General negative pressure annealing approach for creating ultra-high-loading single atom catalyst libraries

Yi Wang, Chongao Li, Xiao Han, Jintao Bai, Xuejing Wang, Lirong Zheng, Chunxia Hong, Zhijun Li, Jinbo Bai, Kunyue Leng (), Yue Lin () and Yunteng Qu ()
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Yi Wang: Northwest University
Chongao Li: Northwest University
Xiao Han: University of Science and Technology of China
Jintao Bai: Northwest University
Xuejing Wang: Northwestern Polytechnical University
Lirong Zheng: Institute of High Energy Physics
Chunxia Hong: Chinese Academy of Science
Zhijun Li: Northeast Petroleum University
Jinbo Bai: LMPS-Laboratoire de Mécanique Paris-Saclay
Kunyue Leng: Northwest University
Yue Lin: University of Science and Technology of China
Yunteng Qu: Northwest University

Nature Communications, 2024, vol. 15, issue 1, 1-9

Abstract: Abstract Catalyst systems populated by high-density single atoms are crucial for improving catalytic activity and selectivity, which can potentially maximize the industrial prospects of heterogeneous single-atom catalysts (SACs). However, achieving high-loading SACs with metal contents above 10 wt% remains challenging. Here we describe a general negative pressure annealing strategy to fabricate ultrahigh-loading SACs with metal contents up to 27.3–44.8 wt% for 13 different metals on a typical carbon nitride matrix. Furthermore, our approach enables the synthesis of high-entropy single-atom catalysts (HESACs) that exhibit the coexistence of multiple metal single atoms with high metal contents. In-situ aberration-corrected HAADF-STEM (AC-STEM) combined with ex-situ X-ray absorption fine structure (XAFS) demonstrate that the negative pressure annealing treatment accelerates the removal of anionic ligand in metal precursors and boosts the bonding of metal species with N defective sites, enabling the formation of dense N-coordinated metal sites. Increasing metal loading on a platinum (Pt) SAC to 41.8 wt% significantly enhances the activity of propane oxidation towards liquid products, including acetone, methanol, and acetic acid et al. This work presents a straightforward and universal approach for achieving many low-cost and high-density SACs for efficient catalytic transformations.

Date: 2024
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DOI: 10.1038/s41467-024-50061-1

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