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Carbon nitride supported Fe(2) cluster catalysts with superior performance for alkene epoxidation
Sub-nano metal clusters often exhibit unique and unexpected properties, which make them particularly attractive as catalysts. Herein, we report a “precursor-preselected” wet-chemistry strategy to synthesize highly dispersed Fe(2) clusters that are supported on mesoporous carbon nitride (mpg-C(3)N(4)...
Autores principales: | , , , , , , , , , , , , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
Nature Publishing Group UK
2018
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Materias: | |
Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6003949/ https://www.ncbi.nlm.nih.gov/pubmed/29907774 http://dx.doi.org/10.1038/s41467-018-04845-x |
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author | Tian, Shubo Fu, Qiang Chen, Wenxing Feng, Quanchen Chen, Zheng Zhang, Jian Cheong, Weng-Chon Yu, Rong Gu, Lin Dong, Juncai Luo, Jun Chen, Chen Peng, Qing Draxl, Claudia Wang, Dingsheng Li, Yadong |
author_facet | Tian, Shubo Fu, Qiang Chen, Wenxing Feng, Quanchen Chen, Zheng Zhang, Jian Cheong, Weng-Chon Yu, Rong Gu, Lin Dong, Juncai Luo, Jun Chen, Chen Peng, Qing Draxl, Claudia Wang, Dingsheng Li, Yadong |
author_sort | Tian, Shubo |
collection | PubMed |
description | Sub-nano metal clusters often exhibit unique and unexpected properties, which make them particularly attractive as catalysts. Herein, we report a “precursor-preselected” wet-chemistry strategy to synthesize highly dispersed Fe(2) clusters that are supported on mesoporous carbon nitride (mpg-C(3)N(4)). The obtained Fe(2)/mpg-C(3)N(4) sample exhibits superior catalytic performance for the epoxidation of trans-stilbene to trans-stilbene oxide, showing outstanding selectivity of 93% at high conversion of 91%. Molecular oxygen is the only oxidant and no aldehyde is used as co-reagent. Under the same condition, by contrast, iron porphyrin, single-atom Fe, and small Fe nanoparticles (ca. 3 nm) are nearly reactively inert. First-principles calculations reveal that the unique reactivity of the Fe(2) clusters originates from the formation of active oxygen species. The general applicability of the synthesis approach is further demonstrated by producing other diatomic clusters like Pd(2) and Ir(2), which lays the foundation for discovering diatomic cluster catalysts. |
format | Online Article Text |
id | pubmed-6003949 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2018 |
publisher | Nature Publishing Group UK |
record_format | MEDLINE/PubMed |
spelling | pubmed-60039492018-06-18 Carbon nitride supported Fe(2) cluster catalysts with superior performance for alkene epoxidation Tian, Shubo Fu, Qiang Chen, Wenxing Feng, Quanchen Chen, Zheng Zhang, Jian Cheong, Weng-Chon Yu, Rong Gu, Lin Dong, Juncai Luo, Jun Chen, Chen Peng, Qing Draxl, Claudia Wang, Dingsheng Li, Yadong Nat Commun Article Sub-nano metal clusters often exhibit unique and unexpected properties, which make them particularly attractive as catalysts. Herein, we report a “precursor-preselected” wet-chemistry strategy to synthesize highly dispersed Fe(2) clusters that are supported on mesoporous carbon nitride (mpg-C(3)N(4)). The obtained Fe(2)/mpg-C(3)N(4) sample exhibits superior catalytic performance for the epoxidation of trans-stilbene to trans-stilbene oxide, showing outstanding selectivity of 93% at high conversion of 91%. Molecular oxygen is the only oxidant and no aldehyde is used as co-reagent. Under the same condition, by contrast, iron porphyrin, single-atom Fe, and small Fe nanoparticles (ca. 3 nm) are nearly reactively inert. First-principles calculations reveal that the unique reactivity of the Fe(2) clusters originates from the formation of active oxygen species. The general applicability of the synthesis approach is further demonstrated by producing other diatomic clusters like Pd(2) and Ir(2), which lays the foundation for discovering diatomic cluster catalysts. Nature Publishing Group UK 2018-06-15 /pmc/articles/PMC6003949/ /pubmed/29907774 http://dx.doi.org/10.1038/s41467-018-04845-x Text en © The Author(s) 2018 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/. |
spellingShingle | Article Tian, Shubo Fu, Qiang Chen, Wenxing Feng, Quanchen Chen, Zheng Zhang, Jian Cheong, Weng-Chon Yu, Rong Gu, Lin Dong, Juncai Luo, Jun Chen, Chen Peng, Qing Draxl, Claudia Wang, Dingsheng Li, Yadong Carbon nitride supported Fe(2) cluster catalysts with superior performance for alkene epoxidation |
title | Carbon nitride supported Fe(2) cluster catalysts with superior performance for alkene epoxidation |
title_full | Carbon nitride supported Fe(2) cluster catalysts with superior performance for alkene epoxidation |
title_fullStr | Carbon nitride supported Fe(2) cluster catalysts with superior performance for alkene epoxidation |
title_full_unstemmed | Carbon nitride supported Fe(2) cluster catalysts with superior performance for alkene epoxidation |
title_short | Carbon nitride supported Fe(2) cluster catalysts with superior performance for alkene epoxidation |
title_sort | carbon nitride supported fe(2) cluster catalysts with superior performance for alkene epoxidation |
topic | Article |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6003949/ https://www.ncbi.nlm.nih.gov/pubmed/29907774 http://dx.doi.org/10.1038/s41467-018-04845-x |
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