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Title: Al-doped TiO{sub 2} mesoporous material supported Pd with enhanced catalytic activity for complete oxidation of ethanol

Abstract

Pd catalysts supported on Al-doped TiO{sub 2} mesoporous materials were evaluated in complete oxidation of ethanol. The catalysts synthesized by wet impregnation based on evaporation-induced self-assembly were characterized by X-ray diffraction, measurement of pore structure, XPS, FT-IR, temperature programmed reduction and TEM. Characteristic results showed that the aluminium was doped into the lattice of mesoporous anatase TiO{sub 2} to form Al-O-Ti defect structure. Catalytic results revealed that Al-doped catalysts were much more active than the pristine one, especially at low temperature (≤200 °C). This should be ascribed to the introduction of aluminium ions that suppressed the strong metal-support interaction and increased the active sites of Pd oxides, enhanced the stabilized anatase TiO{sub 2}, improved well dispersed high valence palladium species with high reducibility and enriched chemisorption oxygen. - Graphical abstract: Al-doped Pd/TiO{sub 2} exhibited optimal catalytic performance for ethanol oxidation and CO{sub 2} yield by the suppression of SMSI. - Highlights: • Palladium catalysts supported on Al-doped TiO{sub 2} mesoporous materials were studied. • The introduction of Al can enhance anatase stabilization and increase defect TiO{sub 2}. • The Pd/Al-TiO{sub 2} catalysts show higher ethanol conversion and CO{sub 2} yield than Pd/TiO{sub 2}. • The influence of Al on SMSImore » and catalytic performance were evaluated by TPR and XPS.« less

Authors:
; ; ; ; ; ;
Publication Date:
OSTI Identifier:
22658247
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of Solid State Chemistry; Journal Volume: 248; Other Information: Copyright (c) 2017 Elsevier Science B.V., Amsterdam, The Netherlands, All rights reserved.; Country of input: International Atomic Energy Agency (IAEA)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; 77 NANOSCIENCE AND NANOTECHNOLOGY; ALUMINIUM IONS; CARBON DIOXIDE; CATALYSTS; DOPED MATERIALS; ETHANOL; EXPERIMENTAL DATA; FOURIER TRANSFORMATION; INFRARED SPECTRA; NANOSTRUCTURES; OXIDATION; PORE STRUCTURE; TEMPERATURE RANGE 0065-0273 K; TITANIUM OXIDES; X-RAY DIFFRACTION; X-RAY PHOTOELECTRON SPECTROSCOPY

