The ability to adjust the composition and surface structure of Cu-based nanomaterials is important for designing catalysts to effectively convert CO_(2) into multi-carbon products via electrocatalytic reduction.Herein...The ability to adjust the composition and surface structure of Cu-based nanomaterials is important for designing catalysts to effectively convert CO_(2) into multi-carbon products via electrocatalytic reduction.Herein we report a potential-driven in situ forming Cu/Cu_(2)O catalyst featuring interface and tensile strain characteristics from the partial reduction of Cu_(2)O nanocubes for electrocatalytic enhancement of the electrochemical CO_(2) reduction reaction(CO_(2)RR).The results revealed interesting catalytic relationships between Cu^(+)–Cu^(0) compositions and tensile strain,exhibiting maximum faradaic efficiencies for C2 products in the H-type cell at a Cu^(0):Cu^(+)ratio of∼46:54.As revealed by operando X-ray diffraction analysis,Cu/Cu_(2)O in this ratio exhibits a clear tensile strain in Cu during the CO_(2)RR.The outstanding performance of this composition is attributed to the tensile strain and interface of the surface,in addition to the composition synergy due to the Cu^(0) sites decorating the surface in an electron-rich state and being conducive to CO_(2) adsorption and activation and the Cu^(+) sites enhancing the carbon–carbon coupling to adsorbed ^(*)CO,which were also supported by density functional theory(DFT)calculations and in situ ATR-FTIR.The findings open up a new pathway for the rational design of Cu-based catalysts with enhanced activity and selectivity to boost the CO_(2)RR.展开更多
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文摘The ability to adjust the composition and surface structure of Cu-based nanomaterials is important for designing catalysts to effectively convert CO_(2) into multi-carbon products via electrocatalytic reduction.Herein we report a potential-driven in situ forming Cu/Cu_(2)O catalyst featuring interface and tensile strain characteristics from the partial reduction of Cu_(2)O nanocubes for electrocatalytic enhancement of the electrochemical CO_(2) reduction reaction(CO_(2)RR).The results revealed interesting catalytic relationships between Cu^(+)–Cu^(0) compositions and tensile strain,exhibiting maximum faradaic efficiencies for C2 products in the H-type cell at a Cu^(0):Cu^(+)ratio of∼46:54.As revealed by operando X-ray diffraction analysis,Cu/Cu_(2)O in this ratio exhibits a clear tensile strain in Cu during the CO_(2)RR.The outstanding performance of this composition is attributed to the tensile strain and interface of the surface,in addition to the composition synergy due to the Cu^(0) sites decorating the surface in an electron-rich state and being conducive to CO_(2) adsorption and activation and the Cu^(+) sites enhancing the carbon–carbon coupling to adsorbed ^(*)CO,which were also supported by density functional theory(DFT)calculations and in situ ATR-FTIR.The findings open up a new pathway for the rational design of Cu-based catalysts with enhanced activity and selectivity to boost the CO_(2)RR.
