The exploration of efficient electrocatalysts for the reduction of CO2 to C2H4 is of significant importance but is also a challenging subject.Cu-based bimetallic catalysts are extremely promising for efficient CO2 red...The exploration of efficient electrocatalysts for the reduction of CO2 to C2H4 is of significant importance but is also a challenging subject.Cu-based bimetallic catalysts are extremely promising for efficient CO2 reduction.In this work,we synthesize a series of porous bimetallic Cu–Sb alloys with different compositions for the catalytic reduction of CO2 to C2H4.It is demonstrated that the alloy catalysts are much more efficient than the pure Cu catalyst.The performance of the alloy catalysts depended strongly on the composition.Further,the alloy with a Cu:Sb ratio of 10:1 yielded the best results;it exhibited a high C2H4 Faradaic efficiency of 49.7%and a high current density of 28.5 mA cm?2 at?1.19 V vs.a reversible hydrogen electrode(RHE)in 0.1 M KCl solution.To the best of our knowledge,the electrocatalytic reduction of CO2 to C2H4 using Cu–Sb alloys as catalysts has not been reported.The excellent performance of the porous alloy catalyst is attributed to its favorable electronic configuration,large surface area,high CO2 adsorption rate,and fast charge transfer rate.展开更多
Multifunctional catalysts that integrate high efficiency hydrogen evolution reaction(HER), oxygen evolution reaction(OER) and oxygen reduction reaction(ORR) catalytic activity in a single material are attractive for u...Multifunctional catalysts that integrate high efficiency hydrogen evolution reaction(HER), oxygen evolution reaction(OER) and oxygen reduction reaction(ORR) catalytic activity in a single material are attractive for unitized regenerative fuel cells and overall water splitting technologies. As the best-known HER and ORR electrocatalysts, Pt and its alloys have only moderate OER activity. Ruthenium and iridium oxides exhibit the highest OER activities but not as active as Pt for HER and ORR. Here, we proposed a general principle for achieving trifunctional electrocatalysis for three reactions in a single material. Using the newly-synthesized pyrazine-modified graphdiyne(PR-GDY) as an example, we demonstrated that the synergistic effect of the pyridinic nitrogen and anchored transition-metal(TM) single atoms renders highly-efficient HER/OER/ORR trifunctional electrocatalytic activity. For the Ni-doped PR-GDY, the overpotentials for HER, OER and ORR can be respectively as low as -0.05, 0.29 and 0.38 V, which are comparable or even superior to the best-known single-functional and bi-functional precious electrocatalysts.These computational results offer not only a promising trifunctional electrocatalyst but also a strategy for the design of multifunctional electrocatalysts.展开更多
文摘The exploration of efficient electrocatalysts for the reduction of CO2 to C2H4 is of significant importance but is also a challenging subject.Cu-based bimetallic catalysts are extremely promising for efficient CO2 reduction.In this work,we synthesize a series of porous bimetallic Cu–Sb alloys with different compositions for the catalytic reduction of CO2 to C2H4.It is demonstrated that the alloy catalysts are much more efficient than the pure Cu catalyst.The performance of the alloy catalysts depended strongly on the composition.Further,the alloy with a Cu:Sb ratio of 10:1 yielded the best results;it exhibited a high C2H4 Faradaic efficiency of 49.7%and a high current density of 28.5 mA cm?2 at?1.19 V vs.a reversible hydrogen electrode(RHE)in 0.1 M KCl solution.To the best of our knowledge,the electrocatalytic reduction of CO2 to C2H4 using Cu–Sb alloys as catalysts has not been reported.The excellent performance of the porous alloy catalyst is attributed to its favorable electronic configuration,large surface area,high CO2 adsorption rate,and fast charge transfer rate.
基金supported by the Basic Research Project of Natural Science Foundation of Shandong Province(ZR2018ZB0751)the National Natural Science Foundation of China(11774201)the Taishan Scholar Program of Shandong Province。
文摘Multifunctional catalysts that integrate high efficiency hydrogen evolution reaction(HER), oxygen evolution reaction(OER) and oxygen reduction reaction(ORR) catalytic activity in a single material are attractive for unitized regenerative fuel cells and overall water splitting technologies. As the best-known HER and ORR electrocatalysts, Pt and its alloys have only moderate OER activity. Ruthenium and iridium oxides exhibit the highest OER activities but not as active as Pt for HER and ORR. Here, we proposed a general principle for achieving trifunctional electrocatalysis for three reactions in a single material. Using the newly-synthesized pyrazine-modified graphdiyne(PR-GDY) as an example, we demonstrated that the synergistic effect of the pyridinic nitrogen and anchored transition-metal(TM) single atoms renders highly-efficient HER/OER/ORR trifunctional electrocatalytic activity. For the Ni-doped PR-GDY, the overpotentials for HER, OER and ORR can be respectively as low as -0.05, 0.29 and 0.38 V, which are comparable or even superior to the best-known single-functional and bi-functional precious electrocatalysts.These computational results offer not only a promising trifunctional electrocatalyst but also a strategy for the design of multifunctional electrocatalysts.
