Cargando…

A versatile route to fabricate single atom catalysts with high chemoselectivity and regioselectivity in hydrogenation

Preparation of single atom catalysts (SACs) is of broad interest to materials scientists and chemists but remains a formidable challenge. Herein, we develop an efficient approach to synthesize SACs via a precursor-dilution strategy, in which metalloporphyrin (MTPP) with target metals are co-polymeri...

Descripción completa

Detalles Bibliográficos
Autores principales: He, Xiaohui, He, Qian, Deng, Yuchen, Peng, Mi, Chen, Hongyu, Zhang, Ying, Yao, Siyu, Zhang, Mengtao, Xiao, Dequan, Ma, Ding, Ge, Binghui, Ji, Hongbing
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2019
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6694111/
https://www.ncbi.nlm.nih.gov/pubmed/31413344
http://dx.doi.org/10.1038/s41467-019-11619-6
_version_ 1783443778599649280
author He, Xiaohui
He, Qian
Deng, Yuchen
Peng, Mi
Chen, Hongyu
Zhang, Ying
Yao, Siyu
Zhang, Mengtao
Xiao, Dequan
Ma, Ding
Ge, Binghui
Ji, Hongbing
author_facet He, Xiaohui
He, Qian
Deng, Yuchen
Peng, Mi
Chen, Hongyu
Zhang, Ying
Yao, Siyu
Zhang, Mengtao
Xiao, Dequan
Ma, Ding
Ge, Binghui
Ji, Hongbing
author_sort He, Xiaohui
collection PubMed
description Preparation of single atom catalysts (SACs) is of broad interest to materials scientists and chemists but remains a formidable challenge. Herein, we develop an efficient approach to synthesize SACs via a precursor-dilution strategy, in which metalloporphyrin (MTPP) with target metals are co-polymerized with diluents (tetraphenylporphyrin, TPP), followed by pyrolysis to N-doped porous carbon supported SACs (M(1)/N-C). Twenty-four different SACs, including noble metals and non-noble metals, are successfully prepared. In addition, the synthesis of a series of catalysts with different surface atom densities, bi-metallic sites, and metal aggregation states are achieved. This approach shows remarkable adjustability and generality, providing sufficient freedom to design catalysts at atomic-scale and explore the unique catalytic properties of SACs. As an example, we show that the prepared Pt(1)/N-C exhibits superior chemoselectivity and regioselectivity in hydrogenation. It only converts terminal alkynes to alkenes while keeping other reducible functional groups such as alkenyl, nitro group, and even internal alkyne intact.
format Online
Article
Text
id pubmed-6694111
institution National Center for Biotechnology Information
language English
publishDate 2019
publisher Nature Publishing Group UK
record_format MEDLINE/PubMed
spelling pubmed-66941112019-08-19 A versatile route to fabricate single atom catalysts with high chemoselectivity and regioselectivity in hydrogenation He, Xiaohui He, Qian Deng, Yuchen Peng, Mi Chen, Hongyu Zhang, Ying Yao, Siyu Zhang, Mengtao Xiao, Dequan Ma, Ding Ge, Binghui Ji, Hongbing Nat Commun Article Preparation of single atom catalysts (SACs) is of broad interest to materials scientists and chemists but remains a formidable challenge. Herein, we develop an efficient approach to synthesize SACs via a precursor-dilution strategy, in which metalloporphyrin (MTPP) with target metals are co-polymerized with diluents (tetraphenylporphyrin, TPP), followed by pyrolysis to N-doped porous carbon supported SACs (M(1)/N-C). Twenty-four different SACs, including noble metals and non-noble metals, are successfully prepared. In addition, the synthesis of a series of catalysts with different surface atom densities, bi-metallic sites, and metal aggregation states are achieved. This approach shows remarkable adjustability and generality, providing sufficient freedom to design catalysts at atomic-scale and explore the unique catalytic properties of SACs. As an example, we show that the prepared Pt(1)/N-C exhibits superior chemoselectivity and regioselectivity in hydrogenation. It only converts terminal alkynes to alkenes while keeping other reducible functional groups such as alkenyl, nitro group, and even internal alkyne intact. Nature Publishing Group UK 2019-08-14 /pmc/articles/PMC6694111/ /pubmed/31413344 http://dx.doi.org/10.1038/s41467-019-11619-6 Text en © The Author(s) 2019 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
