Electrochemical CO_(2)reduction reaction(CO_(2)RR)to high-value product,CO,not only provides a key feedstock for the wellestablished Fischer-Tropsch process but also mitigates the greenhouse effect.However,it suffers ...Electrochemical CO_(2)reduction reaction(CO_(2)RR)to high-value product,CO,not only provides a key feedstock for the wellestablished Fischer-Tropsch process but also mitigates the greenhouse effect.However,it suffers from sluggish reaction kinetics,competitive hydrogen evolution reaction,and low selectivity.Herein,we report non-precious Cu-Sn diatomic sites anchored on nitrogen-doped porous carbon(CuSn/NPC)as an efficient catalyst for CO_(2)RR to CO.The catalyst exhibits outstanding selectivity with CO Faradaic efficiency(FE)up to 99.1%,much higher than those of individual Cu(66.2%)and Sn(51.3%)single-atom catalysts.Moreover,high stability is confirmed by consecutive 24 h electrolysis with high selectivity from CO_(2)to CO.Theoretical calculations reveal an obvious activation of CO_(2)with weakened C-O bonds and distorted CO_(2)configuration upon chemisorption on the CuSn/NPC catalyst.It is also suggested CuSn/NPC is more selective for the CO_(2)RR with dominant CO production during the electrolysis,rather than the competing hydrogen evolution reaction.展开更多
基金This work was supported by the startup funding of H.L.X.The XAFS/EXAFS spectra obtained from beamline TPS 44A at National Synchrotron Radiation Research Center(NSRRC)are appreciated.
文摘Electrochemical CO_(2)reduction reaction(CO_(2)RR)to high-value product,CO,not only provides a key feedstock for the wellestablished Fischer-Tropsch process but also mitigates the greenhouse effect.However,it suffers from sluggish reaction kinetics,competitive hydrogen evolution reaction,and low selectivity.Herein,we report non-precious Cu-Sn diatomic sites anchored on nitrogen-doped porous carbon(CuSn/NPC)as an efficient catalyst for CO_(2)RR to CO.The catalyst exhibits outstanding selectivity with CO Faradaic efficiency(FE)up to 99.1%,much higher than those of individual Cu(66.2%)and Sn(51.3%)single-atom catalysts.Moreover,high stability is confirmed by consecutive 24 h electrolysis with high selectivity from CO_(2)to CO.Theoretical calculations reveal an obvious activation of CO_(2)with weakened C-O bonds and distorted CO_(2)configuration upon chemisorption on the CuSn/NPC catalyst.It is also suggested CuSn/NPC is more selective for the CO_(2)RR with dominant CO production during the electrolysis,rather than the competing hydrogen evolution reaction.
