Abstract
The control of single metal atomic sites has been extensively studied in the field of single atom catalysts. By contrast, the precise control of the mesoporous structure in the matrix material, which directly correlates with mass diffusions and may play a dominant role in delivering industrially relevant reaction rates, has been overlooked. Here we report a general method for the synthesis of a single atom catalyst with control of the atomic structure of the single atomic site as well as the mesoporous structure of the carbon support for optimized catalytic performance. Various combinations of metal centres (Ni, Co, Mn, Zn, Cu, Sc and Fe) and mass diffusion channels in two dimensions and three dimensions were achieved. Using CO2 reduction to CO as an example, our Ni single atom catalyst with three-dimensional diffusion channels delivered a practical current of 350 mA cm−2 while maintaining a 93% CO Faradaic efficiency, representing a sixfold improvement in turnover frequency compared to two-dimensional counterparts. [Figure not available: see fulltext.]
| Original language | English |
|---|---|
| Pages (from-to) | 658-667 |
| Number of pages | 10 |
| Journal | Nature Synthesis |
| Volume | 1 |
| Issue number | 8 |
| DOIs | |
| State | Published - Aug 2022 |
Funding
This work was supported by the Welch Foundation Research Grant (C-2051-20200401, H.W.), the Roy E. Campbell Faculty Development Award and Rice University. Aberration-corrected STEM-EELS and electron tomography research conducted as part of a user project at the Center for Nanophase Materials Sciences (CNMS), which is a US Department of Energy, Office of Science User Facility at Oak Ridge National Laboratory. The XAS data were collected at SXRMB of the Canadian Light Source, a national research facility of the University of Saskatchewan, which is supported by the Canada Foundation for Innovation (CFI), the Natural Sciences and Engineering Research Council (NSERC), the National Research Council (NRC), Canadian Institutes of Health Research (CIHR), Government of Saskatchewan and the University of Saskatchewan. This work was supported by the Welch Foundation Research Grant (C-2051-20200401, H.W.), the Roy E. Campbell Faculty Development Award and Rice University. Aberration-corrected STEM-EELS and electron tomography research conducted as part of a user project at the Center for Nanophase Materials Sciences (CNMS), which is a US Department of Energy, Office of Science User Facility at Oak Ridge National Laboratory. The XAS data were collected at SXRMB of the Canadian Light Source, a national research facility of the University of Saskatchewan, which is supported by the Canada Foundation for Innovation (CFI), the Natural Sciences and Engineering Research Council (NSERC), the National Research Council (NRC), Canadian Institutes of Health Research (CIHR), Government of Saskatchewan and the University of Saskatchewan.
