TY - JOUR
T1 - MXene (Ti 3 C 2 ) Vacancy-Confined Single-Atom Catalyst for Efficient Functionalization of CO 2
AU - Zhao, Di
AU - Chen, Zheng
AU - Yang, Wenjuan
AU - Liu, Shoujie
AU - Zhang, Xun
AU - Yu, Yi
AU - Cheong, Weng Chon
AU - Zheng, Lirong
AU - Ren, Fuqiang
AU - Ying, Guobing
AU - Cao, Xing
AU - Wang, Dingsheng
AU - Peng, Qing
AU - Wang, Guoxiu
AU - Chen, Chen
N1 - Publisher Copyright:
© Copyright 2019 American Chemical Society.
PY - 2019/3/6
Y1 - 2019/3/6
N2 - 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 Ti 3-x C 2 T y support and are therefore stabilized onto the sites previously occupied by Ti. Pt-based single-atom catalyst (SAC) Pt 1 /Ti 3-x C 2 T y offers a green route to utilizing greenhouse gas CO 2 , 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 Ti 3-x C 2 T y support feature partial positive charges and atomic dispersion, which helps to significantly decrease the adsorption energy and activation energy of silane, CO 2 , 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.
AB - 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 Ti 3-x C 2 T y support and are therefore stabilized onto the sites previously occupied by Ti. Pt-based single-atom catalyst (SAC) Pt 1 /Ti 3-x C 2 T y offers a green route to utilizing greenhouse gas CO 2 , 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 Ti 3-x C 2 T y support feature partial positive charges and atomic dispersion, which helps to significantly decrease the adsorption energy and activation energy of silane, CO 2 , 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.
UR - http://www.scopus.com/inward/record.url?scp=85061911675&partnerID=8YFLogxK
U2 - 10.1021/jacs.8b13579
DO - 10.1021/jacs.8b13579
M3 - Article
C2 - 30699294
AN - SCOPUS:85061911675
SN - 0002-7863
VL - 141
SP - 4086
EP - 4093
JO - Journal of the American Chemical Society
JF - Journal of the American Chemical Society
IS - 9
ER -