Single-atom catalysts(SACs)have attracted extensive attention in the field of heterogeneous catalysis.However,the fabrication of SACs with high loading and hightemperature stability remains a grand challenge,especiall...Single-atom catalysts(SACs)have attracted extensive attention in the field of heterogeneous catalysis.However,the fabrication of SACs with high loading and hightemperature stability remains a grand challenge,especially on oxide supports.In this work,we have demonstrated that through strong covalent metal-support interaction,highloading and thermally stable single-atom Pt catalysts can be readily prepared by using Fe modified spinel as support.Better catalytic performance in N2O decomposition reaction is obtained on such SACs than their nanocatalyst counterpart and low-surface-area Fe2O3 supported Pt SACs.This work provides a strategy for the fabrication of high-loading and thermally stable SACs for applications at high temperatures.展开更多
Heterogenization of the homogeneous catalysis has been studied for almost 50 years.Single-atom catalysis has the advantages of both homo-and heterogeneous catalysis.It has been proposed,and subsequently experimentally...Heterogenization of the homogeneous catalysis has been studied for almost 50 years.Single-atom catalysis has the advantages of both homo-and heterogeneous catalysis.It has been proposed,and subsequently experimentally verified that single-atom catalysis is able to bridge homo-and heterogeneous catalysis,thus providing a new avenue to realize the heterogenization of homogeneous catalysis.Alkoxycarbonylation of aryl halides is an effective method for the direct synthesis of carboxylic acid derivatives,and is commonly catalyzed by Pd-based homogeneous complexes with N/P-containing ligands and organic/inorganic base.Herein,we firstly reported that Pd1/CeO2 single-atom catalyst showed good performance in the alkoxycarbonylation of aryl iodides reaction.Under base-free and ligand-free conditions,Pd1/CeO2 single-atom catalyst can transfer different aryl iodides to corresponding products.The catalyst can be easily recovered and reused four times without significant loss of reactivity.展开更多
基金supported by the National Key Projects for Fundamental Research and Development of China(2016YFA0202801)the National Natural Science Foundation of China(21673226+3 种基金91645203 and 21590792)the “Transformational Technologies for Clean Energy and Demonstration”the Strategic Priority Research Program of the Chinese Academy of Sciences (XDA21040200 and XDB17000000)supported by the Tsinghua Xuetang Talents Program
文摘Single-atom catalysts(SACs)have attracted extensive attention in the field of heterogeneous catalysis.However,the fabrication of SACs with high loading and hightemperature stability remains a grand challenge,especially on oxide supports.In this work,we have demonstrated that through strong covalent metal-support interaction,highloading and thermally stable single-atom Pt catalysts can be readily prepared by using Fe modified spinel as support.Better catalytic performance in N2O decomposition reaction is obtained on such SACs than their nanocatalyst counterpart and low-surface-area Fe2O3 supported Pt SACs.This work provides a strategy for the fabrication of high-loading and thermally stable SACs for applications at high temperatures.
基金financially supported by the National Natural Science Foundation of China (21776270)the Strategic Priority Research Program of the Chinese Academy of Sciences(XDB17020100)+3 种基金China Postdoctoral Science Foundation(2017M621170)DICP Outstanding Postdoctoral Foundation(2017YB02)Liaoning Revitalization Talents Programdedicated funds for methanol conversion from DICP
文摘Heterogenization of the homogeneous catalysis has been studied for almost 50 years.Single-atom catalysis has the advantages of both homo-and heterogeneous catalysis.It has been proposed,and subsequently experimentally verified that single-atom catalysis is able to bridge homo-and heterogeneous catalysis,thus providing a new avenue to realize the heterogenization of homogeneous catalysis.Alkoxycarbonylation of aryl halides is an effective method for the direct synthesis of carboxylic acid derivatives,and is commonly catalyzed by Pd-based homogeneous complexes with N/P-containing ligands and organic/inorganic base.Herein,we firstly reported that Pd1/CeO2 single-atom catalyst showed good performance in the alkoxycarbonylation of aryl iodides reaction.Under base-free and ligand-free conditions,Pd1/CeO2 single-atom catalyst can transfer different aryl iodides to corresponding products.The catalyst can be easily recovered and reused four times without significant loss of reactivity.
