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

Author

Listed:
  • 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)

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.

Suggested Citation

  • Qianhong Wang & Keng Sang & Changwei Liu & Zhihua Zhang & Wenyao Chen & Te Ji & Lina Li & Cheng Lian & Gang Qian & Jing Zhang & Xinggui Zhou & Weikang Yuan & Xuezhi Duan, 2024. "Nanoparticles as an antidote for poisoned gold single-atom catalysts in sustainable propylene epoxidation," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
  • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-47538-4
    DOI: 10.1038/s41467-024-47538-4
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    References listed on IDEAS

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    1. Zhibo Liu & Fei Huang & Mi Peng & Yunlei Chen & Xiangbin Cai & Linlin Wang & Zenan Hu & Xiaodong Wen & Ning Wang & Dequan Xiao & Hong Jiang & Hongbin Sun & Hongyang Liu & Ding Ma, 2021. "Tuning the selectivity of catalytic nitriles hydrogenation by structure regulation in atomically dispersed Pd catalysts," Nature Communications, Nature, vol. 12(1), pages 1-8, December.
    2. Hongpan Rong & Shufang Ji & Jiatao Zhang & Dingsheng Wang & Yadong Li, 2020. "Synthetic strategies of supported atomic clusters for heterogeneous catalysis," Nature Communications, Nature, vol. 11(1), pages 1-14, December.
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