Selective hydrogenation of CO_(2) to high value-added chemicals,not only gives an effective way to reduce the concentration of CO_(2),but also provides the precursors to advance the industrial manufacturing of chemica...Selective hydrogenation of CO_(2) to high value-added chemicals,not only gives an effective way to reduce the concentration of CO_(2),but also provides the precursors to advance the industrial manufacturing of chemicals and fuels.With the well-defined reticular frameworks and flexible modifiability,metal-organic frameworks(MOFs)can be the ideal platform to construct the enabled catalysts for CO_(2) hydrogenation,because they have shown the great potential for the enhancement of catalytic activity,the precise control of selectivity,and the excellent stability.In this review,we systematically summarize the recent advances in MOFs based catalysts for CO_(2) hydrogenation towards diverse products.Firstly,synthesis strategies for different kinds of MOFs based catalysts are described.Secondly,selective hydrogenation of CO_(2) towards CO and methane is discussed over various metal nanoparticles/MOFs composites.Thirdly,heterogenization and isolation of molecular catalysts by MOFs are elaborated for producing formic acid.Fourthly,selective hydrogenation of CO_(2) toward methanol is discussed in terms of interface structures of Cu,Zn,and metal nodes of MOFs,the synergy between auxiliary sites and noble metal,and tandem catalytic systems of molecular catalysts and Lewis acid sites.Subsequently,the integration of multiple metal sites,promoters,and cocatalysts into MOFs is described for the selective hydrogenation of CO_(2) to C2+products.After those,the key issue about the stability of MOFs based catalysts for CO_(2) hydrogenation reaction is discussed.Finally,the summary and perspective about MOFs based catalysts for selective CO_(2) hydrogenation and mechanism research are proposed.展开更多
Metal-organic framework nanosheets(MONs)as the emerging materials have been attracting great interest because the nanosheets possess a range of fascinating attributes including high surface areas and sufficient access...Metal-organic framework nanosheets(MONs)as the emerging materials have been attracting great interest because the nanosheets possess a range of fascinating attributes including high surface areas and sufficient accessible active sites,and their nanoscale thicknesses are favorable for mass diffusion and transfer of substrates and products with respect to bulk metal-organic frameworks(MOFs).This review first summarizes the synthetic methods of various MONs from top-down and bottom-up methods as well as their diverse composites with different components.Then,the catalytic applications of MON based nanocatalysts are discussed and the relationships among the composition,structure and catalytic performances are revealed.Finally,the challenges and future outlook about the synthesis of diverse MONs and their composites for heterogeneous catalysis are prospected.展开更多
基金financial support from the National Key Research and Development Program of China(No.2021YFA1500403)Strategic Priority Research Program of Chinese Academy of Sciences(No.XDB36000000)+2 种基金the National Natural Science Foundation of China(Nos.22173024,21722102,and 51672053)Beijing Natural Science Foundation(No.2182087)Youth Innovation Promotion Association CAS.
文摘Selective hydrogenation of CO_(2) to high value-added chemicals,not only gives an effective way to reduce the concentration of CO_(2),but also provides the precursors to advance the industrial manufacturing of chemicals and fuels.With the well-defined reticular frameworks and flexible modifiability,metal-organic frameworks(MOFs)can be the ideal platform to construct the enabled catalysts for CO_(2) hydrogenation,because they have shown the great potential for the enhancement of catalytic activity,the precise control of selectivity,and the excellent stability.In this review,we systematically summarize the recent advances in MOFs based catalysts for CO_(2) hydrogenation towards diverse products.Firstly,synthesis strategies for different kinds of MOFs based catalysts are described.Secondly,selective hydrogenation of CO_(2) towards CO and methane is discussed over various metal nanoparticles/MOFs composites.Thirdly,heterogenization and isolation of molecular catalysts by MOFs are elaborated for producing formic acid.Fourthly,selective hydrogenation of CO_(2) toward methanol is discussed in terms of interface structures of Cu,Zn,and metal nodes of MOFs,the synergy between auxiliary sites and noble metal,and tandem catalytic systems of molecular catalysts and Lewis acid sites.Subsequently,the integration of multiple metal sites,promoters,and cocatalysts into MOFs is described for the selective hydrogenation of CO_(2) to C2+products.After those,the key issue about the stability of MOFs based catalysts for CO_(2) hydrogenation reaction is discussed.Finally,the summary and perspective about MOFs based catalysts for selective CO_(2) hydrogenation and mechanism research are proposed.
基金financial support from the Strategic Priority Research Program of Chinese Academy of Sciences(No.XDB36000000)National Key Basic Research Program of China(No.2016YFA0200700,Z.Tang)+4 种基金National Natural Science Foundation of China(Nos.92056204,21890381 and 21721002,Z.Tang,Nos.21722102 and 51672053,G.Li)Beijing Natural Science Foundation(No.2182087,G.Li)Frontier Science Key Project of Chinese Academy of Sciences(No.QYZDJ-SSW-SLH038,Z.Tang)K.C.Wong Education Foundation(Z.Tang)Youth Innovation Promotion Association CAS(No.2016036,G.Li).
文摘Metal-organic framework nanosheets(MONs)as the emerging materials have been attracting great interest because the nanosheets possess a range of fascinating attributes including high surface areas and sufficient accessible active sites,and their nanoscale thicknesses are favorable for mass diffusion and transfer of substrates and products with respect to bulk metal-organic frameworks(MOFs).This review first summarizes the synthetic methods of various MONs from top-down and bottom-up methods as well as their diverse composites with different components.Then,the catalytic applications of MON based nanocatalysts are discussed and the relationships among the composition,structure and catalytic performances are revealed.Finally,the challenges and future outlook about the synthesis of diverse MONs and their composites for heterogeneous catalysis are prospected.