Nanoparticles as an antidote for poisoned gold single-atom catalysts in sustainable propylene epoxidation

Qianhong Wang, Keng Sang, Changwei Liu, Zhihua Zhang, Wenyao Chen (), Te Ji, Lina Li, Cheng Lian, Gang Qian, Jing Zhang, Xinggui Zhou (), Weikang Yuan and Xuezhi Duan ()
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Qianhong Wang: East China University of Science and Technology
Keng Sang: East China University of Science and Technology
Changwei Liu: East China University of Science and Technology
Zhihua Zhang: East China University of Science and Technology
Wenyao Chen: East China University of Science and Technology
Te Ji: Shanghai Advanced Research Institute
Lina Li: Shanghai Advanced Research Institute
Cheng Lian: East China University of Science and Technology
Gang Qian: East China University of Science and Technology
Jing Zhang: East China University of Science and Technology
Xinggui Zhou: East China University of Science and Technology
Weikang Yuan: East China University of Science and Technology
Xuezhi Duan: East China University of Science and Technology

Nature Communications, 2024, vol. 15, issue 1, 1-12

Abstract: Abstract The development of sustainable and anti-poisoning single-atom catalysts (SACs) is essential for advancing their research from laboratory to industry. Here, we present a proof-of-concept study on the poisoning of Au SACs, and the antidote of Au nanoparticles (NPs), with trace addition shown to reinforce and sustain propylene epoxidation. Multiple characterizations, kinetics investigations, and multiscale simulations reveal that Au SACs display remarkable epoxidation activity at a low propylene coverage, but become poisoned at higher coverages. Interestingly, Au NPs can synergistically cooperate with Au SACs by providing distinct active sites required for H2/O2 and C3H6 activations, as well as hydroperoxyl radical to restore poisoned SACs. The difference in reaction order between C3H6 and H2 (nC3H6-nH2) is identified as the descriptor for establishing the volcano curves, which can be fine-tuned by the intimacy and composition of SACs and NPs to achieve a rate-matching scenario for the formation, transfer, and consumption of hydroperoxyl. Consequently, only trace addition of Au NPs antidote (0.3% ratio of SACs) stimulates significant improvements in propylene oxide formation rate, selectivity, and H2 efficiency compared to SACs alone, offering a 56-fold, 3-fold, and 22-fold increase, respectively, whose performances can be maintained for 150 h.

Date: 2024
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DOI: 10.1038/s41467-024-47538-4

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