Bismuth-based electrocatalysts are promising candidates for electrochemical CO_(2)reduction to formate attributing to the accelerated formation of*OCHO intermediate,while the high-energy consumption remains a major ch...Bismuth-based electrocatalysts are promising candidates for electrochemical CO_(2)reduction to formate attributing to the accelerated formation of*OCHO intermediate,while the high-energy consumption remains a major challenge for practicability.Herein,we present the ultrathin Bi_(2)O_(2)CO_(3)nanosheets with abundant oxygen vacancy(Vo-BOC-NS)reconstructed from S,N-co-doped bismuth oxides that can act as durable electrocatalyst for CO_(2)-to-formate conversion with faradic efficiency(FEformate)of>95%,partial current density of 286 mA cm^(-2) with energy efficiency of 73.8%at-0.62 V(vs.RHE)and low overpotential of 200 mV in a flow electrolyzer.The theoretical calculations decipher that the oxygen vacancy can optimize*OCOH adsorption/desorption for the accelerated conversion kinetics.The pair-electrosynthesis tactic of formate co-production can enable a superior FE_(formate) of>90%at wide cell voltage of 2–3.3 V and total yield rate of 3742μmol cm^(-2)h^(-1)at 3.3 V,suggesting great potential for future industrialization.展开更多
A hybrid catalyst structure can provide abundant active sites and tailored electronic properties,but the major challenge lies in achieving delicate control over its composition and architecture to improve the catalyti...A hybrid catalyst structure can provide abundant active sites and tailored electronic properties,but the major challenge lies in achieving delicate control over its composition and architecture to improve the catalytic activity toward different electrochemical reactions simultaneously.Herein,we present the rational design of a magic hybrid structure with low Pt loading(5.90 wt%),composed of CoPt_(3)and CoPt nanoparticles supported on N-doped carbon(CoPt_(3)/CoPt⊂PLNC).Importantly,it shows superior multifunctional catalytic activity in alkaline conditions,requiring a low overpotential of 341 and 20 mV to achieve 10 mA cm^(−2)for the hydrazine oxidation reaction(HzOR)/hydrogen evolution reaction(HER),respectively,and it delivers a half-wave potential of 0.847 V for the oxygen reduction reaction(ORR).Theoretical calculations reveal that the metal-carbon hybrid modulates kinetic behavior and induces electron redistribution,achieving the energetic requirements for multiple electrocatalysis.We demonstrate sustainable H_(2)production utilizing solely the CoPt_(3)/CoPt⊂PLNC catalyst,without external electric power input,suggesting its inspiring practical utility.展开更多
基金Genqiang Zhang acknowledges the financial support from the National Natural Science Foundation of China(Grant No.52072359)the Recruitment Program of Global Experts and the Fundamental Research Funds for the Central Universities(WK2060000016).
文摘Bismuth-based electrocatalysts are promising candidates for electrochemical CO_(2)reduction to formate attributing to the accelerated formation of*OCHO intermediate,while the high-energy consumption remains a major challenge for practicability.Herein,we present the ultrathin Bi_(2)O_(2)CO_(3)nanosheets with abundant oxygen vacancy(Vo-BOC-NS)reconstructed from S,N-co-doped bismuth oxides that can act as durable electrocatalyst for CO_(2)-to-formate conversion with faradic efficiency(FEformate)of>95%,partial current density of 286 mA cm^(-2) with energy efficiency of 73.8%at-0.62 V(vs.RHE)and low overpotential of 200 mV in a flow electrolyzer.The theoretical calculations decipher that the oxygen vacancy can optimize*OCOH adsorption/desorption for the accelerated conversion kinetics.The pair-electrosynthesis tactic of formate co-production can enable a superior FE_(formate) of>90%at wide cell voltage of 2–3.3 V and total yield rate of 3742μmol cm^(-2)h^(-1)at 3.3 V,suggesting great potential for future industrialization.
基金G.Q.Zhang acknowledges the financial support from the National Natural Science Foundation of China(Grant No.52072359)the Recruitment Program of Global Experts and the Fundamental Research Funds for the Central Universities(WK2060000016)The numerical calculations in this paper have been done in the Supercomputing Center of University of Science and Technology of China and TianHe-2 at LvLiang Cloud Computing Center of China.W.T.W.acknowledges the Natural Science Foundation from science and technology department of Guizhou Province(Nos.QHPT[2017]5790-02).
文摘A hybrid catalyst structure can provide abundant active sites and tailored electronic properties,but the major challenge lies in achieving delicate control over its composition and architecture to improve the catalytic activity toward different electrochemical reactions simultaneously.Herein,we present the rational design of a magic hybrid structure with low Pt loading(5.90 wt%),composed of CoPt_(3)and CoPt nanoparticles supported on N-doped carbon(CoPt_(3)/CoPt⊂PLNC).Importantly,it shows superior multifunctional catalytic activity in alkaline conditions,requiring a low overpotential of 341 and 20 mV to achieve 10 mA cm^(−2)for the hydrazine oxidation reaction(HzOR)/hydrogen evolution reaction(HER),respectively,and it delivers a half-wave potential of 0.847 V for the oxygen reduction reaction(ORR).Theoretical calculations reveal that the metal-carbon hybrid modulates kinetic behavior and induces electron redistribution,achieving the energetic requirements for multiple electrocatalysis.We demonstrate sustainable H_(2)production utilizing solely the CoPt_(3)/CoPt⊂PLNC catalyst,without external electric power input,suggesting its inspiring practical utility.
