Single-atom catalysts(SACs)are gaining increasing recognition because of their superior catalytic properties for various reactions.However,the performance of SACs is often limited by the lack of neighboring metal cent...Single-atom catalysts(SACs)are gaining increasing recognition because of their superior catalytic properties for various reactions.However,the performance of SACs is often limited by the lack of neighboring metal centers to cooperate in catalysis.Herein,a synergetic interaction between neighboring Cu atoms of a few-atom catalyst(FAC)on graphdiyne(GDY)is found to greatly enhance the production of acetate in the CO electroreduction reaction relative to Cu SACs.In a 1.0 M KOH electrolyte,this Cu FAC exhibits an acetate Faradaic efficiency of 53.8±1.5%,an ultrahigh relative purity of up to 97 wt%for liquid products,and excellent stability over 23 h continuous electrolysis at–0.8 V versus reversible hydrogen electrode.Theoretical studies suggest that the intersite catalytic communication between two neighboring metal atoms confined in each pore of GDY facilitates the formation of acetic acid through either stepwise hydrogenation of CH_(2)CO^(*)or the direct reaction of H_(2)Owith CH_(2)CO^(*).Our study demonstrates the unprecedented synergetic catalysis of Cu FAC in promoting the selective CO electroreduction toward acetate production.展开更多
The development of highly efficient Pt-based alloy nanocatalysts is important but remains challenging for fuel cells commercialization.Here,a new class of zigzag-like platinum-zinc (Pt-Zn) alloy nanowires (NWs) with r...The development of highly efficient Pt-based alloy nanocatalysts is important but remains challenging for fuel cells commercialization.Here,a new class of zigzag-like platinum-zinc (Pt-Zn) alloy nanowires (NWs) with rough surface and controllable composition is reported.The merits of anisotropic one-dimensional nanostructure,stable high-index facets and coordinatively unsaturated Pt sites endow the composition-optimal Pt94Zn6 NWs with a mass activity of 7.2 and 6.2 times higher than that of commercial Pt black catalysts toward methanol/ethanol oxidation,respectively.Alloying-induced d-band electron modulation and lattice strain effects weaken the adsorption strength of poisoning species,which originally enhances the catalytic activity of Pt-Zn NWs.This study provides a new perspective of Pt-Zn electrocatalysts with intrinsic mechanism for enhanced catalytic performance.展开更多
The article Highly active zigzag-like Pt-Zn alloy nanowires with high-index facets for alcohol electrooxidation, written by Xiaoqiang Cui and Weitao Zheng, was erroneously originally published electronically on the pu...The article Highly active zigzag-like Pt-Zn alloy nanowires with high-index facets for alcohol electrooxidation, written by Xiaoqiang Cui and Weitao Zheng, was erroneously originally published electronically on the publisher’s internet portal (currently SpringerLink) on 6 April 2019 with incomplete Electronic Supplementary Material (ESM), which should contain 16 figures and 3 tables. You will find the complete supplementary material file online linked to this publisher’s erratum.展开更多
基金supported by the National Natural Science Foundation of China(grant nos.21771098,21903016,and 21901110)Shenzhen R&D Fund(grant no.KQTD20180411143418361)+2 种基金Stable Support Plan Program of Shenzhen Natural Science Fund(grant no.20200925152742003)and Educational Commission of Guangdong Province(grant no.2020KTSCX121)S.T.and E.H.are supported by the Assistant Secretary for Energy Efficiency and Renewable Energy,Vehicle Technology Office of the US Department of Energy(DOE)through the Advanced Battery Materials Research(BMR)Program under contract no.DE-SC0012704.
文摘Single-atom catalysts(SACs)are gaining increasing recognition because of their superior catalytic properties for various reactions.However,the performance of SACs is often limited by the lack of neighboring metal centers to cooperate in catalysis.Herein,a synergetic interaction between neighboring Cu atoms of a few-atom catalyst(FAC)on graphdiyne(GDY)is found to greatly enhance the production of acetate in the CO electroreduction reaction relative to Cu SACs.In a 1.0 M KOH electrolyte,this Cu FAC exhibits an acetate Faradaic efficiency of 53.8±1.5%,an ultrahigh relative purity of up to 97 wt%for liquid products,and excellent stability over 23 h continuous electrolysis at–0.8 V versus reversible hydrogen electrode.Theoretical studies suggest that the intersite catalytic communication between two neighboring metal atoms confined in each pore of GDY facilitates the formation of acetic acid through either stepwise hydrogenation of CH_(2)CO^(*)or the direct reaction of H_(2)Owith CH_(2)CO^(*).Our study demonstrates the unprecedented synergetic catalysis of Cu FAC in promoting the selective CO electroreduction toward acetate production.
基金the National Key Research and Development Program of China (No.2016YFA0200400)the National Natural Science Foundation of China (Nos.51571100,51602305, 51522212,51421002,and 51672307)+1 种基金Program for JLU Science and Technology Innovative Research Team (JLUSTIRT,2017TD-09)the Fundamental Research Funds for the Central Universities and the Graduate Innovation Fund of Jilin University.
文摘The development of highly efficient Pt-based alloy nanocatalysts is important but remains challenging for fuel cells commercialization.Here,a new class of zigzag-like platinum-zinc (Pt-Zn) alloy nanowires (NWs) with rough surface and controllable composition is reported.The merits of anisotropic one-dimensional nanostructure,stable high-index facets and coordinatively unsaturated Pt sites endow the composition-optimal Pt94Zn6 NWs with a mass activity of 7.2 and 6.2 times higher than that of commercial Pt black catalysts toward methanol/ethanol oxidation,respectively.Alloying-induced d-band electron modulation and lattice strain effects weaken the adsorption strength of poisoning species,which originally enhances the catalytic activity of Pt-Zn NWs.This study provides a new perspective of Pt-Zn electrocatalysts with intrinsic mechanism for enhanced catalytic performance.
文摘The article Highly active zigzag-like Pt-Zn alloy nanowires with high-index facets for alcohol electrooxidation, written by Xiaoqiang Cui and Weitao Zheng, was erroneously originally published electronically on the publisher’s internet portal (currently SpringerLink) on 6 April 2019 with incomplete Electronic Supplementary Material (ESM), which should contain 16 figures and 3 tables. You will find the complete supplementary material file online linked to this publisher’s erratum.
