Thermal stability of TPA template and size-dependent selectivity of uncalcined TS-1 supported Au catalyst for propene epoxidation with H2 and O2

被引:32
作者
Feng, X. [1 ]
Chen, D. [3 ]
Zhou, X. G. [2 ]
机构
[1] China Univ Petr, State Key Lab Heavy Oil Proc, Qingdao 266580, Peoples R China
[2] E China Univ Sci & Technol, State Key Lab Chem Engn, Shanghai 200237, Peoples R China
[3] Norwegian Univ Sci & Technol, Dept Chem Engn, N-7491 Trondheim, Norway
来源
RSC ADVANCES | 2016年 / 6卷 / 50期
基金
中国博士后科学基金;
关键词
GAS-PHASE EPOXIDATION; DIRECT PROPYLENE EPOXIDATION; DEPOSITION-PRECIPITATION METHOD; GOLD NANOPARTICLES; EFFICIENT CATALYSTS; AU/TS-1; CATALYSTS; ACTIVE-SITES; PERFORMANCE; AU/TIO2; TRANSFORMATION;
D O I
10.1039/c6ra05772a
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
A tetrapropyl-ammonium (TPA) template, as the most critical component inside microporous channels of an uncalcined Au/TS-1 catalyst (Au/TS-1-B), hinders the entrance of Au nanoparticles into the micropores and thus prevents the micropore blocking induced deactivation for direct propene epoxidation with H-2 and O-2. In this work, the essential stability of the TPA template at distinct reaction temperatures is first investigated. It is found that the TPA template inside micropores decomposes to H2O, NH3 and propene after 350 degrees C. Based on a suitable reaction temperature range (< 350 degrees C), the PO formation rate shows a volcano-shaped relationship with reaction temperature and reaches a maximum value of 220 g(PO) h(-1) kg(Cat)(-1) at 260 degrees C, which is a noteworthy result compared with other reported catalysts. Moreover, due to presence of the TPA template inside micropores of TS-1, size-dependent selectivity shown on Au/TS-1-B should be intrinsic because the Au/TS-1-B catalyst exhibits uniform-sized Au nanoparticles and high stability. Hence, a series of Au/TS-1-B catalysts with different Au sizes are then tested for propene epoxidation, and the plausible reaction routes are also discussed.
引用
收藏
页码:44050 / 44056
页数:7
相关论文
共 49 条
  • [1] Propene adsorption on gold particles on TiO2(110)
    Ajo, HM
    Bondzie, VA
    Campbell, CT
    [J]. CATALYSIS LETTERS, 2002, 78 (1-4) : 359 - 368
  • [2] [Anonymous], 2009, FOCUS CATAL
  • [3] Transient technique for identification of true reaction intermediates: Hydroperoxide species in propylene epoxidation on gold/titanosilicate catalysts by X-ray absorption fine structure spectroscopy
    Bravo-Suarez, Juan J.
    Bando, Kyoko K.
    Lu, Jiqing
    Haruta, Masatake
    Fujitani, Tadahiro
    Oyama, S. Ted
    [J]. JOURNAL OF PHYSICAL CHEMISTRY C, 2008, 112 (04) : 1115 - 1123
  • [4] Enhancement of Catalyst Performance in the Direct Propene Epoxidation: A Study into Gold-Titanium Synergy
    Chen, Jiaqi
    Halin, Sander J. A.
    Pidko, Evgeny A.
    Verhoeven, M. W. G. M.
    Perez Ferrandez, Dulce M.
    Hensen, Emiel J. M.
    Schouten, Jaap C.
    Nijhuis, T. Alexander
    [J]. CHEMCATCHEM, 2013, 5 (02) : 467 - 478
  • [5] Activity of silylated titanosilicate supported gold nanoparticles towards direct propylene epoxidation reaction in the presence of trimethylamine
    Chowdhury, B.
    Bando, K. K.
    Bravo-Suarez, J. J.
    Tsubota, Susumu
    Haruta, M.
    [J]. JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL, 2012, 359 : 21 - 27
  • [6] Ionic liquid-enhanced immobilization of biosynthesized Au nanoparticles on TS-1 toward efficient catalysts for propylene epoxidation
    Du, Mingming
    Zhan, Guowu
    Yang, Xin
    Wang, Huixuan
    Lin, Wenshuang
    Zhou, Yao
    Zhu, Jing
    Lin, Ling
    Huang, Jiale
    Sun, Daohua
    Jia, Lishan
    Li, Qingbiao
    [J]. JOURNAL OF CATALYSIS, 2011, 283 (02) : 192 - 201
  • [7] Au/uncalcined TS-1 catalysts for direct propene epoxidation with H2 and O2: Effects of Si/Ti molar ratio and Au loading
    Feng, Xiang
    Duan, Xuezhi
    Yang, Jia
    Qian, Gang
    Zhou, Xinggui
    Chen, De
    Yuan, Weikang
    [J]. CHEMICAL ENGINEERING JOURNAL, 2015, 278 : 234 - 239
  • [8] Au/TS-1 catalyst prepared by deposition-precipitation method for propene epoxidation with H2/O2: Insights into the effects of slurry aging time and Si/Ti molar ratio
    Feng, Xiang
    Duan, Xuezhi
    Cheng, Hongye
    Qian, Gang
    Chen, De
    Yuan, Weikang
    Zhou, Xinggui
    [J]. JOURNAL OF CATALYSIS, 2015, 325 : 128 - 135
  • [9] Insights into size-dependent activity and active sites of Au nanoparticles supported on TS-1 for propene epoxidation with H2 and O2
    Feng, Xiang
    Duan, Xuezhi
    Qian, Gang
    Zhou, Xinggui
    Chen, De
    Yuan, Weikang
    [J]. JOURNAL OF CATALYSIS, 2014, 317 : 99 - 104
  • [10] Au nanoparticles deposited on the external surfaces of TS-1: Enhanced stability and activity for direct propylene epoxidation with H2 and O2
    Feng, Xiang
    Duan, Xuezhi
    Qian, Gang
    Zhou, Xinggui
    Chen, De
    Yuan, Weikang
    [J]. APPLIED CATALYSIS B-ENVIRONMENTAL, 2014, 150 : 396 - 401