Dynamic co-catalysis of Au single atoms and nanoporous Au for methane pyrolysis

Abstract 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.