Citation Formats

Zhu, Jing, E-mail: mlczjsls123@163.com, Mu, Wentao, E-mail: mwt15035687833@163.com, Su, Liqing, E-mail: suliqing0163@163.com, Li, Xingying, E-mail: lixingying0479@link.tyut.edu.cn, Guo, Yuyu, E-mail: guoyuyu0455@link.tyut.edu.cn, Zhang, Shen, E-mail: zhangshen0472@link.tyut.edu.cn, and Li, Zhe, E-mail: lizhe@tyut.edu.cn. Al-doped TiO{sub 2} mesoporous material supported Pd with enhanced catalytic activity for complete oxidation of ethanol. United States: N. p., 2017. Web. doi:10.1016/J.JSSC.2017.01.028.
Zhu, Jing, E-mail: mlczjsls123@163.com, Mu, Wentao, E-mail: mwt15035687833@163.com, Su, Liqing, E-mail: suliqing0163@163.com, Li, Xingying, E-mail: lixingying0479@link.tyut.edu.cn, Guo, Yuyu, E-mail: guoyuyu0455@link.tyut.edu.cn, Zhang, Shen, E-mail: zhangshen0472@link.tyut.edu.cn, & Li, Zhe, E-mail: lizhe@tyut.edu.cn. Al-doped TiO{sub 2} mesoporous material supported Pd with enhanced catalytic activity for complete oxidation of ethanol. United States. doi:10.1016/J.JSSC.2017.01.028.
Zhu, Jing, E-mail: mlczjsls123@163.com, Mu, Wentao, E-mail: mwt15035687833@163.com, Su, Liqing, E-mail: suliqing0163@163.com, Li, Xingying, E-mail: lixingying0479@link.tyut.edu.cn, Guo, Yuyu, E-mail: guoyuyu0455@link.tyut.edu.cn, Zhang, Shen, E-mail: zhangshen0472@link.tyut.edu.cn, and Li, Zhe, E-mail: lizhe@tyut.edu.cn. Sat . "Al-doped TiO{sub 2} mesoporous material supported Pd with enhanced catalytic activity for complete oxidation of ethanol". United States. doi:10.1016/J.JSSC.2017.01.028.
@article{osti_22658247,
title = {Al-doped TiO{sub 2} mesoporous material supported Pd with enhanced catalytic activity for complete oxidation of ethanol},
author = {Zhu, Jing, E-mail: mlczjsls123@163.com and Mu, Wentao, E-mail: mwt15035687833@163.com and Su, Liqing, E-mail: suliqing0163@163.com and Li, Xingying, E-mail: lixingying0479@link.tyut.edu.cn and Guo, Yuyu, E-mail: guoyuyu0455@link.tyut.edu.cn and Zhang, Shen, E-mail: zhangshen0472@link.tyut.edu.cn and Li, Zhe, E-mail: lizhe@tyut.edu.cn},
abstractNote = {Pd catalysts supported on Al-doped TiO{sub 2} mesoporous materials were evaluated in complete oxidation of ethanol. The catalysts synthesized by wet impregnation based on evaporation-induced self-assembly were characterized by X-ray diffraction, measurement of pore structure, XPS, FT-IR, temperature programmed reduction and TEM. Characteristic results showed that the aluminium was doped into the lattice of mesoporous anatase TiO{sub 2} to form Al-O-Ti defect structure. Catalytic results revealed that Al-doped catalysts were much more active than the pristine one, especially at low temperature (≤200 °C). This should be ascribed to the introduction of aluminium ions that suppressed the strong metal-support interaction and increased the active sites of Pd oxides, enhanced the stabilized anatase TiO{sub 2}, improved well dispersed high valence palladium species with high reducibility and enriched chemisorption oxygen. - Graphical abstract: Al-doped Pd/TiO{sub 2} exhibited optimal catalytic performance for ethanol oxidation and CO{sub 2} yield by the suppression of SMSI. - Highlights: • Palladium catalysts supported on Al-doped TiO{sub 2} mesoporous materials were studied. • The introduction of Al can enhance anatase stabilization and increase defect TiO{sub 2}. • The Pd/Al-TiO{sub 2} catalysts show higher ethanol conversion and CO{sub 2} yield than Pd/TiO{sub 2}. • The influence of Al on SMSI and catalytic performance were evaluated by TPR and XPS.},
doi = {10.1016/J.JSSC.2017.01.028},
journal = {Journal of Solid State Chemistry},
number = ,
volume = 248,
place = {United States},
year = {Sat Apr 15 00:00:00 EDT 2017},
month = {Sat Apr 15 00:00:00 EDT 2017}
}
