CAS OpenIR
MXene (Ti3C2) Vacancy-Confined Single-Atom Catalyst for Efficient Functionalization of CO2
Zhao, Di1; Chen, Zheng1; Yang, Wenjuan1; Liu, Shoujie1,2; Zhang, Xun3; Yu, Yi3; Cheong, Weng-Chon1; Zheng, Lirong4; Ren, Fuqiang5; Ying, Guobing6; Cao, Xing1; Wang, Dingsheng1; Peng, Qing1; Wang, Guoxiu7; Chen, Chen1
2019-03-06
Source PublicationJOURNAL OF THE AMERICAN CHEMICAL SOCIETY
ISSN0002-7863
Volume141Issue:9Pages:4086-4093
Abstract

A central topic in single-atom catalysis is building strong interactions between single atoms and the support for stabilization. Herein we report the preparation of stabilized single-atom catalysts via a simultaneous self-reduction stabilization process at room temperature using ultrathin two-dimensional Ti(3-x)C(2)T(y)MXene nanosheets characterized by abundant Ti-deficit vacancy defects and a high reducing capability. The single atoms therein form strong metal-carbon bonds with the Ti3-xC2Ty support and are therefore stabilized onto the sites previously occupied by Ti. Pt-based single-atom catalyst (SAC) Pt-1/Ti3-xC2Ty offers a green route to utilizing greenhouse gas CO2, via the formylation of amines, as a C-1 source in organic synthesis. DFT calculations reveal that, compared to Pt nanoparticles, the single Pt atoms on Ti3-xC2Ty support feature partial positive charges and atomic dispersion, which helps to significantly decrease the adsorption energy and activation energy of silane, CO2, and aniline, thereby boosting catalytic performance. We believe that these results would open up new opportunities for the fabrication of SACs and the applications of MXenes in organic synthesis.

DOI10.1021/jacs.8b13579
Language英语
WOS KeywordReduction ; Capacitance ; Formamides ; Amines
Funding ProjectBeijing Natural Science Foundation[JQ18007] ; National Key R&D Program of China[2017YFA0700101] ; National Key R&D Program of China[2016YFA0202801] ; National Natural Science Foundation of China[21872076] ; National Natural Science Foundation of China[21573119] ; National Natural Science Foundation of China[21590792] ; National Natural Science Foundation of China[51651201] ; National Natural Science Foundation of China[21866032] ; National Natural Science Foundation of China[21805184] ; China Postdoctoral Science Foundation[2018M631445] ; China Postdoctoral Science Foundation[2018M631444] ; China Postdoctoral Science Foundation[2018M631486] ; National Postdoctoral Program for Innovative Talents[BX201700131]
WOS Research AreaChemistry
WOS SubjectChemistry, Multidisciplinary
Funding OrganizationBeijing Natural Science Foundation ; National Key R&D Program of China ; National Natural Science Foundation of China ; China Postdoctoral Science Foundation ; National Postdoctoral Program for Innovative Talents
WOS IDWOS:000460996500047
PublisherAMER CHEMICAL SOC
Citation statistics
Document Type期刊论文
Identifierhttp://ir.ipe.ac.cn/handle/122111/28297
Collection中国科学院过程工程研究所
Corresponding AuthorChen, Chen
Affiliation1.Tsinghua Univ, Dept Chem, Beijing 100084, Peoples R China
2.Anhui Normal Univ, Coll Chem & Mat Sci, Wuhu 241000, Peoples R China
3.Shanghai Tech Univ, Sch Phys Sci & Technol, Shanghai 201210, Peoples R China
4.Chinese Acad Sci, Beijing Synchrotron Radiat Facil, Beijing 100049, Peoples R China
5.Chinese Acad Sci, Inst Proc Engn, Beijing 100190, Peoples R China
6.Hohai Univ, Coll Mech & Mat, Dept Mat Sci & Engn, Nanjing 211100, Jiangsu, Peoples R China
7.Univ Technol Sydney, Fac Sci, Sch Math & Phys Sci, Ctr Clean Energy Technol, Sydney, NSW 2007, Australia
Recommended Citation
GB/T 7714
Zhao, Di,Chen, Zheng,Yang, Wenjuan,et al. MXene (Ti3C2) Vacancy-Confined Single-Atom Catalyst for Efficient Functionalization of CO2[J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,2019,141(9):4086-4093.
APA Zhao, Di.,Chen, Zheng.,Yang, Wenjuan.,Liu, Shoujie.,Zhang, Xun.,...&Chen, Chen.(2019).MXene (Ti3C2) Vacancy-Confined Single-Atom Catalyst for Efficient Functionalization of CO2.JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,141(9),4086-4093.
MLA Zhao, Di,et al."MXene (Ti3C2) Vacancy-Confined Single-Atom Catalyst for Efficient Functionalization of CO2".JOURNAL OF THE AMERICAN CHEMICAL SOCIETY 141.9(2019):4086-4093.
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