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Mechanism driven design of trimer Ni(1)Sb(2) site delivering superior hydrogenation selectivity to ethylene
Mechanism driven catalyst design with atomically uniform ensemble sites is an important yet challenging issue in heterogeneous catalysis associated with breaking the activity-selectivity trade-off. Herein, a trimer Ni(1)Sb(2) site in NiSb intermetallic featuring superior selectivity is elaborated fo...
Autores principales: | , , , , , , , , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
Nature Publishing Group UK
2022
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Materias: | |
Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9492709/ https://www.ncbi.nlm.nih.gov/pubmed/36131070 http://dx.doi.org/10.1038/s41467-022-33250-8 |
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author | Ge, Xiaohu Dou, Mingying Cao, Yueqiang Liu, Xi Yuwen, Qiang Zhang, Jing Qian, Gang Gong, Xueqing Zhou, Xinggui Chen, Liwei Yuan, Weikang Duan, Xuezhi |
author_facet | Ge, Xiaohu Dou, Mingying Cao, Yueqiang Liu, Xi Yuwen, Qiang Zhang, Jing Qian, Gang Gong, Xueqing Zhou, Xinggui Chen, Liwei Yuan, Weikang Duan, Xuezhi |
author_sort | Ge, Xiaohu |
collection | PubMed |
description | Mechanism driven catalyst design with atomically uniform ensemble sites is an important yet challenging issue in heterogeneous catalysis associated with breaking the activity-selectivity trade-off. Herein, a trimer Ni(1)Sb(2) site in NiSb intermetallic featuring superior selectivity is elaborated for acetylene semi-hydrogenation via a theoretical guidance with a precise synthesis strategy. The trimer Ni(1)Sb(2) site in NiSb intermetallic is predicted to endow acetylene reactant with an adequately but not excessively strong σ-adsorption mode while ethylene product with a weak π-adsorption one, where such compromise delivers higher ethylene formation rate. An in-situ trapping of molten Sb by Ni strategy is developed to realize the construction of Ni(1)Sb(2) site in the intermetallic P6(3)/mmc NiSb catalysts. Such catalyst exhibits ethylene selectivity up to 93.2% at 100% of acetylene conversion, significantly prevailing over the referred Ni catalyst. These insights shed new lights on rational catalyst design by taming active sites to energetically match targeted reaction pathway. |
format | Online Article Text |
id | pubmed-9492709 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2022 |
publisher | Nature Publishing Group UK |
record_format | MEDLINE/PubMed |
spelling | pubmed-94927092022-09-23 Mechanism driven design of trimer Ni(1)Sb(2) site delivering superior hydrogenation selectivity to ethylene Ge, Xiaohu Dou, Mingying Cao, Yueqiang Liu, Xi Yuwen, Qiang Zhang, Jing Qian, Gang Gong, Xueqing Zhou, Xinggui Chen, Liwei Yuan, Weikang Duan, Xuezhi Nat Commun Article Mechanism driven catalyst design with atomically uniform ensemble sites is an important yet challenging issue in heterogeneous catalysis associated with breaking the activity-selectivity trade-off. Herein, a trimer Ni(1)Sb(2) site in NiSb intermetallic featuring superior selectivity is elaborated for acetylene semi-hydrogenation via a theoretical guidance with a precise synthesis strategy. The trimer Ni(1)Sb(2) site in NiSb intermetallic is predicted to endow acetylene reactant with an adequately but not excessively strong σ-adsorption mode while ethylene product with a weak π-adsorption one, where such compromise delivers higher ethylene formation rate. An in-situ trapping of molten Sb by Ni strategy is developed to realize the construction of Ni(1)Sb(2) site in the intermetallic P6(3)/mmc NiSb catalysts. Such catalyst exhibits ethylene selectivity up to 93.2% at 100% of acetylene conversion, significantly prevailing over the referred Ni catalyst. These insights shed new lights on rational catalyst design by taming active sites to energetically match targeted reaction pathway. Nature Publishing Group UK 2022-09-21 /pmc/articles/PMC9492709/ /pubmed/36131070 http://dx.doi.org/10.1038/s41467-022-33250-8 Text en © The Author(s) 2022 https://creativecommons.org/licenses/by/4.0/Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/ (https://creativecommons.org/licenses/by/4.0/) . |
spellingShingle | Article Ge, Xiaohu Dou, Mingying Cao, Yueqiang Liu, Xi Yuwen, Qiang Zhang, Jing Qian, Gang Gong, Xueqing Zhou, Xinggui Chen, Liwei Yuan, Weikang Duan, Xuezhi Mechanism driven design of trimer Ni(1)Sb(2) site delivering superior hydrogenation selectivity to ethylene |
title | Mechanism driven design of trimer Ni(1)Sb(2) site delivering superior hydrogenation selectivity to ethylene |
title_full | Mechanism driven design of trimer Ni(1)Sb(2) site delivering superior hydrogenation selectivity to ethylene |
title_fullStr | Mechanism driven design of trimer Ni(1)Sb(2) site delivering superior hydrogenation selectivity to ethylene |
title_full_unstemmed | Mechanism driven design of trimer Ni(1)Sb(2) site delivering superior hydrogenation selectivity to ethylene |
title_short | Mechanism driven design of trimer Ni(1)Sb(2) site delivering superior hydrogenation selectivity to ethylene |
title_sort | mechanism driven design of trimer ni(1)sb(2) site delivering superior hydrogenation selectivity to ethylene |
topic | Article |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9492709/ https://www.ncbi.nlm.nih.gov/pubmed/36131070 http://dx.doi.org/10.1038/s41467-022-33250-8 |
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