  • This paper studies the mechanism of low temperature CO oxidation over catalysts of 0.003%-0.1 wt.% palladium supported on gamma-Al/sub 2/O/sub 3/, and over a solid solution of copper in gamma-Al/sub 2/O/sub 3/ (0.5-3.0 wt.% CuO). In order to obtain information about the reactive forms of oxygen in CO oxidation over these catalysts, the authors used tagged oxygen (ca 80 atom %) and secondary ion mass spectrometry. To confirm the effect of oxygen isotope exchange on the tracer content of the CO/sub 2/, CO oxidation was carried out with CO/sub 2/ freeze-out in the cycle. CO oxidation over supported palladium, undermore » conditions of reduction or of catalysis, can go via reaction with OH oxygen atoms, but the temperature ranges of these conditions differ by more than 250 degrees. It is noted that over Pd.Cu/Al/sub 2/O/sub 3/ catalysts the mechanism represented is only partly realized. Along with OH oxygen, an adsorbed form of oxygen evidently also contributes to CO formation over these catalysts.« less
  • The oxidation of methanol has been studied over TiO/sub 2/ doped with Al in the nominal range x = 0 ..-->.. 0.1 for Ti/sub 1-x/Al/sub x/O/sub 2/. At a reference temperature of 490 K all the catalysts except TiO/sub 2/ were 99% selective in HCHO. Initial additions of Al to x = 0.001 resulted in 100-fold increase in activity relative to TiO/sub 2/. This has been attributed to the effect of Al in generating new Lewis acid sites, AL/sup 3 +/ and Ti/sup 3 +/, and subsequently varying sensitivity with Al concentration. These variations are discussed with reference to themore » effect of Al/sup 3 +/ in promoting the formation of Ti/sup 3 +/, and hence its influence on the electronic interaction between the new active sites.« less
  • Pt-Mo bimetallic ensembles active for ethene hydrogenation and ethane hydrogenolysis were prepared on silica and alumina using a new Anderson-type plane [PtMo[sub 6]O[sub 24]][sup 8 [minus]] heteropolyanion as a precursor. The structures of the supported bimetallic ensembles were determined by H[sub 2 [minus]]chemisorption, TEM (transmission electron microscopy), analytical TEM, XRD (X-ray diffraction), EXAFS (extended X-ray absorption fine structure), and XANES (X-ray absorption near edge structure). The heteropolyanion framework was maintained when it was supported on silica, but was broken when on alumina. After reduction at 773-823 K, dispersed particles with an eggshell structure (3.0 [plus minus] 0.5 nm) were formedmore » on silica, where a small platinum cluster (ca. 1.0 nm) located in the center was covered with partially oxidized Mo-oxide layers. On alumina bimetallic clusters of 2.0 [plus minus] 0.5 nm were formed, and part of the molybdenum atoms were dispersed in low valence states on the Al[sub 2]O[sub 3] surface.« less
  • When using the TiO 2(110)-supported Pd7 cluster as a model catalyst, we identified the dynamics of supported metal nanoparticles using density functional theory calculations, at the sub-nanometer scale and under reactive environments. Increasing the CO coverage can induce a structural transformation from Pd 7-3D/TiO 2(110) at low coverage to Pd 7-2D/TiO 2(110) at the saturation coverage wherein CO saturation-driven Pd7-2D/TiO 2(110) structure displays superior CO oxidation activity at the interfacial sites, which are highly active for catalyzing O 2 dissociation and CO oxidation via bifunctional synergy.
  • The reactivity of ternary V{sub 2}O{sub 5}-WO{sub 3}/TiO{sub 2}de-NO{sub x} catalysts (V{sub 2}O{sub 5} = 0--1.47% w/w, WO{sub 3} = 0--9% w/w) in the selective catalytic reduction (SCR) reaction is investigated under steady-state and transient conditions. The results indicate that over the investigated catalysts the SCR reaction occurs via a redox mechanism and that the rate-determining step of the reaction is the catalyst reoxidation process. The reactivity of the V{sub 2}O{sub 5}-WO{sub 3}/TiO{sub 2} catalysts increases on increasing either the V{sup 2}O{sub 5} or the WO{sub 3} loading; the reactivity of V and/or W in the ternary catalysts is highermore » than that of the corresponding binary samples. A synergism between the TiO{sub 2}-supported V and W surface oxide species in the SCR reaction is suggested, that is exploited in the enhancement of the catalyst redox properties of the samples. Accordingly, tungsta increases the rate of the SCR reaction of V{sub 2}O{sub 5}/TiO{sub 2} catalysts by favoring the catalyst reoxidation y gas-phase oxygen.« less