Molybdenum disulfide(MoS_(2))has shown significant promise as an economic hydrogen evolution reaction(HER)catalyst for hydrogen generation,but its catalytic performance is still lower than noble metalbased catalysists...Molybdenum disulfide(MoS_(2))has shown significant promise as an economic hydrogen evolution reaction(HER)catalyst for hydrogen generation,but its catalytic performance is still lower than noble metalbased catalysists.Herein,a silver nanoparticles(Ag NPs)-decorated 1T/2H phase layered MoS_(2) electrocatalyst grown on titanium dioxide nanorod arrays(Ag NPs/1T(2H)MoS_(2)/TNRs)was prepared through acid-tunable ammonium ion intercalation.Taking advantage of MoS_(2) layered structure and crystal phase controllability,as-prepared Ag NPs/1T(2H)MoS_(2)/TNRs exhibited ultrahigh HER activity.As-proposed strategy combines facile hydrogen desorption(Ag NPs)with efficient hydrogen adsorption(1T/2H MoS_(2))effectively circumventes the kinetic limitation of hydrogen desorption by 1T/2H MoS_(2).The as-prepared Ag NPs/1T(2H)MoS_(2)/TNRs electrocatalyst exhibited excellent HER activity in 0.5 mol/L H2SO4 with low overpotential(118 mV vs.reversible hydrogen electrode(RHE))and small Tafel slope(38.61 mV/dec).The overpotential exhibts no obvious attenuation after 10 h of constant current flow.First-principles calculation demonstrates that as-prepared 1T/2H MoS_(2) exhibit a large capacity to store protons.These protons can be subsequently transferred to Ag NPs,which significantly increases the hydrogen coverage on the surface of Ag NPs in HER process and thus change the rate-determining step of HER on Ag NPs from water dissociation to hydrogen recombination.This study provides a unique strategy to improve the catalytic activity and stability for MoS_(2)-based electrocatalyst.展开更多
基金supported by the National Natural Science Foundation of China(No.52270078)the Royal Society IEC\NSFC\211201-International Exchanges 2021 Cost Share(NSFC).
文摘Molybdenum disulfide(MoS_(2))has shown significant promise as an economic hydrogen evolution reaction(HER)catalyst for hydrogen generation,but its catalytic performance is still lower than noble metalbased catalysists.Herein,a silver nanoparticles(Ag NPs)-decorated 1T/2H phase layered MoS_(2) electrocatalyst grown on titanium dioxide nanorod arrays(Ag NPs/1T(2H)MoS_(2)/TNRs)was prepared through acid-tunable ammonium ion intercalation.Taking advantage of MoS_(2) layered structure and crystal phase controllability,as-prepared Ag NPs/1T(2H)MoS_(2)/TNRs exhibited ultrahigh HER activity.As-proposed strategy combines facile hydrogen desorption(Ag NPs)with efficient hydrogen adsorption(1T/2H MoS_(2))effectively circumventes the kinetic limitation of hydrogen desorption by 1T/2H MoS_(2).The as-prepared Ag NPs/1T(2H)MoS_(2)/TNRs electrocatalyst exhibited excellent HER activity in 0.5 mol/L H2SO4 with low overpotential(118 mV vs.reversible hydrogen electrode(RHE))and small Tafel slope(38.61 mV/dec).The overpotential exhibts no obvious attenuation after 10 h of constant current flow.First-principles calculation demonstrates that as-prepared 1T/2H MoS_(2) exhibit a large capacity to store protons.These protons can be subsequently transferred to Ag NPs,which significantly increases the hydrogen coverage on the surface of Ag NPs in HER process and thus change the rate-determining step of HER on Ag NPs from water dissociation to hydrogen recombination.This study provides a unique strategy to improve the catalytic activity and stability for MoS_(2)-based electrocatalyst.
