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A single iron site confined in a graphene matrix for the catalytic oxidation of benzene at room temperature

Coordinatively unsaturated (CUS) iron sites are highly active in catalytic oxidation reactions; however, maintaining the CUS structure of iron during heterogeneous catalytic reactions is a great challenge. Here, we report a strategy to stabilize single-atom CUS iron sites by embedding highly dispers...

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Autores principales: Deng, Dehui, Chen, Xiaoqi, Yu, Liang, Wu, Xing, Liu, Qingfei, Liu, Yun, Yang, Huaixin, Tian, Huanfang, Hu, Yongfeng, Du, Peipei, Si, Rui, Wang, Junhu, Cui, Xiaoju, Li, Haobo, Xiao, Jianping, Xu, Tao, Deng, Jiao, Yang, Fan, Duchesne, Paul N., Zhang, Peng, Zhou, Jigang, Sun, Litao, Li, Jianqi, Pan, Xiulian, Bao, Xinhe
Formato: Online Artículo Texto
Lenguaje:English
Publicado: American Association for the Advancement of Science 2015
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC4672762/
https://www.ncbi.nlm.nih.gov/pubmed/26665170
http://dx.doi.org/10.1126/sciadv.1500462
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author Deng, Dehui
Chen, Xiaoqi
Yu, Liang
Wu, Xing
Liu, Qingfei
Liu, Yun
Yang, Huaixin
Tian, Huanfang
Hu, Yongfeng
Du, Peipei
Si, Rui
Wang, Junhu
Cui, Xiaoju
Li, Haobo
Xiao, Jianping
Xu, Tao
Deng, Jiao
Yang, Fan
Duchesne, Paul N.
Zhang, Peng
Zhou, Jigang
Sun, Litao
Li, Jianqi
Pan, Xiulian
Bao, Xinhe
author_facet Deng, Dehui
Chen, Xiaoqi
Yu, Liang
Wu, Xing
Liu, Qingfei
Liu, Yun
Yang, Huaixin
Tian, Huanfang
Hu, Yongfeng
Du, Peipei
Si, Rui
Wang, Junhu
Cui, Xiaoju
Li, Haobo
Xiao, Jianping
Xu, Tao
Deng, Jiao
Yang, Fan
Duchesne, Paul N.
Zhang, Peng
Zhou, Jigang
Sun, Litao
Li, Jianqi
Pan, Xiulian
Bao, Xinhe
author_sort Deng, Dehui
collection PubMed
description Coordinatively unsaturated (CUS) iron sites are highly active in catalytic oxidation reactions; however, maintaining the CUS structure of iron during heterogeneous catalytic reactions is a great challenge. Here, we report a strategy to stabilize single-atom CUS iron sites by embedding highly dispersed FeN(4) centers in the graphene matrix. The atomic structure of FeN(4) centers in graphene was revealed for the first time by combining high-resolution transmission electron microscopy/high-angle annular dark-field scanning transmission electron microscopy with low-temperature scanning tunneling microscopy. These confined single-atom iron sites exhibit high performance in the direct catalytic oxidation of benzene to phenol at room temperature, with a conversion of 23.4% and a yield of 18.7%, and can even proceed efficiently at 0°C with a phenol yield of 8.3% after 24 hours. Both experimental measurements and density functional theory calculations indicate that the formation of the Fe═O intermediate structure is a key step to promoting the conversion of benzene to phenol. These findings could pave the way toward highly efficient nonprecious catalysts for low-temperature oxidation reactions in heterogeneous catalysis and electrocatalysis.
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spelling pubmed-46727622015-12-10 A single iron site confined in a graphene matrix for the catalytic oxidation of benzene at room temperature Deng, Dehui Chen, Xiaoqi Yu, Liang Wu, Xing Liu, Qingfei Liu, Yun Yang, Huaixin Tian, Huanfang Hu, Yongfeng Du, Peipei Si, Rui Wang, Junhu Cui, Xiaoju Li, Haobo Xiao, Jianping Xu, Tao Deng, Jiao Yang, Fan Duchesne, Paul N. Zhang, Peng Zhou, Jigang Sun, Litao Li, Jianqi Pan, Xiulian Bao, Xinhe Sci Adv Research Articles Coordinatively unsaturated (CUS) iron sites are highly active in catalytic oxidation reactions; however, maintaining the CUS structure of iron during heterogeneous catalytic reactions is a great challenge. Here, we report a strategy to stabilize single-atom CUS iron sites by embedding highly dispersed FeN(4) centers in the graphene matrix. The atomic structure of FeN(4) centers in graphene was revealed for the first time by combining high-resolution transmission electron microscopy/high-angle annular dark-field scanning transmission electron microscopy with low-temperature scanning tunneling microscopy. These confined single-atom iron sites exhibit high performance in the direct catalytic oxidation of benzene to phenol at room temperature, with a conversion of 23.4% and a yield of 18.7%, and can even proceed efficiently at 0°C with a phenol yield of 8.3% after 24 hours. Both experimental measurements and density functional theory calculations indicate that the formation of the Fe═O intermediate structure is a key step to promoting the conversion of benzene to phenol. These findings could pave the way toward highly efficient nonprecious catalysts for low-temperature oxidation reactions in heterogeneous catalysis and electrocatalysis. American Association for the Advancement of Science 2015-12-04 /pmc/articles/PMC4672762/ /pubmed/26665170 http://dx.doi.org/10.1126/sciadv.1500462 Text en Copyright © 2015, The Authors http://creativecommons.org/licenses/by-nc/4.0/ This is an open-access article distributed under the terms of the Creative Commons Attribution-NonCommercial license (http://creativecommons.org/licenses/by-nc/4.0/) , which permits use, distribution, and reproduction in any medium, so long as the resultant use is not for commercial advantage and provided the original work is properly cited.
spellingShingle Research Articles
Deng, Dehui
Chen, Xiaoqi
Yu, Liang
Wu, Xing
Liu, Qingfei
Liu, Yun
Yang, Huaixin
Tian, Huanfang
Hu, Yongfeng
Du, Peipei
Si, Rui
Wang, Junhu
Cui, Xiaoju
Li, Haobo
Xiao, Jianping
Xu, Tao
Deng, Jiao
Yang, Fan
Duchesne, Paul N.
Zhang, Peng
Zhou, Jigang
Sun, Litao
Li, Jianqi
Pan, Xiulian
Bao, Xinhe
A single iron site confined in a graphene matrix for the catalytic oxidation of benzene at room temperature
title A single iron site confined in a graphene matrix for the catalytic oxidation of benzene at room temperature
title_full A single iron site confined in a graphene matrix for the catalytic oxidation of benzene at room temperature
title_fullStr A single iron site confined in a graphene matrix for the catalytic oxidation of benzene at room temperature
title_full_unstemmed A single iron site confined in a graphene matrix for the catalytic oxidation of benzene at room temperature
title_short A single iron site confined in a graphene matrix for the catalytic oxidation of benzene at room temperature
title_sort single iron site confined in a graphene matrix for the catalytic oxidation of benzene at room temperature
topic Research Articles
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC4672762/
https://www.ncbi.nlm.nih.gov/pubmed/26665170
http://dx.doi.org/10.1126/sciadv.1500462
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