Preparation of bifunctional Au-Pd/TiO2 catalysts and research on methanol liquid phase one-step oxidation to methyl formate

被引：15

作者：

Shi, Da ^{[1
,2
,3
]}

Liu, Jianfang ^{[1
]}

Sun, Rui ^{[1
]}

Ji, Shengfu ^{[1
]}

Rogers, Scott M. ^{[2
,4
]}

Connolly, Bethany M. ^{[3
]}

Dimitratos, Nikolaos ^{[2
,5
]}

Wheatley, Andrew E. H. ^{[3
]}

机构：

[1] Beijing Univ Chem Technol, State Key Lab Chem Resource Engn, Beijing 100029, Peoples R China

[2] Rutherford Appleton Lab, UK Catalysis Hub, Res Complex Harwell, Didcot OX11 0FA, Oxon, England

[3] Univ Cambridge, Dept Chem, Lensfield Rd, Cambridge CB2 1EW, England

[4] UCL, Dept Chem, 20 Gordon St, London WC1H 0AJ, England

[5] Cardiff Univ, Sch Chem, Cardiff Catalysis Inst, Cardiff CF10 3AT, S Glam, Wales

来源：

CATALYSIS TODAY | 2018年 / 316卷

基金：

英国工程与自然科学研究理事会; 中国国家自然科学基金;

关键词：

Au-Pd/TiO2; Bifunctional catalysts; Liquid methanol; One-step catalytic transformation; Methyl formate; AUPD BIMETALLIC NANOPARTICLES; SOLVENT-FREE OXIDATION; SELECTIVE OXIDATION; CO OXIDATION; FORMIC-ACID; PD; REDUCTION; TIO2; HYDROGENATION; TEMPERATURE;

D O I：

10.1016/j.cattod.2018.01.033

中图分类号：

O69 [应用化学];

学科分类号：

081704 ;

摘要：

A series of Au-Pd/TiO2 bifunctional catalysts with different Au, Pd loading percents have been prepared by solimmobilization method. The related XRD, HR-TEM and XPS characterizations have been undertaken to uderstand the structure of catalysts. Catalytic activity in methanol liquid phase one-step oxidation to methyl formate have been studied in batch reactor. Results show that the nanoparticles are highly dispersed on TiO2 with 6.4 nm mean size. Also, bifunctional catalysts could catalyse the conversion of methanol to methyl formate with high efficiency. With 1wt% Au-1wt% Pd/TiO2 catalysts, when the molar ratio between active components and methanol is 1/2000, the conversion of methanol is 55.7% for 4 h under 100 degrees C and 25 bar. At the same time, the selectivity of methyl formate is up to 74.2%. The Au-Pd/TiO2 bifunctional catalysts also shows great stability for the reaction with stable conversion and selectivity after 5 cycles.

引用

页码：206 / 213

页数：8

共 35 条

[1] Oxidation of Methane to Methanol with Hydrogen Peroxide Using Supported Gold-Palladium Alloy Nanoparticles [J].

Ab Rahim, Mohd Hasbi ;

Forde, Michael M. ;

Jenkins, Robert L. ;

Hammond, Ceri ;

He, Qian ;

Dimitratos, Nikolaos ;

Lopez-Sanchez, Jose Antonio ;

Carley, Albert F. ;

Taylor, Stuart H. ;

Willock, David J. ;

Murphy, Damien M. ;

Kiely, Christopher J. ;

Hutchings, Graham J. .

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2013, 52 (04) :1280-1284

[2] Aqueous Au-Pd colloids catalyze selective CH4 oxidation to CH3OH with O2 under mild conditions [J].

Agarwal, Nishtha ;

Freakley, Simon J. ;

McVicker, Rebecca U. ;

Althahban, Sultan M. ;

Dimitratos, Nikolaos ;

He, Qian ;

Morgan, David J. ;

Jenkins, Robert L. ;

Willock, David J. ;

Taylor, Stuart H. ;

Kiely, Christopher J. ;

Hutchings, Graham J. .

SCIENCE, 2017, 358 (6360) :223-226

[3] Photoinduced oxygen release and persistent photoconductivity in ZnO nanowires [J].

Bao, Jiming ;

Shalish, Ilan ;

Su, Zhihua ;

Gurwitz, Ron ;

Capasso, Federico ;

Wang, Xiaowei ;

Ren, Zhifeng .

NANOSCALE RESEARCH LETTERS, 2011, 6 :1-7

[4] The use of pure methanol as fuel at high compression ratio in a single cylinder gasoline engine [J].

Celik, M. Bahattin ;

Ozdalyan, Bulent ;

Alkan, Faruk .

FUEL, 2011, 90 (04) :1591-1598

[5] Methanol conversion to light olefins over SAPO-34: Reaction network and deactivation kinetics [J].

Chen, D. ;

Grlnvold, A. ;

Moljord, K. ;

Holmen, A. .

INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 2007, 46 (12) :4116-4123

[6] XPS study of the surface chemical state of a Pd/(SiO2+TiO2) catalyst after methane oxidation and SO2 treatment [J].

Chenakin, S. P. ;

Melaet, G. ;

Szukiewicz, R. ;

Kruse, N. .

JOURNAL OF CATALYSIS, 2014, 312 :1-11

[7] The effect of calcination temperature on structure and photocatalytic properties of Au/Pd nanoparticles supported on TiO2 [J].

Cybula, Anna ;

Priebe, Jacqueline B. ;

Pohl, Marga-Martina ;

Sobczak, Janusz W. ;

Schneider, Matthias ;

Zielhiska-Jurek, Anna ;

Brueckner, Angelika ;

Zaleska, Adriana .

APPLIED CATALYSIS B-ENVIRONMENTAL, 2014, 152 :202-211

[8] Au, Pd (mono and bimetallic) catalysts supported on graphite using the immobilisation method - Synthesis and catalytic testing for liquid phase oxidation of glycerol [J].

Dimitratos, N ;

Porta, F ;

Prati, L .

APPLIED CATALYSIS A-GENERAL, 2005, 291 (1-2) :210-214

[9] Solvent-free oxidation of primary alcohols to aldehydes using Au-Pd/TiO2 catalysts [J].

Enache, DI ;

Edwards, JK ;

Landon, P ;

Solsona-Espriu, B ;

Carley, AF ;

Herzing, AA ;

Watanabe, M ;

Kiely, CJ ;

Knight, DW ;

Hutchings, GJ .

SCIENCE, 2006, 311 (5759) :362-365

[10] Synthesis and electrocatalytic activity of Au@Pd core-shell nanothorns for the oxygen reduction reaction [J].

Fu, Gengtao ;

Liu, Zhenyuan ;

Chen, Yu ;

Lin, Jun ;

Tang, Yawen ;

Lu, Tianhong .

NANO RESEARCH, 2014, 7 (08) :1205-1214

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