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Abstract
The sintering of supported metal nanoparticles is a major route to the deactivation of industrial heterogeneous catalysts, which largely increase the cost and decrease the productivity. Here, we discover that supported palladium/gold/platinum nanoparticles distributed at the interface of oxide supports and nitrogen-doped carbon shells would undergo an unexpected nitrogen-doped carbon atomization process against the sintering at high temperatures, during which the nanoparticles can be transformed into more active atomic species. The in situ transmission electron microscopy images reveal the abundant nitrogen defects in carbon shells provide atomic diffusion sites for the mobile atomistic palladium species detached from the palladium nanoparticles. More important, the catalytic activity of sintered and deactivated palladium catalyst can be recovered by this unique N-doped carbon atomization process. Our findings open up a window to preparation of sintering-resistant single atoms catalysts and regeneration of deactivated industrial catalysts.
Sintering supported metal nanoparticles is the common route to the deactivation of industrial heterogeneous catalysts. Here, the authors report a carbon atomization process that allows one not only to redisperse metal nanoparticles, but also to recover deactivated catalysts.
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1 University of Science and Technology of China, Hefei National Laboratory for Physical Sciences at the Microscale, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), School of Chemistry and Materials Science, and National Synchrotron Radiation Laboratory, Hefei, China (GRID:grid.59053.3a) (ISNI:0000000121679639)
2 Tianjin University of Technology, Center for Electron Microscopy and Tianjin Key Lab of Advanced Functional Porous Materials, Institute for New Energy Materials & Low-Carbon Technologies, School of Materials Science and Engineering, Tianjin, China (GRID:grid.265025.6)
3 Nanjing University of Science and Technology, Nano and Heterogeneous Materials Center, School of Materials Science and Engineering, Nanjing, China (GRID:grid.410579.e) (ISNI:0000 0000 9116 9901)
4 Shanghai University, NEST Lab, Department of Chemistry, College of Science, Shanghai, China (GRID:grid.39436.3b) (ISNI:0000 0001 2323 5732)
5 Tsinghua University, Department of Chemistry, Beijing, China (GRID:grid.12527.33) (ISNI:0000 0001 0662 3178)
6 University of Science and Technology of China, National Synchrotron Radiation Laboratory, Hefei, China (GRID:grid.59053.3a) (ISNI:0000000121679639)
7 University of Science and Technology of China, Hefei National Laboratory for Physical Sciences at the Microscale, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), School of Chemistry and Materials Science, and National Synchrotron Radiation Laboratory, Hefei, China (GRID:grid.59053.3a) (ISNI:0000000121679639); Nanjing University of Science and Technology, Nano and Heterogeneous Materials Center, School of Materials Science and Engineering, Nanjing, China (GRID:grid.410579.e) (ISNI:0000 0000 9116 9901)