Multimetallic catalysts of RuO2-CuO-Cs2O-TiO2/SiO2 for direct gas-phase epoxidation of propylene to propylene oxide

被引:20
作者
Chukeaw, T. [1 ]
Seubsai, A. [1 ,2 ,3 ]
Phon-in, P. [1 ]
Charoen, K. [1 ]
Witoon, T. [1 ]
Donphai, W. [1 ,4 ]
Parpainainar, P. [1 ]
Chareonpanich, M. [1 ,4 ]
Noon, D. [5 ]
Zohour, B. [5 ]
Senkan, S. [5 ]
机构
[1] Kasetsart Univ, Dept Chem Engn, Fac Engn, Bangkok 10900, Thailand
[2] Kasetsart Univ, Ctr Adv Studies Ind Technol, Bangkok 10900, Thailand
[3] Kasetsart Univ, Fac Engn, Bangkok 10900, Thailand
[4] Kasetsart Univ, NANOTEC Ctr Nanoscale Mat Design Green Nanotechno, Bangkok 10900, Thailand
[5] Univ Calif Los Angeles, Dept Chem & Biomol Engn, Los Angeles, CA 90095 USA
关键词
MOLECULAR-OXYGEN; NITROUS-OXIDE; PERFORMANCE; SILICA; COPPER; PROPENE; MECHANISM; OXIDATION; BEHAVIOR; SITES;
D O I
10.1039/c6ra12559j
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
RuO2-CuO/SiO2 catalysts doped with Cs2O and TiO2 were investigated for the direct gas phase epoxidation of propylene to propylene oxide (PO) using molecular oxygen under atmospheric pressure. The optimal catalyst was achieved at Ru/Cu/Cs/Ti = 8.3/4.2/0.6/0.8 by weight and total metal loading of 21 wt% on SiO2 support. NH3 and CO2 temperature programmed desorption measurements of RuO2-CuO/SiO2 catalyst modified with Cs2O showed that the surface's acidity decreased, resulting in enhanced PO selectivity. The addition of TiO2 increased the PO formation rate by promoting the synergy effect between RuO2 and CuO. Using the Box-Behnken design of experiments on the RuO2-CuO-Cs2O-TiO2/SiO2 catalyst, an extraordinarily high optimal PO formation rate of 3015 g(PO) h(-1) kg(cat)(-1) was obtained with a feed comprised of O-2/C3H6 at a volume ratio of 3.1 and (O-2 + C3H6)/He at a volume ratio of 0.26, all at 272 degrees C and 34 cm(3) min(-1). To the knowledge of the authors, this is the highest PO formation rate ever reported for direct propylene epoxidation via O-2.
引用
收藏
页码:56116 / 56126
页数:11
相关论文
共 57 条
[31]   Direct epoxidation of propylene with hydrogen peroxide over TS-1 catalysts: Effect of hydrophobicity of the catalysts [J].
Park, Sunyoung ;
Cho, Kyung Min ;
Youn, Min Hye ;
Seo, Jeong Gil ;
Jung, Ji Chul ;
Baeck, Sung-Hyeon ;
Kim, Tae Jin ;
Chung, Young-Min ;
Oh, Seung-Hoon ;
Song, In Kyu .
CATALYSIS COMMUNICATIONS, 2008, 9 (15) :2485-2488
[32]   Propylene epoxidation with in situ generated H2O2 in supercritical conditions [J].
Prieto, Alejandro ;
Palomino, Miguel ;
Diaz, Urbano ;
Corma, Avelino .
CATALYSIS TODAY, 2014, 227 :87-95
[33]  
Ring K.L., 2016, CHEM EC HDB PROPYLEN
[34]   ELECTRONIC-STRUCTURE OF ANATASE TIO2 OXIDE [J].
SANJINES, R ;
TANG, H ;
BERGER, H ;
GOZZO, F ;
MARGARITONDO, G ;
LEVY, F .
JOURNAL OF APPLIED PHYSICS, 1994, 75 (06) :2945-2951
[35]   Epoxidation of propylene to propylene oxide with molecular oxygen over Sb2O3-CuO-NaCl/SiO2 catalysts [J].
Seubsai, Anusorn ;
Noon, Daniel ;
Chukeaw, Thanaphat ;
Zohour, Bahman ;
Donphai, Waleeporn ;
Chareonpanich, Metta ;
Senkan, Selim .
JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY, 2015, 32 :292-297
[36]   Key Mechanistic Insight into the Direct Gas-Phase Epoxidation of Propylene by the RuO2-CuO-NaCl/SiO2 Catalyst [J].
Seubsai, Anusorn ;
Zohour, Bahman ;
Noon, Daniel ;
Senkan, Selim .
CHEMCATCHEM, 2014, 6 (05) :1215-1219
[37]   The Effects of Cofeeding Chlorinated Hydrocarbons in the Direct Epoxidation of Propylene by Molecular Oxygen [J].
Seubsai, Anusorn ;
Senkan, Selim .
CHEMCATCHEM, 2011, 3 (11) :1751-1754
[38]   New Catalytic Materials for the Direct Epoxidation of Propylene by Molecular Oxygen [J].
Seubsai, Anusorn ;
Kahn, Michael ;
Senkan, Selim .
CHEMCATCHEM, 2011, 3 (01) :174-179
[39]   Evaluation of Rh/CexTi1-xO2 catalysts for synthesis of oxygenates from syngas using XPS and TPR techniques [J].
Sheerin, Ephraim ;
Reddy, Gunugunuri K. ;
Smirniotis, Panagiotis .
CATALYSIS TODAY, 2016, 263 :75-83
[40]   Catalytic epoxidation of propylene with CO/O2 over Au/TiO2 [J].
Sobolev, Vladimir I. ;
Koltunov, Konstantin Yu. .
APPLIED CATALYSIS A-GENERAL, 2014, 476 :197-203