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

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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Syngas to ethanol on Mocu(211)surface:Effect of promoter Mo on C-O bond breaking and C-C bond formation

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Chinese Journal of Chemical Engineering 2022年第5期35卷 78-89页

作者： Lijuan He cuimei Zhi Lixia Ling Riguang Zhang Baojun Wang State Key Laboratory of Clean and Efficient Coal Utilization Taiyuan University of TechnologyTaiyuan 030024China Key Laboratory of Coal Science and Technology(Taiyuan University of Technology) Ministry of Education and Shanxi ProvinceTaiyuan 030024China College of Chemistry and Bioengineering Taiyuan University of Science and TechnologyTaiyuan 030024China College of Chemistry and Chemical Engineering Taiyuan University of TechnologyTaiyuan 030024China

The mechanism of syngas to ethanol on Mocu(211)surface has been researched by density functional theory(DFT)calculation,and the effects of Mo as a promoter on C-O bond breaking and C-C bond formation have been discussed.Calculations show that cu-Mo atoms constitute the active sites on Mocu(211)surface after Mo atom being served as a promoter of cu catalyst.Compared with cu(211),Mocu(211)has two improvements.Firstly,CH_(3) is the most advantageous monomer on the Mocu(211)surface,which provides abundant CH_(3) intermediate for syngas to ethanol.Secondly,the C-C bond is formed mainly by inserting CHO into the abundant CH_(3),and the generated CH_(3)CHO through multiple steps of hydrogenation to generate C_(2)H_(5)OH.The key of the promoter Mo on the Mocu(211)surface also has been verified by the analysis of its electronic properties.Differential charge density shows that the massive electron transfer from Mo to cu,projected density of states(pDOS)shows that the electron transfer from Mo to cu makes the d-band center of Mocu(211)nearer to the Fermi level,these indicate that the Mocu(211)catalytic capacity increased.The addition of Mo in the cu-based catalyst not only can effectively solve the problem of C-O bond breaking,but also promote C-C bond formation.About the influence of Mo content on C-O bond breaking and C-C bond formation,compared with Mocu(211),the DFT results and the d-band center of Mo_(2)cu(211)show that the increase of Mo content could not promote the synergistic effect of cu/Mo on the generation of ethanol more effectively.

关键词： Syngas Ethanol DFT cu catalyst Promoter Mo

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CO2 electrolysis at industrial current densities using anion exchange membrane based electrolyzers

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Science China Chemistry 2020年第12期63卷 1711-1715页

作者： Pengfei Wei Hefei Li Long Lin Dunfeng Gao Xiaomin Zhang Huimin Gong Guangyan Qing Rui Cai Guoxiong Wang Xinhe Bao State Key Laboratory of Catalysis Dalian National Laboratory for Clean EnergyDalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China University of Chinese Academy of Sciences Beijing 100049China

Significant progress on electrocatalytic CO2 reduction reaction (CO2RR) has been achieved in recent years.However,the research and development of electrolyzer device for CO2RR is scarce.Here we use anion exchange membrane to develop zerogap electrolyzers for CO2RR.The electrochemical properties of the electrolyzers with Pd/C and cu cathodes are investigated.The Pd/C cathode shows a current density of 200 mA cm^-2with CO Faradaic efficiency of 98%and energy efficiency of 48.8%,while the cu cathode shows a current density of 350 mA cm^-2with total CO2RR Faradaic efficiency of 81.9%and energy efficiency of 30.5%.This work provides a promising demonstration of CO2 electrolyzer using anion exchange membrane for CO2 electrolysis at industrial current densities.

关键词： CO2 electrolysis electrolyzer industrial current density anion exchange membrane energy efficiency Pd/C catalyst cu catalyst

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