A composite metal-organic frameworks(MOFs)structure,designated as Co-hmta@La-salen,was synthesized through coordination interactions between a one-dimensional lanthanum MOFs(La-salen)with high density of uncoordinated...A composite metal-organic frameworks(MOFs)structure,designated as Co-hmta@La-salen,was synthesized through coordination interactions between a one-dimensional lanthanum MOFs(La-salen)with high density of uncoordinated imine(-CH=N-)groups and a cobalt-based MOFs(Co-hmta)structure prepared using hydrogen bonding stacking with hexamethylenetetramine(hmta)as the organic ligand.Subsequently,the Co-hmta@La-salen composite was chosen as a template for the pyrolysis process to synthesize a La(OH)_(3)supported metallic Co catalyst incorporating carbon-nitrogen(Co/La(OH)_(3)-CNhmta)catalyst.The catalytic results show that Co/La(OH)_(3)-CN-hmta(54%and 46%selectivity for aniline and N-phenylbenzylamine,respectively)displays superior cascade performance compared to classic Co/La(OH)_(3)-CN-nit catalyst(69%and 31%selectivity for aniline and N-phenylbenzylamine,respectively).Moreover,the kinetic test results indicate that N-alkylation is the rate-limiting step of the overall cascade reaction.The Co/La(OH)_(3)-CN-hmta catalyst can be separated from the reaction system using a magnet,and it also exhibits good cyclic stability.All of these suggest that the“MOFs plus MOFs via coordination”templating method can be employed as an efficient strategy for the preparation of supported catalysts.展开更多
Photocatalysis is widely regarded as a highly promising sustainable technique for addressing the challenges posed by environmental pollution and energy provision.In recent years,metal-loaded MOFs has become a rising s...Photocatalysis is widely regarded as a highly promising sustainable technique for addressing the challenges posed by environmental pollution and energy provision.In recent years,metal-loaded MOFs has become a rising star within the domain of photocatalysis due to its high specific surface area and porosity,adjustable structure,diverse and abundant catalytic components,which has exhibited excellent photocatalytic activity and exhibit great potential in a range of disciplines.In this paper,the principles for evaluating the photocatalytic performance of MOFs-based materials were firstly introduced,and some typical examples were also listed accordingly.Along with this,particular emphasis is paid to the main factors affecting the photocatalytic performance of metal-loaded MOFs.Then the synthesis and design strategies of MOFs loaded metal entities of varying sizes(single atoms,nanoclusters,and nanoparticles),and their applications in photocatalytic CO_(2)reduction,hydrogen production,photooxidation and photocatalytic hydrogenation were summarized and discussed.Finally,the opportunities and challenges faced in this kind of MOFs-based composites were analyzed from different perspectives.This report is expected to help researchers design and develop high-performance MOFs-based photocatalytic materials.展开更多
基金Project supported by the Natural Science Foundation of Jiangsu Province (BK20210066)Natural Science Foundation of Heilongjiang Province (ZD2022E007).
文摘A composite metal-organic frameworks(MOFs)structure,designated as Co-hmta@La-salen,was synthesized through coordination interactions between a one-dimensional lanthanum MOFs(La-salen)with high density of uncoordinated imine(-CH=N-)groups and a cobalt-based MOFs(Co-hmta)structure prepared using hydrogen bonding stacking with hexamethylenetetramine(hmta)as the organic ligand.Subsequently,the Co-hmta@La-salen composite was chosen as a template for the pyrolysis process to synthesize a La(OH)_(3)supported metallic Co catalyst incorporating carbon-nitrogen(Co/La(OH)_(3)-CNhmta)catalyst.The catalytic results show that Co/La(OH)_(3)-CN-hmta(54%and 46%selectivity for aniline and N-phenylbenzylamine,respectively)displays superior cascade performance compared to classic Co/La(OH)_(3)-CN-nit catalyst(69%and 31%selectivity for aniline and N-phenylbenzylamine,respectively).Moreover,the kinetic test results indicate that N-alkylation is the rate-limiting step of the overall cascade reaction.The Co/La(OH)_(3)-CN-hmta catalyst can be separated from the reaction system using a magnet,and it also exhibits good cyclic stability.All of these suggest that the“MOFs plus MOFs via coordination”templating method can be employed as an efficient strategy for the preparation of supported catalysts.
基金supported by the Beijing Natural Science Foundation(No.L233011)Guangdong Province Natural Science Foundation(No.2022A1515011918)USTB Research Center for International People-to-People Exchange in Science.Technology and Civilization(No.2023KFYB003)。
文摘Photocatalysis is widely regarded as a highly promising sustainable technique for addressing the challenges posed by environmental pollution and energy provision.In recent years,metal-loaded MOFs has become a rising star within the domain of photocatalysis due to its high specific surface area and porosity,adjustable structure,diverse and abundant catalytic components,which has exhibited excellent photocatalytic activity and exhibit great potential in a range of disciplines.In this paper,the principles for evaluating the photocatalytic performance of MOFs-based materials were firstly introduced,and some typical examples were also listed accordingly.Along with this,particular emphasis is paid to the main factors affecting the photocatalytic performance of metal-loaded MOFs.Then the synthesis and design strategies of MOFs loaded metal entities of varying sizes(single atoms,nanoclusters,and nanoparticles),and their applications in photocatalytic CO_(2)reduction,hydrogen production,photooxidation and photocatalytic hydrogenation were summarized and discussed.Finally,the opportunities and challenges faced in this kind of MOFs-based composites were analyzed from different perspectives.This report is expected to help researchers design and develop high-performance MOFs-based photocatalytic materials.
