期刊
NATURE COMMUNICATIONS
卷 11, 期 1, 页码 -出版社
NATURE PUBLISHING GROUP
DOI: 10.1038/s41467-020-15806-8
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资金
- National Key RAMP
- D Program of China [2017YFA0700104]
- National Science Fund for Distinguished Young Scholars [51825102]
- National Natural Science Foundation of China [51671145, 21506148, 51761165012, 51971157]
- Tianjin Science Fund for Distinguished Young Scholars [19JCJQJC61800]
- National Program for Thousand Young Talents of China
Nanocatalysts and single-atom catalysts are both vital for heterogeneous catalysis. They are recognized as two different categories of catalysts. Nevertheless, recent theoretical works have indicated that Au nanoparticles/clusters release Au single atoms in CO oxidation, and they co-catalyze the oxidation. However, to date, neither experimental evidence for the co-catalysis nor direct observations on any heterogeneous catalysis process of single-atom catalysts are reported. Here, the dynamic process of nanoporous Au to catalyze methane pyrolysis is monitored by in situ transmission electron microscopy with high spatial-temporal resolutions. It demonstrates that nanoporous Au surfaces partially disintegrate, releasing Au single atoms. As demonstrated by DFT calculation, the single atoms could co-catalyze the reaction with nanoporous Au. Moreover, the single atoms dynamically aggregate into nanoparticles, which re-disintegrate back to single atoms. This work manifests that under certain conditions, the heterogeneous catalysis processes of nanocatalysts and single-atom catalysts are not independent, where their dynamic co-catalysis exists. Nanocatalysts and single-atom catalysts are generally considered as two categories with distinct performances. Here, in situ TEM study of catalytic methane pyrolysis over nanoporous Au reveals a highly dynamic process where co-catalysis exists among various catalyst forms.
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