Enhanced Acidic CO2-to-C2+ Reduction via Ionic Liquid Layer Modification
Qiyou Wang
Hunan Joint International Research Center for Carbon Dioxide Resource Utilization, State Key Laboratory of Powder Metallurgy, School of Physics, Central South University, Changsha, 410083 P. R. China
Search for more papers by this authorYuxiang Liu
Hunan Joint International Research Center for Carbon Dioxide Resource Utilization, State Key Laboratory of Powder Metallurgy, School of Physics, Central South University, Changsha, 410083 P. R. China
Search for more papers by this authorYao Tan
Hunan Joint International Research Center for Carbon Dioxide Resource Utilization, State Key Laboratory of Powder Metallurgy, School of Physics, Central South University, Changsha, 410083 P. R. China
Search for more papers by this authorYusen Xiao
Hunan Joint International Research Center for Carbon Dioxide Resource Utilization, State Key Laboratory of Powder Metallurgy, School of Physics, Central South University, Changsha, 410083 P. R. China
Search for more papers by this authorLiling Liao
Department of Physics and Synergetic Innovation Center for Quantum Effects and Applications, Hunan Normal University, Changsha, 410081 P. R. China
Search for more papers by this authorJunwei Fu
Hunan Joint International Research Center for Carbon Dioxide Resource Utilization, State Key Laboratory of Powder Metallurgy, School of Physics, Central South University, Changsha, 410083 P. R. China
Search for more papers by this authorShilin Zhao
School of Energy Science and Engineering, Central South University, Changsha, 410083 P. R. China
Search for more papers by this authorHongmei Li
Hunan Joint International Research Center for Carbon Dioxide Resource Utilization, State Key Laboratory of Powder Metallurgy, School of Physics, Central South University, Changsha, 410083 P. R. China
Search for more papers by this authorCheng-Wei Kao
National Synchrotron Radiation Research Center, Hsinchu, 300092 Taiwan
Search for more papers by this authorTing-Shan Chan
National Synchrotron Radiation Research Center, Hsinchu, 300092 Taiwan
Search for more papers by this authorHaiqing Zhou
Department of Physics and Synergetic Innovation Center for Quantum Effects and Applications, Hunan Normal University, Changsha, 410081 P. R. China
Search for more papers by this authorFeng Li
Department of Mechanical and Industrial Engineering, University of Toronto, 5 King's College Road, Toronto, Ontario, M5S 3G8 Canada
Search for more papers by this authorLiyuan Chai
School of Metallurgy and Environment, Central South University, Changsha, Hunan, 410083 P. R. China
Search for more papers by this authorZhang Lin
School of Metallurgy and Environment, Central South University, Changsha, Hunan, 410083 P. R. China
Search for more papers by this authorCorresponding Author
Kang Liu
Hunan Joint International Research Center for Carbon Dioxide Resource Utilization, State Key Laboratory of Powder Metallurgy, School of Physics, Central South University, Changsha, 410083 P. R. China
E-mail: [email protected]; [email protected]
Search for more papers by this authorCorresponding Author
Min Liu
Hunan Joint International Research Center for Carbon Dioxide Resource Utilization, State Key Laboratory of Powder Metallurgy, School of Physics, Central South University, Changsha, 410083 P. R. China
School of Metallurgy and Environment, Central South University, Changsha, Hunan, 410083 P. R. China
E-mail: [email protected]; [email protected]
Search for more papers by this authorQiyou Wang
Hunan Joint International Research Center for Carbon Dioxide Resource Utilization, State Key Laboratory of Powder Metallurgy, School of Physics, Central South University, Changsha, 410083 P. R. China
Search for more papers by this authorYuxiang Liu
Hunan Joint International Research Center for Carbon Dioxide Resource Utilization, State Key Laboratory of Powder Metallurgy, School of Physics, Central South University, Changsha, 410083 P. R. China
Search for more papers by this authorYao Tan
Hunan Joint International Research Center for Carbon Dioxide Resource Utilization, State Key Laboratory of Powder Metallurgy, School of Physics, Central South University, Changsha, 410083 P. R. China
Search for more papers by this authorYusen Xiao
