摘要：Alkali-water electrolyzers and hydroxide exchange membrane fuel cells are emerging as promising technologies to realize hydrogen *** cost-effective electrode materials with high activities towards corresponding hydrogen evolution(HER)and oxidation(HOR)reactions plays a crucial role in commercial hydrogen production and ***,we fabricated a V-doped Ni_(3)N/Ni heterostructure(V-Ni_(3)N/Ni)through a controlled nitridation treatment on a V-incorporated nickel hydroxide *** resultant catalyst exhibits comparable catalytic activity and durability to commercial Pt/C in terms of both HER(a low overpotential of 44 mV at the current density of 10 mA·cm^(-2))and HOR(a high current density of 1.54 mA·cm^(-2)at 0.1 V versus reversible hydrogen electrode)under alkaline *** superior activity of V-Ni_(3)N/Ni grown on different substrates further implies its intrinsic *** functional theory(DFT)calculations reveal that the coupled metallic Ni and doped V can promote the water adsorption,accelerate the Volmer step of alkaline HER,as well as optimize the adsorption and desorption of hydrogen intermediate(H^(*))to reach a balancedΔGH*value.

摘要：A series of Ru/FeOx catalysts were synthesized for the selective hydrogenation of CO2to *** characterizations of the catalysts through X‐ray diffraction,X‐ray photoelectron spectroscopy,transmission electron microscopy,and temperature‐programmed techniques were performed to directly monitor the surface chemical properties and the catalytic performance to elucidate the reaction *** dispersed Ru species were observed on the surface of FeOx regardless of the initial Ru *** the Ru loading resulted in changes to the Ru coverage over the FeOx surface,which had a significant impact on the interaction between Ru and adsorbed H,and concomitantly,the H2activation capacity via the ability for *** having0.01%of Ru loading exhibited100%selectivity toward CO resulting from the very strong interaction between Ru and adsorbed H,which limits the desorption of the activated H species and hinders over‐reduction of CO to *** increasing the Ru loading of the catalysts to above0.01%resulted in the adsorbed H to be easily dissociated,as a result of a weaker interaction with Ru,which allowed excessive CO reduction to produce *** how to selectively design the catalyst by tuning the initial loading of the active phase has broader implications on the design of supported metal catalysts toward preparing liquid fuels from CO2.?2018,Dalian Institute of Chemical Physics,Chinese Academy of Sciences toward preparing liquid fuels from CO2.?2018,Dalian Institute of Chemical Physics,Chinese Academy of *** by Elsevier *** rights reserved.

摘要：Evaluating the effect of metal surface density on catalytic performance is critical for designing high-activity metal-based *** this study,a series of ceria(CeCO_(2))-supported Ru catalysts(Ru/CeCO_(2))were prepared to analyze the effect of Ru surface density on the catalytic performance of Ru/CeCO_(2) for ammonia *** the Ru/CeCO_(2) catalysts with Ru surface densities lower than 0.68 Ru nm^(-2),the Ru layers were in close contact with CeCO_(2),and electrons were transferred directly from the CeCO_(2) defect sites to the Ru *** such cases,the adsorption of hydrogen species on the Ru sites in the vicinity of 0 atoms was high,leading to a high ammonia synthesis activity and strong hydrogen *** contrast,the preferential aggregation of Ru species into large particles on top of the Ru overlayer resulted in the coexistence of Ru clusters and particles,for catalysts with a Ru surface density higher than 1.4 Ru nm^(-2),for which Ru particles were isolated from the direct electronic influence of CeCO_(2).Consequently,the Ru-Ceth interactions were weak,and hydrogen poisoning can be significantly ***,electron transfer and hydrogen adsorption synergistically affected the synthesis of ammonia over Ru/CeCO_(2) catalysts,and catalyst samples with a Ru surface density lower than 0.31 Ru nm^(-2) or exactly 2.1 Ru nm^(-2) exhibited high catalytic activity for ammonia synthesis.