He, Xiaohui
He, Qian
Deng, Yuchen
Peng, Mi
Chen, Hongyu
Zhang, Ying
Yao, Siyu
Zhang, Mengtao
Xiao, Dequan
Ma, Ding
Ge, Binghui
Ji, Hongbing
A versatile route to fabricate single atom catalysts with high chemoselectivity and regioselectivity in hydrogenation
title A versatile route to fabricate single atom catalysts with high chemoselectivity and regioselectivity in hydrogenation
title_full A versatile route to fabricate single atom catalysts with high chemoselectivity and regioselectivity in hydrogenation
title_fullStr A versatile route to fabricate single atom catalysts with high chemoselectivity and regioselectivity in hydrogenation
title_full_unstemmed A versatile route to fabricate single atom catalysts with high chemoselectivity and regioselectivity in hydrogenation
title_short A versatile route to fabricate single atom catalysts with high chemoselectivity and regioselectivity in hydrogenation
title_sort versatile route to fabricate single atom catalysts with high chemoselectivity and regioselectivity in hydrogenation
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6694111/
https://www.ncbi.nlm.nih.gov/pubmed/31413344
http://dx.doi.org/10.1038/s41467-019-11619-6
work_keys_str_mv AT hexiaohui aversatileroutetofabricatesingleatomcatalystswithhighchemoselectivityandregioselectivityinhydrogenation
AT heqian aversatileroutetofabricatesingleatomcatalystswithhighchemoselectivityandregioselectivityinhydrogenation
AT dengyuchen aversatileroutetofabricatesingleatomcatalystswithhighchemoselectivityandregioselectivityinhydrogenation
AT pengmi aversatileroutetofabricatesingleatomcatalystswithhighchemoselectivityandregioselectivityinhydrogenation
AT chenhongyu aversatileroutetofabricatesingleatomcatalystswithhighchemoselectivityandregioselectivityinhydrogenation
AT zhangying aversatileroutetofabricatesingleatomcatalystswithhighchemoselectivityandregioselectivityinhydrogenation
AT yaosiyu aversatileroutetofabricatesingleatomcatalystswithhighchemoselectivityandregioselectivityinhydrogenation
AT zhangmengtao aversatileroutetofabricatesingleatomcatalystswithhighchemoselectivityandregioselectivityinhydrogenation
AT xiaodequan aversatileroutetofabricatesingleatomcatalystswithhighchemoselectivityandregioselectivityinhydrogenation
AT mading aversatileroutetofabricatesingleatomcatalystswithhighchemoselectivityandregioselectivityinhydrogenation
AT gebinghui aversatileroutetofabricatesingleatomcatalystswithhighchemoselectivityandregioselectivityinhydrogenation
AT jihongbing aversatileroutetofabricatesingleatomcatalystswithhighchemoselectivityandregioselectivityinhydrogenation
AT hexiaohui versatileroutetofabricatesingleatomcatalystswithhighchemoselectivityandregioselectivityinhydrogenation
AT heqian versatileroutetofabricatesingleatomcatalystswithhighchemoselectivityandregioselectivityinhydrogenation
AT dengyuchen versatileroutetofabricatesingleatomcatalystswithhighchemoselectivityandregioselectivityinhydrogenation
AT pengmi versatileroutetofabricatesingleatomcatalystswithhighchemoselectivityandregioselectivityinhydrogenation
AT chenhongyu versatileroutetofabricatesingleatomcatalystswithhighchemoselectivityandregioselectivityinhydrogenation
AT zhangying versatileroutetofabricatesingleatomcatalystswithhighchemoselectivityandregioselectivityinhydrogenation
AT yaosiyu versatileroutetofabricatesingleatomcatalystswithhighchemoselectivityandregioselectivityinhydrogenation
AT zhangmengtao versatileroutetofabricatesingleatomcatalystswithhighchemoselectivityandregioselectivityinhydrogenation
AT xiaodequan versatileroutetofabricatesingleatomcatalystswithhighchemoselectivityandregioselectivityinhydrogenation
AT mading versatileroutetofabricatesingleatomcatalystswithhighchemoselectivityandregioselectivityinhydrogenation
AT gebinghui versatileroutetofabricatesingleatomcatalystswithhighchemoselectivityandregioselectivityinhydrogenation
AT jihongbing versatileroutetofabricatesingleatomcatalystswithhighchemoselectivityandregioselectivityinhydrogenation