Catalytic Activity Control via Crossover between Two Different Microstructures

Handle URI:
http://hdl.handle.net/10754/625450
Title:
Catalytic Activity Control via Crossover between Two Different Microstructures
Authors:
Zhou, Yuheng; Zhu, Yihan; Wang, Zhi-Qiang; Zou, Shihui; Ma, Guicen; Xia, Ming; Kong, Xueqian; Xiao, Liping; Gong, Xue-Qing; Fan, Jie
Abstract:
Metal nanocatalysts hold great promise for a wide range of heterogeneous catalytic reactions, while the optimization strategy of catalytic activity is largely restricted by particle size or shape control. Here, we demonstrate that a reversible microstructural control through the crossover between multiply-twinned nanoparticle (MTP) and single crystal (SC) can be readily achieved by solvent post-treatment on gold nanoparticles (AuNPs). Polar solvents (e.g. water, methanol) direct the transformation from MTP to SC accompanied by the disappearance of twinning and stacking faults. A reverse transformation from SC to MTP is achieved in non-polar solvent (e.g. toluene) mixed with thiol ligands. The transformation between two different microstructures is directly observed by in-situ TEM and leads to a drastic modulation of catalytic activity towards the gas-phase selective oxidation of alcohols. There is a quasi-linear relationship between TOFs and MTP concentrations. Based on the combined experimental and theoretical investigations of alcohol chemisorption on these nanocatalysts, we propose that the exposure of {211}-like microfacets associated with twin boundaries and stack faults accounts for the strong chemisorption of alcohol molecules on MTP AuNPs and thus the exceptionally high catalytic activity.
KAUST Department:
King Abdullah University of Science and Technology, Thuwal, 999088, Kingdom of Saudi Arabia.
Citation:
Zhou Y, Zhu Y, Wang Z-Q, Zou S, Ma G, et al. (2017) Catalytic Activity Control via Crossover between Two Different Microstructures. Journal of the American Chemical Society. Available: http://dx.doi.org/10.1021/jacs.7b05476.
Publisher:
American Chemical Society (ACS)
Journal:
Journal of the American Chemical Society
Issue Date:
8-Sep-2017
DOI:
10.1021/jacs.7b05476
Type:
Article
ISSN:
0002-7863; 1520-5126
Sponsors:
This work was supported by National Natural Science Foundation of China (21271153, 21421004, 21373181, 21222307, U1402233), Major Research Plan Of National Natural Science Foundation of China (91545113, 91545103), Fok Ying Tung Education Foundation (131015) and the Fundamental Research Funds for the Central Universities (2014XZZX003-02). The authors are grateful to the King Abdullah University of Science and Technology (KAUST) in Saudi Arabia for providing the characterization of the in situ HRTEM.
Additional Links:
http://pubs.acs.org/doi/abs/10.1021/jacs.7b05476
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Articles

Full metadata record

DC FieldValue Language
dc.contributor.authorZhou, Yuhengen
dc.contributor.authorZhu, Yihanen
dc.contributor.authorWang, Zhi-Qiangen
dc.contributor.authorZou, Shihuien
dc.contributor.authorMa, Guicenen
dc.contributor.authorXia, Mingen
dc.contributor.authorKong, Xueqianen
dc.contributor.authorXiao, Lipingen
dc.contributor.authorGong, Xue-Qingen
dc.contributor.authorFan, Jieen
dc.date.accessioned2017-09-14T06:03:51Z-
dc.date.available2017-09-14T06:03:51Z-
dc.date.issued2017-09-08en
dc.identifier.citationZhou Y, Zhu Y, Wang Z-Q, Zou S, Ma G, et al. (2017) Catalytic Activity Control via Crossover between Two Different Microstructures. Journal of the American Chemical Society. Available: http://dx.doi.org/10.1021/jacs.7b05476.en
dc.identifier.issn0002-7863en
dc.identifier.issn1520-5126en
dc.identifier.doi10.1021/jacs.7b05476en
dc.identifier.urihttp://hdl.handle.net/10754/625450-
dc.description.abstractMetal nanocatalysts hold great promise for a wide range of heterogeneous catalytic reactions, while the optimization strategy of catalytic activity is largely restricted by particle size or shape control. Here, we demonstrate that a reversible microstructural control through the crossover between multiply-twinned nanoparticle (MTP) and single crystal (SC) can be readily achieved by solvent post-treatment on gold nanoparticles (AuNPs). Polar solvents (e.g. water, methanol) direct the transformation from MTP to SC accompanied by the disappearance of twinning and stacking faults. A reverse transformation from SC to MTP is achieved in non-polar solvent (e.g. toluene) mixed with thiol ligands. The transformation between two different microstructures is directly observed by in-situ TEM and leads to a drastic modulation of catalytic activity towards the gas-phase selective oxidation of alcohols. There is a quasi-linear relationship between TOFs and MTP concentrations. Based on the combined experimental and theoretical investigations of alcohol chemisorption on these nanocatalysts, we propose that the exposure of {211}-like microfacets associated with twin boundaries and stack faults accounts for the strong chemisorption of alcohol molecules on MTP AuNPs and thus the exceptionally high catalytic activity.en
dc.description.sponsorshipThis work was supported by National Natural Science Foundation of China (21271153, 21421004, 21373181, 21222307, U1402233), Major Research Plan Of National Natural Science Foundation of China (91545113, 91545103), Fok Ying Tung Education Foundation (131015) and the Fundamental Research Funds for the Central Universities (2014XZZX003-02). The authors are grateful to the King Abdullah University of Science and Technology (KAUST) in Saudi Arabia for providing the characterization of the in situ HRTEM.en
dc.publisherAmerican Chemical Society (ACS)en
dc.relation.urlhttp://pubs.acs.org/doi/abs/10.1021/jacs.7b05476en
dc.rightsThis document is the Accepted Manuscript version of a Published Work that appeared in final form in Journal of the American Chemical Society, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see http://pubs.acs.org/doi/abs/10.1021/jacs.7b05476.en
dc.titleCatalytic Activity Control via Crossover between Two Different Microstructuresen
dc.typeArticleen
dc.contributor.departmentKing Abdullah University of Science and Technology, Thuwal, 999088, Kingdom of Saudi Arabia.en
dc.identifier.journalJournal of the American Chemical Societyen
dc.eprint.versionPost-printen
dc.contributor.institutionKey Lab of Applied Chemistry of Zhejiang Province, Department of Chemistry, Zhejiang University, Hangzhou, 310027, China.en
dc.contributor.institutionKey Laboratory for Advanced Materials, Centre for Computational Chemistry and Research Institute of Industrial Catalysis, East China University of Science and Technology, Shanghai, China.en
kaust.authorZhu, Yihanen
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