Nanoparticles as an antidote for poisoned gold single-atom catalysts in sustainable propylene epoxidation
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...
| Main Authors: | , , , , , , , , , , , , |
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| Format: | Article |
| Language: | English |
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Nature Portfolio
2024-04-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-024-47538-4 |
| _version_ | 1797199344277913600 |
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| author | 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 |
| author_facet | 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 |
| author_sort | Qianhong Wang |
| collection | DOAJ |
| description | 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. |
| first_indexed | 2024-04-24T07:14:16Z |
| format | Article |
| id | doaj.art-878036e7968f40de8989efb16c383fe8 |
| institution | Directory Open Access Journal |
| issn | 2041-1723 |
| language | English |
| last_indexed | 2024-04-24T07:14:16Z |
| publishDate | 2024-04-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj.art-878036e7968f40de8989efb16c383fe82024-04-21T11:24:34ZengNature PortfolioNature Communications2041-17232024-04-0115111210.1038/s41467-024-47538-4Nanoparticles as an antidote for poisoned gold single-atom catalysts in sustainable propylene epoxidationQianhong Wang0Keng Sang1Changwei Liu2Zhihua Zhang3Wenyao Chen4Te Ji5Lina Li6Cheng Lian7Gang Qian8Jing Zhang9Xinggui Zhou10Weikang Yuan11Xuezhi Duan12State Key Laboratory of Chemical Engineering, East China University of Science and TechnologyState Key Laboratory of Chemical Engineering, East China University of Science and TechnologyState Key Laboratory of Chemical Engineering, East China University of Science and TechnologyState Key Laboratory of Chemical Engineering, East China University of Science and TechnologyState Key Laboratory of Chemical Engineering, East China University of Science and TechnologyShanghai Synchrotron Radiation Facility, Shanghai Advanced Research InstituteShanghai Synchrotron Radiation Facility, Shanghai Advanced Research InstituteState Key Laboratory of Chemical Engineering, East China University of Science and TechnologyState Key Laboratory of Chemical Engineering, East China University of Science and TechnologyState Key Laboratory of Chemical Engineering, East China University of Science and TechnologyState Key Laboratory of Chemical Engineering, East China University of Science and TechnologyState Key Laboratory of Chemical Engineering, East China University of Science and TechnologyState Key Laboratory of Chemical Engineering, East China University of Science and TechnologyAbstract 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.https://doi.org/10.1038/s41467-024-47538-4 |
| spellingShingle | 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 Nanoparticles as an antidote for poisoned gold single-atom catalysts in sustainable propylene epoxidation Nature Communications |
| title | Nanoparticles as an antidote for poisoned gold single-atom catalysts in sustainable propylene epoxidation |
| title_full | Nanoparticles as an antidote for poisoned gold single-atom catalysts in sustainable propylene epoxidation |
| title_fullStr | Nanoparticles as an antidote for poisoned gold single-atom catalysts in sustainable propylene epoxidation |
| title_full_unstemmed | Nanoparticles as an antidote for poisoned gold single-atom catalysts in sustainable propylene epoxidation |
| title_short | Nanoparticles as an antidote for poisoned gold single-atom catalysts in sustainable propylene epoxidation |
| title_sort | nanoparticles as an antidote for poisoned gold single atom catalysts in sustainable propylene epoxidation |
| url | https://doi.org/10.1038/s41467-024-47538-4 |
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