Electrocatalytic CO_(2)reduction reaction(CO_(2)RR)to produce multicarbon(C_(2+))products over Cubased catalysts represents an ideal approach for renewable energy storage and carbon emissions reduction.The Cu^(0)/Cu^(...Electrocatalytic CO_(2)reduction reaction(CO_(2)RR)to produce multicarbon(C_(2+))products over Cubased catalysts represents an ideal approach for renewable energy storage and carbon emissions reduction.The Cu^(0)/Cu^(δ+)interfaces are widely recognized as crucial sites that promote C-C coupling and enhance the generation of C2+products.However,a major challenge arises from the tendency of Cu^(δ+)active sites within Cu^(0)/Cu^(δ+)interfaces to undergo reduction to Cu^(0)during the CO_(2)RR process,leading to a decline in catalytic performance.Hence,it is crucial to establish durable Cu^(0)/Cu^(δ+)interfaces to enhance the conversion of CO_(2)to C_(2+)products.In this work,an iodine modification strategy is proposed to prepare a stable Cu@CuI composite catalyst with well-maintained Cu^(0)/Cu^(δ+)interfaces through a one-step redox reaction between iodine and copper.The optimized Cu@CuI-3composite catalyst demonstrates an excellent performance in CO_(2)RR,achieving a Faradaic efficiency of 75.7%for C^(2+)products and a partial current density of 288 mA·cm^(-2)at-1.57 V_(RHE)in a flow cell.Operando techniques reveal that a numerous persistent Cu^(δ+)species exist on the surface of the Cu@CuI-X composite catalyst even after CO_(2)RR due to the presence of adsorbed iodine ions,which prevent complete reduction of Cu^(δ+)species to Cu^(0)owing to their high electronegativity.Density functional theory calculations further verify that adsorbed iodine ions on the surface of Cu@CuI-X serve as charge regulators by adjusting local charge density,thereby facilitating the formation of*CHO intermediates from CO_(2)and lowering the energy barriers associated with coupling the*CHO and*CO intermediates during CO_(2)RR.Consequently,this phenomenon enhances the selectivity toward C_(2+)products during electrocatalytic CO_(2)reduction.展开更多
针对传统采集系统价格昂贵、接口不灵活、实时性差等缺点,提出一种基于LabWindows/CVI的高速数据采集系统。该系统使用Universal Serial BUS 2.0(USB2.0)接口,以LabWindows/CVI搭建数据采集系统的软件平台,采用调用动态链接库的方法完...针对传统采集系统价格昂贵、接口不灵活、实时性差等缺点,提出一种基于LabWindows/CVI的高速数据采集系统。该系统使用Universal Serial BUS 2.0(USB2.0)接口,以LabWindows/CVI搭建数据采集系统的软件平台,采用调用动态链接库的方法完成上位机和系统间的通信,利用LabWindows/CVI的多线程实现数据的实时采集。试验结果表明:该系统调试方便、界面友好、实时性好、运行稳定,可广泛使用。展开更多
基金financially supported by the National Natural Science Foundation of China(Nos.52073009,52272182,51872013 and 52011530190)the Program of the Ministry of Education of China for Introducing Talents of Discipline to Universities(No.B14009)。
文摘Electrocatalytic CO_(2)reduction reaction(CO_(2)RR)to produce multicarbon(C_(2+))products over Cubased catalysts represents an ideal approach for renewable energy storage and carbon emissions reduction.The Cu^(0)/Cu^(δ+)interfaces are widely recognized as crucial sites that promote C-C coupling and enhance the generation of C2+products.However,a major challenge arises from the tendency of Cu^(δ+)active sites within Cu^(0)/Cu^(δ+)interfaces to undergo reduction to Cu^(0)during the CO_(2)RR process,leading to a decline in catalytic performance.Hence,it is crucial to establish durable Cu^(0)/Cu^(δ+)interfaces to enhance the conversion of CO_(2)to C_(2+)products.In this work,an iodine modification strategy is proposed to prepare a stable Cu@CuI composite catalyst with well-maintained Cu^(0)/Cu^(δ+)interfaces through a one-step redox reaction between iodine and copper.The optimized Cu@CuI-3composite catalyst demonstrates an excellent performance in CO_(2)RR,achieving a Faradaic efficiency of 75.7%for C^(2+)products and a partial current density of 288 mA·cm^(-2)at-1.57 V_(RHE)in a flow cell.Operando techniques reveal that a numerous persistent Cu^(δ+)species exist on the surface of the Cu@CuI-X composite catalyst even after CO_(2)RR due to the presence of adsorbed iodine ions,which prevent complete reduction of Cu^(δ+)species to Cu^(0)owing to their high electronegativity.Density functional theory calculations further verify that adsorbed iodine ions on the surface of Cu@CuI-X serve as charge regulators by adjusting local charge density,thereby facilitating the formation of*CHO intermediates from CO_(2)and lowering the energy barriers associated with coupling the*CHO and*CO intermediates during CO_(2)RR.Consequently,this phenomenon enhances the selectivity toward C_(2+)products during electrocatalytic CO_(2)reduction.
文摘针对传统采集系统价格昂贵、接口不灵活、实时性差等缺点,提出一种基于LabWindows/CVI的高速数据采集系统。该系统使用Universal Serial BUS 2.0(USB2.0)接口,以LabWindows/CVI搭建数据采集系统的软件平台,采用调用动态链接库的方法完成上位机和系统间的通信,利用LabWindows/CVI的多线程实现数据的实时采集。试验结果表明:该系统调试方便、界面友好、实时性好、运行稳定,可广泛使用。
