eco_(2)R和电化学co还... 详细信息

电化学二氧化碳还原(Eco_(2)R)是一种将碳和可再生能源的能量储存在多碳产品(C_(2+))的化学键中的有效途径.然而,反应涉及的复杂步骤为co_(2)直接转化为C_(2+)设置了巨大的障碍.一种利用co作为“中转站”,通过串联Eco_(2)R和电化学co还原(EcoR)以提高生产C_(2+)的选择性和反应速率的策略引起了人们的广泛关注.本文总结了铜基电催化剂在EcoR中催化特定C_(2+)生成的设计策略.其次,从各个方面总结了催化剂工程的代表性设计策略,并介绍了电解反应器改进方面的最新进展.最后,阐述了该研究领域面临的主要挑战和未来前景.这些见解和观点将为铜基电催化剂的设计提供有益指导.

关键词： co electroreduction Cu-based catalysts multi-car-bon products

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Applying machine-learning screening of single transition metal atoms anchored on N-dopedγ-graphyne for carbon monoxide electroreduction toward C_(1)products

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Nano Research 2023年第8期16卷 11511-11520页

作者： Dongxu Jiao Dantong Zhang Dewen Wang Jinchang Fan Xingcheng Ma Jingxiang Zhao Weitao Zheng Xiaoqiang Cui State Key Laboratory of Automotive Simulation and control School of Materials Science and Engineeringand Key Laboratory of Automobile Materials of MOEJilin UniversityChangchun 130012China college of Chemistry and Chemical Engineering and Key Laboratory of Photonic and Electronic Bandgap MaterialsMinistry of EducationHarbin Normal UniversityHarbin 150025China Multiscale Crystal Materials Research Center Shenzhen Institute of Advanced TechnologyChinese Academy of SciencesShenzhen 518055China

Carbon monoxide electroreduction(coER)has been a key part of tandem electrolysis of carbon dioxide(co_(2)),in which searching for high catalytic performance coER electrocatalysts remains a great challenge.Herein,by means of density functional theory(DFT)computations,we explored the potential of a series of transition metal atoms anchored on N-dopedγ-graphyne(TM@N-GY,TM from Ti to Au)as the coER electrocatalysts.We found that the final product selectivity of these single-atom catalysts depended on the position of the metal atom in the periodic table,with metals in the front and middle of each periodic period exhibiting high selectivity for CH_(4),while metals in the back producing CH_(3)OH.Machine learning(ML)found that metal atomic number was intrinsic to the difference in coER performance of these single-atom catalysts(SACs).The free energy changes showed that Mn@N-GY and Ni@N-GY exhibited outstanding coER catalytic performance for producing CH_(4)and CH_(3)OH,respectively.Our results provide theoretical and experimental guidance for designing efficient coER catalysts to generate C_(1)products.

关键词： co electroreduction single atom catalysts γ-graphyne density functional theory machine learning

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Few-Atom copper Catalyst for the Electrochemical Reduction of co to Acetate:Synergetic Catalysis between Neighboring Cu Atoms

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CCS Chemistry 2023年第5期5卷 1176-1188页

作者： Weifeng Rong Haiyuan Zou Sha Tan Enyuan Hu Fan Li Chao Tang Hao Dai Shuting Wei Yongfei Ji Lele Duan Shenzhen Grubbs Institute and Department of Chemistry Southern University of Science and TechnologyShenzhenGuangdong 518055 Chemistry Division Brookhaven National LaboratoryUptonNew York 11973 School of Chemistry and Chemical Engineering Guangzhou UniversityGuangzhouGuangdong 510006 School of Chemical Engineering Shandong University of TechnologyZiboShandong 255049

Single-atom catalysts(SACs)are gaining increasing recognition because of their superior catalytic properties for various reactions.However,the performance of SACs is often limited by the lack of neighboring metal centers to cooperate in catalysis.Herein,a synergetic interaction between neighboring Cu atoms of a few-atom catalyst(FAC)on graphdiyne(GDY)is found to greatly enhance the production of acetate in the co electroreduction reaction relative to Cu SACs.In a 1.0 M KOH electrolyte,this Cu FAC exhibits an acetate Faradaic efficiency of 53.8±1.5%,an ultrahigh relative purity of up to 97 wt%for liquid products,and excellent stability over 23 h continuous electrolysis at–0.8 V versus reversible hydrogen electrode.Theoretical studies suggest that the intersite catalytic communication between two neighboring metal atoms confined in each pore of GDY facilitates the formation of acetic acid through either stepwise hydrogenation of CH_(2)co^(*)or the direct reaction of H_(2)Owith CH_(2)co^(*).Our study demonstrates the unprecedented synergetic catalysis of Cu FAC in promoting the selective co electroreduction toward acetate production.

关键词： co electroreduction synergetic catalysis few-atom catalyst graphdiyne acetate

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