Cargando…

In situ dynamic tracking of heterogeneous nanocatalytic processes by shell-isolated nanoparticle-enhanced Raman spectroscopy

Surface molecular information acquired in situ from a catalytic process can greatly promote the rational design of highly efficient catalysts by revealing structure-activity relationships and reaction mechanisms. Raman spectroscopy can provide this rich structural information, but normal Raman is no...

Descripción completa

Detalles Bibliográficos
Autores principales: Zhang, Hua, Wang, Chen, Sun, Han-Lei, Fu, Gang, Chen, Shu, Zhang, Yue-Jiao, Chen, Bing-Hui, Anema, Jason R., Yang, Zhi-Lin, Li, Jian-Feng, Tian, Zhong-Qun
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group 2017
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5458081/
https://www.ncbi.nlm.nih.gov/pubmed/28537269
http://dx.doi.org/10.1038/ncomms15447
_version_ 1783241680229498880
author Zhang, Hua
Wang, Chen
Sun, Han-Lei
Fu, Gang
Chen, Shu
Zhang, Yue-Jiao
Chen, Bing-Hui
Anema, Jason R.
Yang, Zhi-Lin
Li, Jian-Feng
Tian, Zhong-Qun
author_facet Zhang, Hua
Wang, Chen
Sun, Han-Lei
Fu, Gang
Chen, Shu
Zhang, Yue-Jiao
Chen, Bing-Hui
Anema, Jason R.
Yang, Zhi-Lin
Li, Jian-Feng
Tian, Zhong-Qun
author_sort Zhang, Hua
collection PubMed
description Surface molecular information acquired in situ from a catalytic process can greatly promote the rational design of highly efficient catalysts by revealing structure-activity relationships and reaction mechanisms. Raman spectroscopy can provide this rich structural information, but normal Raman is not sensitive enough to detect trace active species adsorbed on the surface of catalysts. Here we develop a general method for in situ monitoring of heterogeneous catalytic processes through shell-isolated nanoparticle-enhanced Raman spectroscopy (SHINERS) satellite nanocomposites (Au-core silica-shell nanocatalyst-satellite structures), which are stable and have extremely high surface Raman sensitivity. By combining operando SHINERS with density functional theory calculations, we identify the working mechanisms for CO oxidation over PtFe and Pd nanocatalysts, which are typical low- and high-temperature catalysts, respectively. Active species, such as surface oxides, superoxide/peroxide species and Pd–C/Pt–C bonds are directly observed during the reactions. We demonstrate that in situ SHINERS can provide a deep understanding of the fundamental concepts of catalysis.
format Online
Article
Text
id pubmed-5458081
institution National Center for Biotechnology Information
language English
publishDate 2017
publisher Nature Publishing Group
record_format MEDLINE/PubMed
spelling pubmed-54580812017-07-11 In situ dynamic tracking of heterogeneous nanocatalytic processes by shell-isolated nanoparticle-enhanced Raman spectroscopy Zhang, Hua Wang, Chen Sun, Han-Lei Fu, Gang Chen, Shu Zhang, Yue-Jiao Chen, Bing-Hui Anema, Jason R. Yang, Zhi-Lin Li, Jian-Feng Tian, Zhong-Qun Nat Commun Article Surface molecular information acquired in situ from a catalytic process can greatly promote the rational design of highly efficient catalysts by revealing structure-activity relationships and reaction mechanisms. Raman spectroscopy can provide this rich structural information, but normal Raman is not sensitive enough to detect trace active species adsorbed on the surface of catalysts. Here we develop a general method for in situ monitoring of heterogeneous catalytic processes through shell-isolated nanoparticle-enhanced Raman spectroscopy (SHINERS) satellite nanocomposites (Au-core silica-shell nanocatalyst-satellite structures), which are stable and have extremely high surface Raman sensitivity. By combining operando SHINERS with density functional