Hunan Joint International Research Center for Carbon Dioxide Resource Utilization, State Key Laboratory of Powder Metallurgy, School of Physics, Central South University, Changsha, 410083 P. R. China
Search for more papers by this authorLiling Liao
Department of Physics and Synergetic Innovation Center for Quantum Effects and Applications, Hunan Normal University, Changsha, 410081 P. R. China
Search for more papers by this authorJunwei Fu
Hunan Joint International Research Center for Carbon Dioxide Resource Utilization, State Key Laboratory of Powder Metallurgy, School of Physics, Central South University, Changsha, 410083 P. R. China
Search for more papers by this authorShilin Zhao
School of Energy Science and Engineering, Central South University, Changsha, 410083 P. R. China
Search for more papers by this authorHongmei Li
Hunan Joint International Research Center for Carbon Dioxide Resource Utilization, State Key Laboratory of Powder Metallurgy, School of Physics, Central South University, Changsha, 410083 P. R. China
Search for more papers by this authorCheng-Wei Kao
National Synchrotron Radiation Research Center, Hsinchu, 300092 Taiwan
Search for more papers by this authorTing-Shan Chan
National Synchrotron Radiation Research Center, Hsinchu, 300092 Taiwan
Search for more papers by this authorHaiqing Zhou
Department of Physics and Synergetic Innovation Center for Quantum Effects and Applications, Hunan Normal University, Changsha, 410081 P. R. China
Search for more papers by this authorFeng Li
Department of Mechanical and Industrial Engineering, University of Toronto, 5 King's College Road, Toronto, Ontario, M5S 3G8 Canada
Search for more papers by this authorLiyuan Chai
School of Metallurgy and Environment, Central South University, Changsha, Hunan, 410083 P. R. China
Search for more papers by this authorZhang Lin
School of Metallurgy and Environment, Central South University, Changsha, Hunan, 410083 P. R. China
Search for more papers by this authorCorresponding Author
Kang Liu
Hunan Joint International Research Center for Carbon Dioxide Resource Utilization, State Key Laboratory of Powder Metallurgy, School of Physics, Central South University, Changsha, 410083 P. R. China
E-mail: [email protected]; [email protected]
Search for more papers by this authorCorresponding Author
Min Liu
Hunan Joint International Research Center for Carbon Dioxide Resource Utilization, State Key Laboratory of Powder Metallurgy, School of Physics, Central South University, Changsha, 410083 P. R. China
School of Metallurgy and Environment, Central South University, Changsha, Hunan, 410083 P. R. China
E-mail: [email protected]; [email protected]
Search for more papers by this authorAbstract
Acidic CO2 electroreduction reaction (CO2RR) garners significant attention as a promising approach for cutting carbon density, as it effectively mitigates CO2 loss by suppressing carbonate species formation. Unfortunately, achieving efficient multi-carbon products (C2+) production in acidic media remains challenging due to two main limitations: weak CO adsorption on Cu sites and competitive H* adsorption caused by the high concentration protons (H+). To overcome these challenges, a cation-anion-modification strategy is proposed using an ionic liquid layer—1-Propyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide ([PMIM][NTf2])—on Cu surface. Density functional theory calculations predict that PMIM+ cation strengthens *CO adsorption through quasi-hydrogen bonding, while NTf2− anion creates a hydrophobic environment, effectively reducing H* coverage and promoting *CO adsorption. Resistance tests demonstrate that [PMIM][NTf2] modification effectively reduced proton diffusion. Attenuated total reflection infrared spectroscopy (ATR-IR) confirmed the reinforcement of *CO adsorption on the modified Cu surface. As a result, the [PMIM][NTf2] modified Cu catalyst achieved a remarkable partial current density of ≈640 mA cm−2 for C2+ products, with exceptional faradaic efficiency of 80.1% and durability of ≈20 h at a partial current density exceeding 500 mA cm−2 in a flow cell. This study highlights the potential of cation-anion modification strategies for significantly enhancing CO2RR in acidic media.
Conflict of Interest
The authors declare no conflict of interest.
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