Engineering the desired dual metal sites to realize C-C coupling of CO_(2)is of great importance for the practical applications of CO_(2)electroreduction reaction(CER).Herein,an efficient strategy for constructing het...Engineering the desired dual metal sites to realize C-C coupling of CO_(2)is of great importance for the practical applications of CO_(2)electroreduction reaction(CER).Herein,an efficient strategy for constructing heterogeneous Pt^(δ+)-Cu^(δ+)dual sites to strengthen the generation and coupling of*CO and*CHO(or*COH)during CER process is presented in this work.The radiilarger Pt not only stabilizes the Cu^(δ+)ut also induces a tensile strain in Pt^(δ+)-Cu^(δ+)dual sites.The obtained Pt^(δ+)-Cu^(δ+)dual sites achieve a total Faradaic efficiency and current density of C2products with 70.9%and586.9 mA·cm-2at-1.20 V(vs.RHE),which is higher than that of Cu^(δ+)single site(55.4%,286.9 mA·cm^(-2)).The in situ attenuated total reflection surface-enhanced infrared absorption spectroscopy(ATR-SEIRAS)reveals that the Pt^(δ+)-Cu^(δ+)dual sites can promote the generation of C1intermediates(such as*CO,*COOH,*COH,and*CHO)and C-C coupling.Additional in situ surface-enhanced Raman spectra demonstrate that Pt^(δ+)Cu^(δ+)dual sites can induce the generation of the high-frequency peak for*CO_(atop),thus accelerating the C-C coupling.This work provides a promising avenue for stabilizing and enhancing the performance of Cu^(δ+)sites toward CER.展开更多
基金financially supported by the National Natural Science Foundation of China(No.22305101)the Natural Science Foundation of Jiangsu Province(No.BK20231032)+2 种基金the Special Fund Project of Jiangsu Province for Scientific and Technological Innovation in Carbon Peaking and Carbon Neutrality(No.BK20220023)the Fundamental Research Funds for the Central Universities(No.JUSRP123020)the Startup Funding at Jiangnan University(No.1045219032220100)。
文摘Engineering the desired dual metal sites to realize C-C coupling of CO_(2)is of great importance for the practical applications of CO_(2)electroreduction reaction(CER).Herein,an efficient strategy for constructing heterogeneous Pt^(δ+)-Cu^(δ+)dual sites to strengthen the generation and coupling of*CO and*CHO(or*COH)during CER process is presented in this work.The radiilarger Pt not only stabilizes the Cu^(δ+)ut also induces a tensile strain in Pt^(δ+)-Cu^(δ+)dual sites.The obtained Pt^(δ+)-Cu^(δ+)dual sites achieve a total Faradaic efficiency and current density of C2products with 70.9%and586.9 mA·cm-2at-1.20 V(vs.RHE),which is higher than that of Cu^(δ+)single site(55.4%,286.9 mA·cm^(-2)).The in situ attenuated total reflection surface-enhanced infrared absorption spectroscopy(ATR-SEIRAS)reveals that the Pt^(δ+)-Cu^(δ+)dual sites can promote the generation of C1intermediates(such as*CO,*COOH,*COH,and*CHO)and C-C coupling.Additional in situ surface-enhanced Raman spectra demonstrate that Pt^(δ+)Cu^(δ+)dual sites can induce the generation of the high-frequency peak for*CO_(atop),thus accelerating the C-C coupling.This work provides a promising avenue for stabilizing and enhancing the performance of Cu^(δ+)sites toward CER.
