Structure-Property Relationships of Pt-Sn Nanoparticles Supported on Al2O3 for the Dehydrogenation of Methylcyclohexane

被引：48
作者：
Murata, Kazumasa [1 ]
Kurimoto, Natsuki [1 ]
Yamamoto, Yuta [2 ]
Oda, Akira [1 ,3 ]
Ohyama, Junya [3 ,4 ]
Satsuma, Atsushi [1 ,3 ]
机构：
[1] Nagoya Univ, Grad Sch Engn, Nagoya, Aichi 4648603, Japan
[2] Nagoya Univ, Inst Mat & Syst Sustainabil, Nagoya, Aichi 4648603, Japan
[3] Kyoto Univ, Elements Strategy Initiat Catalysts & Batteries E, Kyoto 6158520, Japan
[4] Kumamoto Univ, Fac Adv Sci & Technol, Kumamoto 8608555, Japan
来源：
ACS APPLIED NANO MATERIALS | 2021年 / 4卷 / 05期
关键词：
Pt-Sn catalyst; dehydrogenation; methylcyclohexane; nanoparticle; alloy; local structure; WATER-GAS SHIFT; PROPANE DEHYDROGENATION; CATALYTIC-PROPERTIES; PARTICLE-SIZE; CO OXIDATION; HYDROGEN GENERATION; PLATINUM CATALYSTS; FTIR SPECTROSCOPY; CLUSTERS; CYCLOHEXANE;
D O I：
10.1021/acsanm.1c00128
中图分类号：
TB3 [工程材料学];
学科分类号：
0805 ; 080502 ;
摘要：
The structure-catalytic property relationships of Al2O3-supported Pt-Sn nanoparticles (Pt-Sn/Al2O3) in the dehydrogenation of methylcyclohexane (MCH) were investigated by varying the Sn/Pt ratios of the catalysts. The initial activity and the deactivation rate of the Pt-Sn/Al2O3 catalysts in the MCH dehydrogenation decreased in line with an increase in the Sn/Pt ratio from 0 to 3. The Pt-Sn/Al2O3 catalyst with a Sn/Pt ratio of 2 showed good activity, durability, and toluene selectivity in the MCH dehydrogenation among the series of catalysts. The dispersion of Pt in the Pt-Sn/Al2O3 catalysts was observed to decrease with an increase in the Sn/Pt ratio. Structural changes in the catalysts from Pt-Sn clusters to intermetallic Pt3Sn and PtSn nanoparticles were also observed using scanning transmission electron microscopy and X-ray diffraction. According to structural analysis using X-ray absorption fine-structure spectroscopy and infrared spectroscopy using carbon monoxide as a probe, the electron density of Pt increased, and the fraction of Pt-Pt adjacent sites decreased with an increase in the Sn/Pt ratio. Comparing the catalytic properties and the structures of the Pt-Sn/Al2O3 catalysts, their initial activities were correlated with the dispersion of Pt. In addition, the durability and selectivity of the catalysts were enhanced due to an increase in the electron density of Pt and a decrease in the number of Pt-Pt adjacent sites. Overall, the properties of the catalysts in the MCH dehydrogenation are determined by the local structure of Pt atoms rather than the crystal structure of the Pt-Sn alloy nanoparticles on Al2O3.
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收藏
页码：4532 / 4541
页数：10
相关论文
共 58 条
[1]   Kinetics on NiZn Bimetallic Catalysts for Hydrogen Evolution via Selective Dehydrogenation of Methylcyclohexane to Toluene [J].
Al-ShaikhAli, Anaam H. ;
Jedid, Abdesslem ;
Anjum, Dalaver H. ;
Cavallo, Luigi ;
Takanabe, Kazuhiro .
ACS CATALYSIS, 2017, 7 (03) :1592-1600
[2]   THE [PTCL2(SNCL3)2]2-ION - CRYSTAL-STRUCTURE OF 2 SALTS [J].
ALCOCK, NW ;
NELSON, JH .
JOURNAL OF THE CHEMICAL SOCIETY-DALTON TRANSACTIONS, 1982, (12) :2415-2418
[3]   FTIR STUDY OF BIMETALLIC PT-SN/AL2O3 CATALYSTS [J].
BALAKRISHNAN, K ;
SCHWANK, J .
JOURNAL OF CATALYSIS, 1992, 138 (02) :491-499
[4]   Effect of the Pt Precursor and Loading on the Structural Parameters and Catalytic Properties of Pt/Al2O3 [J].
Borges, Lais R. ;
Lopez-Castillo, Alejandro ;
Meira, Debora M. ;
Gallo, Jean Marcel R. ;
Zanchet, Daniela ;
Bueno, Jose Maria C. .
CHEMCATCHEM, 2019, 11 (13) :3064-3074
[5]   Interference phenomena in the EXAFS spectra of Pt-Sn bimetallic catalysts [J].
Borgna, A ;
Stagg, SM ;
Resasco, DE .
JOURNAL OF PHYSICAL CHEMISTRY B, 1998, 102 (26) :5077-5081
[6]  
Boudart M., 1969, ADV CATAL, V20, P153, DOI DOI 10.1016/S0360-0564(08)60271-0
[7]   IN-SITU X-RAY-ABSORPTION SPECTROSCOPIC STUDY OF A HIGHLY DISPERSED PTSN/AL2O3 CATALYST [J].
CABALLERO, A ;
DEXPERT, H ;
DIDILLON, B ;
LEPELTIER, F ;
CLAUSE, O ;
LYNCH, J .
JOURNAL OF PHYSICAL CHEMISTRY, 1993, 97 (43) :11283-11285
[8]   Identification of Active Sites on High-Performance Pt/Al2O3 Catalyst for Cryogenic CO Oxidation [J].
Chen, Yang ;
Feng, Yingxin ;
Li, Lin ;
Liu, Jingyue ;
Pan, Xiaoli ;
Liu, Wei ;
Wei, Fenfei ;
Cui, Yitao ;
Qiao, Botao ;
Sun, Xiucheng ;
Li, Xiaoyu ;
Lin, Jian ;
Lin, Sen ;
Wang, Xiaodong ;
Zhang, Tao .
ACS CATALYSIS, 2020, 10 (15) :8815-8824
[9]   CHEMISORPTION AND CATALYTIC PROPERTIES OF SUPPORTED PLATINUM [J].
CUSUMANO, JA ;
DEMBINSKI, GW ;
SINFELT, JH .
JOURNAL OF CATALYSIS, 1966, 5 (03) :471-+
[10]   Characterization of mono- and bi-metallic platinum catalysts using CO FTIR spectroscopy - Size effects and topological segregation [J].
deMenorval, LC ;
Chaqroune, A ;
Coq, B ;
Figueras, F .
JOURNAL OF THE CHEMICAL SOCIETY-FARADAY TRANSACTIONS, 1997, 93 (20) :3715-3720
123456