Tailoring the nanostructure/morphology and chemical composition is important to regulate the electronic configuration of electrocatalysts and thus enhance their performance for water and urea electrolysis.Herein,the n...Tailoring the nanostructure/morphology and chemical composition is important to regulate the electronic configuration of electrocatalysts and thus enhance their performance for water and urea electrolysis.Herein,the nitrogen-doped carbon-decorated tricomponent metal phosphides of FeP4 nanotube@Ni-Co-P nanocage(NC-FNCP)with unique nested hollow architectures are fabricated by a self-sacrifice template strategy.Benefiting from the multi-component synergy,the modification of nitrogen-doped carbon,and the modulation of nested porous hollow morphology,NC-FNCP facilitates rapid electron/mass transport in water and urea electrolysis.NC-FNCP-based anode shows low potentials of 248 mV and 1.37 V(vs.reversible hydrogen electrode)to attain 10 mA/cm^(2) for oxygen evolution reaction(OER)and urea oxidation reaction(UOR),respectively.In addition,the overall urea electrolysis drives 10 mA/cm^(2) at a comparatively low voltage of 1.52 V(vs.RHE)that is 110 mV lower than that of overall water electrolysis,as well as exhibits excellent stability over 20 h.This work strategizes a multi-shell-structured electrocatalyst with multi-compositions and explores its applications in a sustainable combination of hydrogen production and sewage remediation.展开更多
Developing low-cost,efficient,and stable non-precious-metal electrocatalysts with controlled crystal structure,morphology and compositions are highly desirable for hydrogen and oxygen evolution reactions.Herein,a seri...Developing low-cost,efficient,and stable non-precious-metal electrocatalysts with controlled crystal structure,morphology and compositions are highly desirable for hydrogen and oxygen evolution reactions.Herein,a series of phosphorus-doped Fe_(7)S_(8)nanowires integrated within carbon(P-Fe_(7)S_(8)@C)are rationally synthesized via a one-step phosphorization of one-dimensional(1D)Fe-based organicinorganic nanowires.The as-obtained P-Fe_(7)S_(8)@C catalysts with modified electronic configurations present typical porous structure,providing plentiful active sites for rapid reaction kinetics.Density functional calculations demonstrate that the doping Fe_(7)S_(8)with P can effectively enhance the electron density of Fe_(7)S_(8)around the Fermi level and weaken the Fe-H bonding,leading to the decrease of adsorption free energy barrier on active sites.As a result,the optimal catalyst of P-Fe_(7)S_(8)-600@C exhibits a relatively low overpotential of 136 mV for hydrogen evolution reaction(HER)to reach the current density of 10 mA/cm^(2),and a significantly low overpotential of 210 mV for oxygen evolution reaction(OER)at 20 mA/cm^(2)in alkaline media.The work presented here may pave the way to design and synthesis of other prominent Fe-based catalysts for water splitting via electronic regulation.展开更多
基金the National Natural Science Foundation of China(No.21601120)the Science and Technology Commission of Shanghai Municipality(Nos.17ZR1410500 and 19ZR1418100)+3 种基金Science and Technology Program of Shanghai(No.21010500300)STINT Joint China-Sweden Mobility Project(No.CH2017-7243)Swedish Government strategic faculty grant in material science(SFO,MATLIU)in Advanced Functional Materials(AFM)(VR Dnr.5.1-2015-5959)We also appreciate the High-Performance Computing Center of Shanghai University,and Shanghai Engineering Research Center of Intelligent Computing System(No.19DZ2252600)for providing the computing resources and technical support.
文摘Tailoring the nanostructure/morphology and chemical composition is important to regulate the electronic configuration of electrocatalysts and thus enhance their performance for water and urea electrolysis.Herein,the nitrogen-doped carbon-decorated tricomponent metal phosphides of FeP4 nanotube@Ni-Co-P nanocage(NC-FNCP)with unique nested hollow architectures are fabricated by a self-sacrifice template strategy.Benefiting from the multi-component synergy,the modification of nitrogen-doped carbon,and the modulation of nested porous hollow morphology,NC-FNCP facilitates rapid electron/mass transport in water and urea electrolysis.NC-FNCP-based anode shows low potentials of 248 mV and 1.37 V(vs.reversible hydrogen electrode)to attain 10 mA/cm^(2) for oxygen evolution reaction(OER)and urea oxidation reaction(UOR),respectively.In addition,the overall urea electrolysis drives 10 mA/cm^(2) at a comparatively low voltage of 1.52 V(vs.RHE)that is 110 mV lower than that of overall water electrolysis,as well as exhibits excellent stability over 20 h.This work strategizes a multi-shell-structured electrocatalyst with multi-compositions and explores its applications in a sustainable combination of hydrogen production and sewage remediation.
基金the National Natural Science Foundation of China(Nos.21601120 and 21805181)the Science and Technology Commission of Shanghai Municipality(Nos.17ZR1410500 and 19ZR1418100)+1 种基金the High Performance Computing Center of Shanghai UniversityShanghai Engineering Research Center of Intelligent Computing System(No.19DZ2252600)for providing the computing resources and technical support。
文摘Developing low-cost,efficient,and stable non-precious-metal electrocatalysts with controlled crystal structure,morphology and compositions are highly desirable for hydrogen and oxygen evolution reactions.Herein,a series of phosphorus-doped Fe_(7)S_(8)nanowires integrated within carbon(P-Fe_(7)S_(8)@C)are rationally synthesized via a one-step phosphorization of one-dimensional(1D)Fe-based organicinorganic nanowires.The as-obtained P-Fe_(7)S_(8)@C catalysts with modified electronic configurations present typical porous structure,providing plentiful active sites for rapid reaction kinetics.Density functional calculations demonstrate that the doping Fe_(7)S_(8)with P can effectively enhance the electron density of Fe_(7)S_(8)around the Fermi level and weaken the Fe-H bonding,leading to the decrease of adsorption free energy barrier on active sites.As a result,the optimal catalyst of P-Fe_(7)S_(8)-600@C exhibits a relatively low overpotential of 136 mV for hydrogen evolution reaction(HER)to reach the current density of 10 mA/cm^(2),and a significantly low overpotential of 210 mV for oxygen evolution reaction(OER)at 20 mA/cm^(2)in alkaline media.The work presented here may pave the way to design and synthesis of other prominent Fe-based catalysts for water splitting via electronic regulation.
