The decentralized production of H_(2)O_(2) via a twoelectron oxygen reduction reaction(2e^(-)ORR)has emerged as a promising alternative to the energy-intensive anthraquinone(AQ)process.However,its practical applicatio...The decentralized production of H_(2)O_(2) via a twoelectron oxygen reduction reaction(2e^(-)ORR)has emerged as a promising alternative to the energy-intensive anthraquinone(AQ)process.However,its practical application requires 2eORR electrocatalysts with high activity and selectivity.Herein,we report the synthesis of metallic Ni nanoparticles anchored on bacterial cellulose-derived carbon fibers(Ni-NPs/BCCF)via a facile impregnation-pyrolysis method as efficient electrocatalysts for 2 e-ORR to H_(2)O_(2).By tuning the amount of Ni precursor,the best electrocatalytic performance toward 2 eORR was achieved for Ni-NPs/BCCF-20.7,affording a high H_(2)O_(2) selectivity of ~90% and an onset potential of 0.75 V vs.reversible hydrogen electrode(RHE)in an alkaline electrolyte.Ni-NPs/BCCF-20.7 achieved the largest H_(2)O_(2) yield rate of 162.7±13.7 mmol gcat^(-1)h^(-1) and the highest Faradaic efficiency of 93.9%±4.2% at 0.2 and 0.5 V vs.RHE from the bulk ORR system,respectively.Theoretical calculations revealed the more favorable"end-on"adsorption configuration of molecular oxygen on the exposed Ni(111)plane,which can effectively suppress the O-O bond dissociation,resulting in high selectivity for H_(2)O_(2) generation.展开更多
基金financially supported by the National Natural Science Foundation of China(51872292)China Postdoctoral Science Foundation(E04BFGCV)the CASHIPS Director’s Fund(YZJJ2021QN18)。
文摘The decentralized production of H_(2)O_(2) via a twoelectron oxygen reduction reaction(2e^(-)ORR)has emerged as a promising alternative to the energy-intensive anthraquinone(AQ)process.However,its practical application requires 2eORR electrocatalysts with high activity and selectivity.Herein,we report the synthesis of metallic Ni nanoparticles anchored on bacterial cellulose-derived carbon fibers(Ni-NPs/BCCF)via a facile impregnation-pyrolysis method as efficient electrocatalysts for 2 e-ORR to H_(2)O_(2).By tuning the amount of Ni precursor,the best electrocatalytic performance toward 2 eORR was achieved for Ni-NPs/BCCF-20.7,affording a high H_(2)O_(2) selectivity of ~90% and an onset potential of 0.75 V vs.reversible hydrogen electrode(RHE)in an alkaline electrolyte.Ni-NPs/BCCF-20.7 achieved the largest H_(2)O_(2) yield rate of 162.7±13.7 mmol gcat^(-1)h^(-1) and the highest Faradaic efficiency of 93.9%±4.2% at 0.2 and 0.5 V vs.RHE from the bulk ORR system,respectively.Theoretical calculations revealed the more favorable"end-on"adsorption configuration of molecular oxygen on the exposed Ni(111)plane,which can effectively suppress the O-O bond dissociation,resulting in high selectivity for H_(2)O_(2) generation.
