A general synthesis of single atom catalysts with controllable atomic and mesoporous structures

Wu, Zhen-Yu; Zhu, Peng; Cullen, David A.; Hu, Yongfeng; Yan, Qiang-Qiang; Shen, Shan-Cheng; Chen, Feng-Yang; Yu, Haoran; Shakouri, Mohsen; Arregui-Mena, Jose D.; Ziabari, Amirkoushyar; Paterson, Alisa R.; Liang, Hai-Wei; Wang, Haotian

doi:10.1038/s44160-022-00129-x

A general synthesis of single atom catalysts with controllable atomic and mesoporous structures

Journal Article · Thu Aug 04 00:00:00 EDT 2022 · Nature Synthesis

DOI:https://doi.org/10.1038/s44160-022-00129-x· OSTI ID:1883712

^[1]; ^[1]; ^[2]; Hu, Yongfeng ^[3]; Yan, Qiang-Qiang ^[4]; Shen, Shan-Cheng ^[4]; ^[1]; ^[2]; Shakouri, Mohsen ^[3]; ^[2]; ^[2]; Paterson, Alisa R. ^[3]; ^[4]; ^[1]

Rice Univ., Houston, TX (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Univ. of Saskatchewan, Saskatoon, SK (Canada)
Univ. of Science and Technology of China, Hefei (China)

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. In this work, 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.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: Canada Foundation for Innovation (CFI); Canadian Institutes of Health Research (CIHR); Government of Saskatchewan; National Research Council (NRC); Natural Sciences and Engineering Research Council (NSERC); Rice University; Roy E. Campbell Faculty Development Award; USDOE Office of Science (SC), Basic Energy Sciences (BES); University of Saskatchewan; Welch Foundation

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1883712

Journal Information:: Nature Synthesis, Journal Name: Nature Synthesis Journal Issue: 8 Vol. 1; ISSN 2731-0582

Publisher:: Springer NatureCopyright Statement

Country of Publication:: United States

Language:: English

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