Deformable catalytic material with excellent flexible structure is a new type of catalyst that has been applied in various chemical reactions,especially electrocatalytic hydrogen evolution reaction(HER).In recent year...Deformable catalytic material with excellent flexible structure is a new type of catalyst that has been applied in various chemical reactions,especially electrocatalytic hydrogen evolution reaction(HER).In recent years,deformable catalysts for HER have made great progress and would become a research hotspot.The catalytic activities of deformable catalysts could be adjustable by the strain engineering and surface reconfiguration.The surface curvature of flexible catalytic materials is closely related to the electrocatalytic HER properties.Here,firstly,we systematically summarized self-adaptive catalytic performance of deformable catalysts and various micro–nanostructures evolution in catalytic HER process.Secondly,a series of strategies to design highly active catalysts based on the mechanical flexibility of lowdimensional nanomaterials were summarized.Last but not least,we presented the challenges and prospects of the study of flexible and deformable micro–nanostructures of electrocatalysts,which would further deepen the understanding of catalytic mechanisms of deformable HER catalyst.展开更多
One of the central tasks in the field of heterogeneous catalysis is to establish structure‐function relationships for these catalysts,especially for precious metals dispersed on the sub‐nanometer scale.Here,we repor...One of the central tasks in the field of heterogeneous catalysis is to establish structure‐function relationships for these catalysts,especially for precious metals dispersed on the sub‐nanometer scale.Here,we report the preparation of MgAl2O4‐supported Pt nanoparticles,amorphous aggregates and single atoms,and evaluate their ability to catalyze the hydrogenation of benzaldehyde.The Pt species were characterized by N2adsorption,X‐ray diffraction(XRD),aberration‐corrected transmission electron microscopy(ACTEM),CO chemisorption and in situ Fourier transform infrared spectroscopy of the chemisorbed CO,as well as by inductively coupled plasma atomic emission spectroscopy.They existed as isolated or neighboring single atoms on the MgAl2O4support,and formed amorphous Pt aggregates and then nanocrystallites with increased Pt loading.On the MgAl2O4support,single Pt atoms were highly active in the selective catalytic hydrogenation of benzaldehyde to benzyl alcohol.The terrace atoms of the Pt particles were more active but less selective;this was presumably due to their ability to form bridged carbonyl adsorbates.The MgAl2O4‐supported single‐atom Pt catalyst is a novel catalyst with a high precious atom efficiency and excellent catalytic hydrogenation ability and selectivity.展开更多
基金This work was financially supported by the National Natural Science Foundation of China(Nos.51902101 and 21875203)the Natural Science Foundation of Hunan Province(Nos.2021JJ40044 and 2023JJ50287)Natural Science Foundation of Jiangsu Province(No.BK20201381).
文摘Deformable catalytic material with excellent flexible structure is a new type of catalyst that has been applied in various chemical reactions,especially electrocatalytic hydrogen evolution reaction(HER).In recent years,deformable catalysts for HER have made great progress and would become a research hotspot.The catalytic activities of deformable catalysts could be adjustable by the strain engineering and surface reconfiguration.The surface curvature of flexible catalytic materials is closely related to the electrocatalytic HER properties.Here,firstly,we systematically summarized self-adaptive catalytic performance of deformable catalysts and various micro–nanostructures evolution in catalytic HER process.Secondly,a series of strategies to design highly active catalysts based on the mechanical flexibility of lowdimensional nanomaterials were summarized.Last but not least,we presented the challenges and prospects of the study of flexible and deformable micro–nanostructures of electrocatalysts,which would further deepen the understanding of catalytic mechanisms of deformable HER catalyst.
基金supported by the National Natural Science Foundation of China(21403213,21673226,21376236,U1462121)the"Hundred Talents Programme"of the Chinese Academy of Sciences+3 种基金the"Strategic Priority Research Program"of the Chinese Academy of Sciences(XDB17020100)National Key R&D Program of China(2016YFA0202801)Department of Science and Technology of Liaoning province under contract of 2015020086-101the Natural Science Foundation of Hunan Province(2016JJ2128)~~
文摘One of the central tasks in the field of heterogeneous catalysis is to establish structure‐function relationships for these catalysts,especially for precious metals dispersed on the sub‐nanometer scale.Here,we report the preparation of MgAl2O4‐supported Pt nanoparticles,amorphous aggregates and single atoms,and evaluate their ability to catalyze the hydrogenation of benzaldehyde.The Pt species were characterized by N2adsorption,X‐ray diffraction(XRD),aberration‐corrected transmission electron microscopy(ACTEM),CO chemisorption and in situ Fourier transform infrared spectroscopy of the chemisorbed CO,as well as by inductively coupled plasma atomic emission spectroscopy.They existed as isolated or neighboring single atoms on the MgAl2O4support,and formed amorphous Pt aggregates and then nanocrystallites with increased Pt loading.On the MgAl2O4support,single Pt atoms were highly active in the selective catalytic hydrogenation of benzaldehyde to benzyl alcohol.The terrace atoms of the Pt particles were more active but less selective;this was presumably due to their ability to form bridged carbonyl adsorbates.The MgAl2O4‐supported single‐atom Pt catalyst is a novel catalyst with a high precious atom efficiency and excellent catalytic hydrogenation ability and selectivity.
