The electrochemical CO_(2) reduction reaction(CO_(2)RR)to produce syngas offers a powerful strategy for achieving sustainable chemical production.Achieving syngas with tunable CO/H_(2) ratios within a wide potential w...The electrochemical CO_(2) reduction reaction(CO_(2)RR)to produce syngas offers a powerful strategy for achieving sustainable chemical production.Achieving syngas with tunable CO/H_(2) ratios within a wide potential window is highly desirable but challenging.Here,by doping Ga into Cu_(2)(OH)_(2)CO_(3) to engineer the interfacial hydrophobicity and electronic structure,we effectively controlled CO and H_(2) production during CO_(2) electroreduction.We tuned the CO/H_(2) ratio from 0.15 to 2.1,achieving a maximum 100% syngas production in a wide potential window(-0.6 to -1.8 V vs.RHE).Various characterization techniques,including in situ attenuated total reflection surface-enhanced infrared absorption spectroscopy(ATR-SEIRAS)and in situ electrochemical impedance spectroscopy(EIS),revealed that appropriate Ga doping into Cu_(2)(OH)2CO_(3) facilitates CO_(2) mass transfer at the catalyst surface,thereby enhancing CO_(2)RR activity.In contrast,when the Ga doping ratio reaches 1.0,excessive surface hydrophobicity hinders CO_(2) reduction but facilitates the hydrogen evolution reaction(HER).Moreover,the Ga-induced modulation of the Cu+/Cu^(2+)ratio further exerts a synergistic effect on C^(2+)product selectivity.Additionally,as the Ga doping increases,the*CO binding configuration shifts from linearly bonded to bridge bonded,revealing the reaction pathway.This versatile control of the CO/H_(2) ratio in the CO_(2)RR offers significant opportunities for the direct transformation of CO_(2) into syngas.展开更多
基金supported by the National Natural Science Foundation of China(22035002,22378192,and U22B20148)the Jiangsu Funding Program for Excellent Postdoctoral Talent(2024ZB272)+1 种基金the Postdoctoral Fellowship Program of China Postdoctoral Science Foundation(GZC20240701)the International Science and Technology Cooperation Project of Innovative Supporting Plan of Jiangsu Province(BZ2022040).
文摘The electrochemical CO_(2) reduction reaction(CO_(2)RR)to produce syngas offers a powerful strategy for achieving sustainable chemical production.Achieving syngas with tunable CO/H_(2) ratios within a wide potential window is highly desirable but challenging.Here,by doping Ga into Cu_(2)(OH)_(2)CO_(3) to engineer the interfacial hydrophobicity and electronic structure,we effectively controlled CO and H_(2) production during CO_(2) electroreduction.We tuned the CO/H_(2) ratio from 0.15 to 2.1,achieving a maximum 100% syngas production in a wide potential window(-0.6 to -1.8 V vs.RHE).Various characterization techniques,including in situ attenuated total reflection surface-enhanced infrared absorption spectroscopy(ATR-SEIRAS)and in situ electrochemical impedance spectroscopy(EIS),revealed that appropriate Ga doping into Cu_(2)(OH)2CO_(3) facilitates CO_(2) mass transfer at the catalyst surface,thereby enhancing CO_(2)RR activity.In contrast,when the Ga doping ratio reaches 1.0,excessive surface hydrophobicity hinders CO_(2) reduction but facilitates the hydrogen evolution reaction(HER).Moreover,the Ga-induced modulation of the Cu+/Cu^(2+)ratio further exerts a synergistic effect on C^(2+)product selectivity.Additionally,as the Ga doping increases,the*CO binding configuration shifts from linearly bonded to bridge bonded,revealing the reaction pathway.This versatile control of the CO/H_(2) ratio in the CO_(2)RR offers significant opportunities for the direct transformation of CO_(2) into syngas.
