TY - JOUR
T1 - Small-Molecule Modification Provides Pt Nucleation Sites for Enhanced Propane Dehydrogenation Performance
AU - Zhang, Bianqin
AU - Wu, Zhiwei
AU - Xing, Shuangfeng
AU - Zhang, Jianyuan
AU - Zhao, Shichao
AU - Xiong, Mi
AU - Luo, Jing
AU - Qin, Yong
AU - Gao, Zhe
N1 - Publisher Copyright:
© 2023 American Chemical Society.
PY - 2023/3/30
Y1 - 2023/3/30
N2 - The rational synthesis of catalysts with controllable structures and the study of their structure-activity relationships to break the limitations of traditional catalysts remain challenging. Herein, tetrakis(dimethylamido)tin (TDMASn) exposures were used to modify silicalite-1 (S-1) lacking suitable chemisorption sites on their surfaces to provide Pt nucleation sites, obtaining a Pt/20TDMASn/S-1 sample. For comparison, Pt species supported on bare S-1 (Pt/S-1) and Pt species supported on the S-1 of pre-deposited SnO2 (Pt/20SnO2/S-1) were also prepared. Catalysts were characterized extensively by X-ray diffraction, temperature-programmed reduction, transmission electron microscopy, X-ray photoelectron spectroscopy, and diffuse-reflectance infrared Fourier transform spectroscopy of adsorbed CO. The results showed that this surface modification (TDMASn or SnO2) yielded up to about a 40-times increase in Pt content after 20 cycles of Pt atomic layer deposition (ALD). Compared with Pt/20SnO2/S-1, Pt/20TDMASn/S-1 had a smaller particle size, stronger interactions between the metal species and the support, and a lower Sn0 content, thus resulting in a remarkably higher initial propane conversion in the propane dehydrogenation (PDH) reaction. The catalytic activity could also be optimized based on the number of ALD-TDMASn exposures. As a consequence, Sn not only provided nucleation sites for Pt but also acted as a promoter to enhance the catalyst performance. This fundamental understanding will help researchers obtain suitable catalysts for PDH processes.
AB - The rational synthesis of catalysts with controllable structures and the study of their structure-activity relationships to break the limitations of traditional catalysts remain challenging. Herein, tetrakis(dimethylamido)tin (TDMASn) exposures were used to modify silicalite-1 (S-1) lacking suitable chemisorption sites on their surfaces to provide Pt nucleation sites, obtaining a Pt/20TDMASn/S-1 sample. For comparison, Pt species supported on bare S-1 (Pt/S-1) and Pt species supported on the S-1 of pre-deposited SnO2 (Pt/20SnO2/S-1) were also prepared. Catalysts were characterized extensively by X-ray diffraction, temperature-programmed reduction, transmission electron microscopy, X-ray photoelectron spectroscopy, and diffuse-reflectance infrared Fourier transform spectroscopy of adsorbed CO. The results showed that this surface modification (TDMASn or SnO2) yielded up to about a 40-times increase in Pt content after 20 cycles of Pt atomic layer deposition (ALD). Compared with Pt/20SnO2/S-1, Pt/20TDMASn/S-1 had a smaller particle size, stronger interactions between the metal species and the support, and a lower Sn0 content, thus resulting in a remarkably higher initial propane conversion in the propane dehydrogenation (PDH) reaction. The catalytic activity could also be optimized based on the number of ALD-TDMASn exposures. As a consequence, Sn not only provided nucleation sites for Pt but also acted as a promoter to enhance the catalyst performance. This fundamental understanding will help researchers obtain suitable catalysts for PDH processes.
UR - https://www.scopus.com/pages/publications/85150442138
U2 - 10.1021/acs.jpcc.3c00013
DO - 10.1021/acs.jpcc.3c00013
M3 - 文章
AN - SCOPUS:85150442138
SN - 1932-7447
VL - 127
SP - 5754
EP - 5762
JO - Journal of Physical Chemistry C
JF - Journal of Physical Chemistry C
IS - 12
ER -