Electrocatalytic nitrogen reduction reaction is a carbon-free and energy-saving strategy for efficient synthesis of ammonia under ambient conditions.Here,we report the synthesis of nanosized Bi2O3 particles grown on f...Electrocatalytic nitrogen reduction reaction is a carbon-free and energy-saving strategy for efficient synthesis of ammonia under ambient conditions.Here,we report the synthesis of nanosized Bi2O3 particles grown on functionalized exfoliated graphene(Bi2O3/FEG)via a facile electrochemical deposition method.The obtained free-standing Bi2O3/FEG achieves a high Faradaic efficiency of 11.2%and a large NH3 yield of 4.21±0.14μgNH3 h^-1 cm^-2 at-0.5 V versus reversible hydrogen electrode in 0.1 M Na2SO4,better than that in the strong acidic and basic media.Benefiting from its strong interaction of Bi 6p band with the N2p orbitals,binder-free characteristic,and facile electron transfer,Bi2O3/FEG achieves superior catalytic performance and excellent long-term stability as compared with most of the previous reported catalysts.This study is significant to design low-cost,high-efficient Bi-based electrocatalysts for electrochemical ammonia synthesis.展开更多
The BiOCl(BOC)synthesized by the water bath heating method was treated with sodium borohydride(NaBH_(4))to introduce oxygen vacancies(OVs).At the same time,Au nanoparticles were loaded to prepare a series of Au/BiOCl ...The BiOCl(BOC)synthesized by the water bath heating method was treated with sodium borohydride(NaBH_(4))to introduce oxygen vacancies(OVs).At the same time,Au nanoparticles were loaded to prepare a series of Au/BiOCl samples with different ratios.OVs and Au nanoparticles can promote the light absorption of host photocatalyst in the visible region.The calculated work function of BiOCl and Au can verify the existence of Ohmic contact between the interface of them,which is conducive to the separation of charge carriers.Through a series of photoelectric tests,it was verified experimentally that the separation of charge carriers is indeed enhanced.The high-energy hot electrons produced by Au under the surface plasmon resonance(SPR)effect can increase the counts of electrons to participate in the CO_(2)reduction reaction.Especially for 1.0%-Au/BOC,the yields of CO can reach 43.16μmol g^(−1)h^(−1),which is 6.6 times more than that of BOC.Therefore,loading precious metal on semiconductors is an effective strategy to promote the photocatalytic performance of CO_(2)reduction reactions.展开更多
基金financially supported by Liaoning Revitalization Talents Program—Pan Deng Scholars(XLYC1802005)Liaoning BaiQianWan Talents Program+4 种基金the National Science Fund of Liaoning Province for Excellent Young ScholarsScience and Technology Innovative Talents Support Program of Shenyang(RC180166)Australian Research Council(ARC)through Discovery Early Career Researcher Award(DE150101306)and Linkage Project(LP160100927)Faculty of Science Strategic Investment Funding of University of NewcastleCSIRO Newcastl Energy Centre。
文摘Electrocatalytic nitrogen reduction reaction is a carbon-free and energy-saving strategy for efficient synthesis of ammonia under ambient conditions.Here,we report the synthesis of nanosized Bi2O3 particles grown on functionalized exfoliated graphene(Bi2O3/FEG)via a facile electrochemical deposition method.The obtained free-standing Bi2O3/FEG achieves a high Faradaic efficiency of 11.2%and a large NH3 yield of 4.21±0.14μgNH3 h^-1 cm^-2 at-0.5 V versus reversible hydrogen electrode in 0.1 M Na2SO4,better than that in the strong acidic and basic media.Benefiting from its strong interaction of Bi 6p band with the N2p orbitals,binder-free characteristic,and facile electron transfer,Bi2O3/FEG achieves superior catalytic performance and excellent long-term stability as compared with most of the previous reported catalysts.This study is significant to design low-cost,high-efficient Bi-based electrocatalysts for electrochemical ammonia synthesis.
基金supported by the National Natural Science Foundation of China(Nos.51772183.52072230)the Yulin Science and Technology Project(No.CXY-2020-040)。
文摘The BiOCl(BOC)synthesized by the water bath heating method was treated with sodium borohydride(NaBH_(4))to introduce oxygen vacancies(OVs).At the same time,Au nanoparticles were loaded to prepare a series of Au/BiOCl samples with different ratios.OVs and Au nanoparticles can promote the light absorption of host photocatalyst in the visible region.The calculated work function of BiOCl and Au can verify the existence of Ohmic contact between the interface of them,which is conducive to the separation of charge carriers.Through a series of photoelectric tests,it was verified experimentally that the separation of charge carriers is indeed enhanced.The high-energy hot electrons produced by Au under the surface plasmon resonance(SPR)effect can increase the counts of electrons to participate in the CO_(2)reduction reaction.Especially for 1.0%-Au/BOC,the yields of CO can reach 43.16μmol g^(−1)h^(−1),which is 6.6 times more than that of BOC.Therefore,loading precious metal on semiconductors is an effective strategy to promote the photocatalytic performance of CO_(2)reduction reactions.
