Supported atomically dispersed metal catalysts(ADMCs)have received enormous attention due to their high atom utilization efficiency,mass activity and excellent selectivity.Single-atom site catalysts(SACs)with monometa...Supported atomically dispersed metal catalysts(ADMCs)have received enormous attention due to their high atom utilization efficiency,mass activity and excellent selectivity.Single-atom site catalysts(SACs)with monometal-center as the quintessential ADMCs have been extensively studied in the catalysis-related fields.Beyond SACs,novel atomically dispersed metal catalysts(NADMCs)with flexible active sites featuring two or more catalytically centers including dual-atom and triple-atom catalysts have drawn ever-increasing attention recently.Owing to the presence of multiple neighboring active sites,NADMCs could exhibit much higher activity and selectivity compared with SACs,especially in those complicated reactions with multi-step intermediates.This review comprehensively outlines the recent exciting advances on the NADMCs with emphasis on the deeper understanding of the synergistic interactions among multiple metal atoms and underlying structure-performance relationships.It starts with the systematical introduction of principal synthetic approaches for NADMCs highlighting the key issues of each fabrication method including the atomically precise control in the design of metal nuclearity,and then the state-of-the-art characterizations for identifying and monitoring the atomic structure of NADMCs are explored.Thereafter,the recent development of NADMCs in energy-related applications is systematically discussed.Finally,we provide some new insights into the remaining challenges and opportunities for the development of NADMCs.展开更多
Methane partial oxidation to methanol （MPOM） using dielectric barrier discharge over a Fe2O3-CuO/γ-Al2O3 catalyst was performed.The multicomponent catalyst was combined with plasma in two different configurations,i...Methane partial oxidation to methanol （MPOM） using dielectric barrier discharge over a Fe2O3-CuO/γ-Al2O3 catalyst was performed.The multicomponent catalyst was combined with plasma in two different configurations,i.e.,in-plasma catalysis （IPC） and post-plasma catalysis （PPC）.It was found that the catalytic performance of the catalysts for MPOM was strongly dependent on the hybrid configuration.A better synergistic performance of plasma and catalysis was achieved in the IPC configuration,but the catalysts packed in the discharge zone showed lower stability than those connected to the discharge zone in sequence.Active species,such as ozone,atomic oxygen and methyl radicals,were produced from the plasma-catalysis process,and made a major contribution to methanol synthesis.These active species were identified by the means of in situ optical emission spectra,ozone measurement and FT-IR spectra.It was confirmed that the amount of active species in the IPC system was greater than that in the PPC system.The results of TG,XRD,and N2 adsorption-desorption revealed that carbon deposition on the spent catalyst surface was responsible for the catalyst deactivation in the IPC configuration.展开更多
基金the Beijing Natural Science Foundation(No.2224096)the National Key R&D Program of China(No.2018YFA0702003)+3 种基金the Science and Technology Key Project of Guangdong Province,China(No.2020B010188002)the China Postdoctoral Science Foundation(Nos.2021M690086 and 2021TQ0170)X.B.Z.acknowledges funding support from the Office of China Postdoctoral Council(No.YJ20200277)the“Shuimu Tsinghua Scholar Program"(No.2020SM109)of Tsinghua University,China.
文摘Supported atomically dispersed metal catalysts(ADMCs)have received enormous attention due to their high atom utilization efficiency,mass activity and excellent selectivity.Single-atom site catalysts(SACs)with monometal-center as the quintessential ADMCs have been extensively studied in the catalysis-related fields.Beyond SACs,novel atomically dispersed metal catalysts(NADMCs)with flexible active sites featuring two or more catalytically centers including dual-atom and triple-atom catalysts have drawn ever-increasing attention recently.Owing to the presence of multiple neighboring active sites,NADMCs could exhibit much higher activity and selectivity compared with SACs,especially in those complicated reactions with multi-step intermediates.This review comprehensively outlines the recent exciting advances on the NADMCs with emphasis on the deeper understanding of the synergistic interactions among multiple metal atoms and underlying structure-performance relationships.It starts with the systematical introduction of principal synthetic approaches for NADMCs highlighting the key issues of each fabrication method including the atomically precise control in the design of metal nuclearity,and then the state-of-the-art characterizations for identifying and monitoring the atomic structure of NADMCs are explored.Thereafter,the recent development of NADMCs in energy-related applications is systematically discussed.Finally,we provide some new insights into the remaining challenges and opportunities for the development of NADMCs.
基金supported by the National Natural Science Foundation of China(No. 20836008 and U0633003)the Zhejiang Provincial Natural Science Foundation of China(No. Y5080192)+3 种基金the Project of Science and Technology Department of Zhejiang Province of China(2007C13061)MOST Project of China(No. 2007AA06Z339,No. 2008BAC32B06 and No. 2007AA06A409)the Open Project Program of Key Laboratory of Non-point Sources Pollution Controlthe Ministry of Agriculture of the People’s Republic of China and Science Foundation of Chinese University
文摘Methane partial oxidation to methanol （MPOM） using dielectric barrier discharge over a Fe2O3-CuO/γ-Al2O3 catalyst was performed.The multicomponent catalyst was combined with plasma in two different configurations,i.e.,in-plasma catalysis （IPC） and post-plasma catalysis （PPC）.It was found that the catalytic performance of the catalysts for MPOM was strongly dependent on the hybrid configuration.A better synergistic performance of plasma and catalysis was achieved in the IPC configuration,but the catalysts packed in the discharge zone showed lower stability than those connected to the discharge zone in sequence.Active species,such as ozone,atomic oxygen and methyl radicals,were produced from the plasma-catalysis process,and made a major contribution to methanol synthesis.These active species were identified by the means of in situ optical emission spectra,ozone measurement and FT-IR spectra.It was confirmed that the amount of active species in the IPC system was greater than that in the PPC system.The results of TG,XRD,and N2 adsorption-desorption revealed that carbon deposition on the spent catalyst surface was responsible for the catalyst deactivation in the IPC configuration.
