Piezocatalysis and pyrocatalysis can achieve catalytic action with the application of external mechanical energy and varying temperatures.These catalytic processes have been widely applied in various fields,providing ...Piezocatalysis and pyrocatalysis can achieve catalytic action with the application of external mechanical energy and varying temperatures.These catalytic processes have been widely applied in various fields,providing innovative solutions to issues such as water pollution,energy shortages,and global warming.Despite the continuous breakthroughs in the catalytic performance of piezocatalysts and pyrocatalysts,powder-based catalysts face significant limitations due to their inability to be retrieved and the risk of secondary pollution,severely restricting their application.Methods such as compression molding,3 D printing,and the preparation of ceramic-polymer bulk composites can effectively address the issue of catalyst retrievability.However,bulk catalysts,which lose a significant amount of surface area,still need their catalytic performance further enhanced.Therefore,achieving piezocatalysts and pyrocatalysts with excellent catalytic performance and retrievability is of increasing importance.展开更多
Regulating the selectivity of catalysts in selective hydrogenation reactions at the atomic level is highly desirable but remains a grand challenge. Here we report a simple and practical strategy to synthesize a monoli...Regulating the selectivity of catalysts in selective hydrogenation reactions at the atomic level is highly desirable but remains a grand challenge. Here we report a simple and practical strategy to synthesize a monolithic single-atom catalyst(SAC) with isolated Pd atoms supported on bulk nitrogen-doped carbon foams(Pd-SAs/CNF). Moreover, we demonstrate that the single-atom Pd sites with unique electronic structure endow Pd-SAs/CNF with an isolated site effect, leading to excellent activity and selectivity in 4-nitrophenylacetylene semi-hydrogenation reaction. In addition, benefiting from the great integrity and excellent mechanical strength, monolithic Pd-SAs/CNF catalyst is easy to separate from the reaction system for conducting the subsequent recycling. The cyclic test demonstrates the excellent reusability and stability of monolithic Pd-SAs/CNF catalyst.The discovery of isolated site effect provides a new approach to design highly selective catalysts. And the development of monolithic SACs provides new opportunities to advance the practical applications of single-atom catalysts.展开更多
基金Project(2022YFB3807404)supported by the National Key Research and Development Program of ChinaProject(52302158)supported by the National Natural Science Foundation of China。
文摘Piezocatalysis and pyrocatalysis can achieve catalytic action with the application of external mechanical energy and varying temperatures.These catalytic processes have been widely applied in various fields,providing innovative solutions to issues such as water pollution,energy shortages,and global warming.Despite the continuous breakthroughs in the catalytic performance of piezocatalysts and pyrocatalysts,powder-based catalysts face significant limitations due to their inability to be retrieved and the risk of secondary pollution,severely restricting their application.Methods such as compression molding,3 D printing,and the preparation of ceramic-polymer bulk composites can effectively address the issue of catalyst retrievability.However,bulk catalysts,which lose a significant amount of surface area,still need their catalytic performance further enhanced.Therefore,achieving piezocatalysts and pyrocatalysts with excellent catalytic performance and retrievability is of increasing importance.
基金supported by the National Key R&D Program of China (2018YFA0702003)the National Natural Science Foundation of China (21890383,21671117,21871159 and 21901135)+1 种基金the National Postdoctoral Program for Innovative Talents (BX20180160)the China Postdoctoral Science Foundation (2018M640113)。
文摘Regulating the selectivity of catalysts in selective hydrogenation reactions at the atomic level is highly desirable but remains a grand challenge. Here we report a simple and practical strategy to synthesize a monolithic single-atom catalyst(SAC) with isolated Pd atoms supported on bulk nitrogen-doped carbon foams(Pd-SAs/CNF). Moreover, we demonstrate that the single-atom Pd sites with unique electronic structure endow Pd-SAs/CNF with an isolated site effect, leading to excellent activity and selectivity in 4-nitrophenylacetylene semi-hydrogenation reaction. In addition, benefiting from the great integrity and excellent mechanical strength, monolithic Pd-SAs/CNF catalyst is easy to separate from the reaction system for conducting the subsequent recycling. The cyclic test demonstrates the excellent reusability and stability of monolithic Pd-SAs/CNF catalyst.The discovery of isolated site effect provides a new approach to design highly selective catalysts. And the development of monolithic SACs provides new opportunities to advance the practical applications of single-atom catalysts.