theory calculations, we identify the working mechanisms for CO oxidation over PtFe and Pd nanocatalysts, which are typical low- and high-temperature catalysts, respectively. Active species, such as surface oxides, superoxide/peroxide species and Pd–C/Pt–C bonds are directly observed during the reactions. We demonstrate that in situ SHINERS can provide a deep understanding of the fundamental concepts of catalysis. Nature Publishing Group 2017-05-24 /pmc/articles/PMC5458081/ /pubmed/28537269 http://dx.doi.org/10.1038/ncomms15447 Text en Copyright © 2017, The Author(s) http://creativecommons.org/licenses/by/4.0/ This work is licensed under a Creative Commons Attribution 4.0 International License. The images or other third party material in this article are included in the article's Creative Commons license, unless indicated otherwise in the credit line; if the material is not included under the Creative Commons license, users will need to obtain permission from the license holder to reproduce the material. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/
spellingShingle Article
Zhang, Hua
Wang, Chen
Sun, Han-Lei
Fu, Gang
Chen, Shu
Zhang, Yue-Jiao
Chen, Bing-Hui
Anema, Jason R.
Yang, Zhi-Lin
Li, Jian-Feng
Tian, Zhong-Qun
In situ dynamic tracking of heterogeneous nanocatalytic processes by shell-isolated nanoparticle-enhanced Raman spectroscopy
title In situ dynamic tracking of heterogeneous nanocatalytic processes by shell-isolated nanoparticle-enhanced Raman spectroscopy
title_full In situ dynamic tracking of heterogeneous nanocatalytic processes by shell-isolated nanoparticle-enhanced Raman spectroscopy
title_fullStr In situ dynamic tracking of heterogeneous nanocatalytic processes by shell-isolated nanoparticle-enhanced Raman spectroscopy
title_full_unstemmed In situ dynamic tracking of heterogeneous nanocatalytic processes by shell-isolated nanoparticle-enhanced Raman spectroscopy
title_short In situ dynamic tracking of heterogeneous nanocatalytic processes by shell-isolated nanoparticle-enhanced Raman spectroscopy
title_sort in situ dynamic tracking of heterogeneous nanocatalytic processes by shell-isolated nanoparticle-enhanced raman spectroscopy
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5458081/
https://www.ncbi.nlm.nih.gov/pubmed/28537269
http://dx.doi.org/10.1038/ncomms15447
work_keys_str_mv AT zhanghua insitudynamictrackingofheterogeneousnanocatalyticprocessesbyshellisolatednanoparticleenhancedramanspectroscopy
AT wangchen insitudynamictrackingofheterogeneousnanocatalyticprocessesbyshellisolatednanoparticleenhancedramanspectroscopy
AT sunhanlei insitudynamictrackingofheterogeneousnanocatalyticprocessesbyshellisolatednanoparticleenhancedramanspectroscopy
AT fugang insitudynamictrackingofheterogeneousnanocatalyticprocessesbyshellisolatednanoparticleenhancedramanspectroscopy
AT chenshu insitudynamictrackingofheterogeneousnanocatalyticprocessesbyshellisolatednanoparticleenhancedramanspectroscopy
AT zhangyuejiao insitudynamictrackingofheterogeneousnanocatalyticprocessesbyshellisolatednanoparticleenhancedramanspectroscopy
AT chenbinghui insitudynamictrackingofheterogeneousnanocatalyticprocessesbyshellisolatednanoparticleenhancedramanspectroscopy
AT anemajasonr insitudynamictrackingofheterogeneousnanocatalyticprocessesbyshellisolatednanoparticleenhancedramanspectroscopy
AT yangzhilin insitudynamictrackingofheterogeneousnanocatalyticprocessesbyshellisolatednanoparticleenhancedramanspectroscopy
AT lijianfeng insitudynamictrackingofheterogeneousnanocatalyticprocessesbyshellisolatednanoparticleenhancedramanspectroscopy
AT tianzhongqun insitudynamictrackingofheterogeneousnanocatalyticprocessesbyshellisolatednanoparticleenhancedramanspectroscopy