Preparation and Catalytic Performance of the Confined Pt Catalyst by Atomic Layer Deposition

doi:10.19894/j.issn.1000-0518.230346

Chinese Journal of Applied Chemistry ›› 2024, Vol. 41 ›› Issue (4): 547-556.DOI: 10.19894/j.issn.1000-0518.230346

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Preparation and Catalytic Performance of the Confined Pt Catalyst by Atomic Layer Deposition

Mei-Hua WANG¹, Yu FENG¹, Yun-Kun WANG¹, Xu-Dong ZHAO¹, Wen YANG¹(), Chuan DONG²()

^1.Instrumental Analysis Center，School of Material Science and Engineering，Taiyuan University of Science and Technology，Taiyuan 030024，China
^2.Institute of Environmental Science，Shanxi University，Taiyuan 030006，China

Received:2023-11-06 Accepted:2024-02-20 Published:2024-04-01 Online:2024-04-28
Contact: Wen YANG,Chuan DONG
About author:dc@sxu.edu.cn
yangwen@tyust.edu.cn；
Supported by:
Shanxi Province Science and Technology Innovation Talent Team Special Project(202204051001002);Shanxi Province Basic Research Program Funding Project(20210302124471);the National Natural Science Foundation of China(22208230);Shanxi Provincial Excellent Support Program for Returned Overseas Scholars(20230033)

Abstract

Abstract:

It is of great significance to select appropriate supports to support Pt nanoparticles for the preparation of efficient phenol hydrogenation catalysts. In this paper， Pt nanoparticles confined into the inner wall of titanium oxide nanotubes were prepared by template assisted method of atomic layer deposition technology. The specific preparation method was to use carbon nanofibers as templates， successively depositing Pt nanoparticles and thick titanium oxide shell on the templates surface. Then， the templates were removed by high-temperature sintering， through which Pt nanoparticles confined into the inner wall of titanium oxide nanotubes can be obtained. The particle size of the Pt nanoparticles ranged from 2.0 to 3.2 nm at a sintering temperature of 500 ℃， with an average size of 2.6 nm. Transmission electron microscopy results confirmed that Pt nanoparticles with highly uniform size were evenly dispersed and embedded into the inner wall of the hollow channel of titanium oxide nanotubes. The results of the catalytic performance of phenol hydrogenation show that the small-size Pt nanoparticles have the best phenol hydrogenation activity， with a Turnover Frequency （TOF） value of 482.1 h^-1 at a sintering temperature of 500 ℃. In addition， compared with the conventional Pt nanoparticles with the same size supported on the outer wall of titanium oxide nanotubes， it is found that the confined catalyst shows better catalytic activity. Furthermore， due to the protective effect of titanium oxide nanotubes， it can effectively prevent the aggregation and falling off of Pt nanoparticles in the reaction process. After the reaction， the Pt content only decreased by 4.52%， and there were no significant changes in the morphology observed， thus the confined catalyst showing excellent catalytic stability compared with the supported catalyst.

Key words: Atomic layer deposition, Confined catalyst, Pt catalyst, Phenol hydrogenation

CLC Number:

O643.3

Mei-Hua WANG, Yu FENG, Yun-Kun WANG, Xu-Dong ZHAO, Wen YANG, Chuan DONG. Preparation and Catalytic Performance of the Confined Pt Catalyst by Atomic Layer Deposition[J]. Chinese Journal of Applied Chemistry, 2024, 41(4): 547-556.

Figures/Tables 9

Fig.1 The schematic diagram of the preparation process of the confined Pt catalyst

Fig.2 TEM images of （A） TiO2 nanotubes and （B） Pt nanoparticles in TiO2 nanotubes. High resolution transmission electron microscopy of Pt nanoparticles （C， D）. The STEM （E） and Mapping element diagram of Pt nanoparticles in TiO2 nanotubes， representing O （G）， Pt （H）， Ti （I） and their overlap （F）

Fig.3 TEM images of Pt nanoparticles in TiO2 nanotubes sintered at （A） 550，（B） 530 and （C） 500 ℃ and size distribution of corresponding Pt nanoparticles （D， E， F）

Fig.4 Time dependence of catalytic activity of the prepared catalysts for phenol hydrogenation

Table 1 Catalytic performance of these samples for the hydrogenation of phenol

Sample	w（ Pt）/% ^a	Conversion/% ^b	Selectivity/% ^c	TOF/h^-1^d
TNT@Pt	2.55	46.2	98.7	281.5
Pt@TNT（500 ℃）	2.44	75.1	97.0	482.1
Pt@TNT（530 ℃） Pt@TNT（550 ℃） Pt@TNT4^th	2.36 2.49 2.33	56.8 39.9 70.3	97.2 96.8 98.5	377.1 249.9 472.7
TNT@Pt4^th	1.01	10.3	94.3	159.1

Fig.5 （A） The recycling stability of phenol hydrogenation for the catalysts （the reaction time is 1 h per run for both catalysts）；（B） The comparison of TOF values of phenol hydrogenation

Fig.6 TEM images of （A） Pt@TNT after reaction，（B） TNT@Pt before， after reaction （C） and size distribution of corresponding Pt nanoparticles （D， E， F）

Fig.7 Pt4f （A） and Ti2p （B） XPS spectra of Pt@TNT and TNT@Pt catalysts

Fig.8 The schematic diagram of the structure models and TEM images of Pt-TiO2 interfaces of Pt@TNT （A， B） and TNT@Pt （C，D） catalysts.

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Preparation and Catalytic Performance of the Confined Pt Catalyst by Atomic Layer Deposition

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