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 50 条
  • [21] Selective silylation boosts propylene epoxidation with H2 and O2 over Au/TS-1
    Aly, Mostafa
    Saeys, Mark
    CHEM CATALYSIS, 2021, 1 (04): : 761 - 762
  • [22] Direct propylene epoxidation with H2 and O2 over In modified Au/TS-1 catalysts
    Lu, Ji-Qing
    Li, Na
    Pan, Xiao-Rong
    Zhang, Chao
    Luo, Meng-Fei
    CATALYSIS COMMUNICATIONS, 2012, 28 : 179 - 182
  • [23] Au supported defect free TS-1 for enhanced performance of gas phase propylene epoxidation with H2 and O2
    Li, Wenqian
    Qiu, Minghuang
    Li, Wanting
    Ge, Lixia
    Zhang, Kun
    Chen, Xinqing
    SUSTAINABLE ENERGY & FUELS, 2022, 6 (10) : 2462 - 2470
  • [24] Differences in catalytic sites for selective oxidation of propane and direct propene epoxidation using H2 and O2 on Au/TS-1 catalysts
    Zhang, Zhihua
    Liu, Fan
    Cao, Yueqiang
    Zhong, Yuxia
    Duan, Xuezhi
    Zhou, Xinggui
    CHEMICAL ENGINEERING JOURNAL, 2025, 508
  • [25] Gas-phase epoxidation of propylene in the presence of H2 and O2 over small gold ensembles in uncalcined TS-1
    Lee, Wen-Sheng
    Akatay, M. Cem
    Stach, Eric A.
    Ribeiro, Fabio H.
    Delgass, W. Nicholas
    JOURNAL OF CATALYSIS, 2014, 313 : 104 - 112
  • [26] Enhancing the dynamic electron transfer of Au species on wormhole-like TS-1 for boosting propene epoxidation performance with H2 and O2
    Lin, Dong
    Zheng, Xiuhui
    Feng, Xiang
    Sheng, Nan
    Song, Zhaoning
    Liu, Yibin
    Chen, Xiaobo
    Cai, Zhenping
    Chen, De
    Yang, Chaohe
    GREEN ENERGY & ENVIRONMENT, 2020, 5 (04) : 433 - 443
  • [27] 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
    APPLIED CATALYSIS B-ENVIRONMENTAL, 2014, 150 : 396 - 401
  • [28] Enhancing the dynamic electron transfer of Au species on wormhole-like TS-1 for boosting propene epoxidation performance with H2 and O2
    Dong Lin
    Xiuhui Zheng
    Xiang Feng
    Nan Sheng
    Zhaoning Song
    Yibin Liu
    Xiaobo Chen
    Zhenping Cai
    De Chen
    Chaohe Yang
    Green Energy & Environment, 2020, 5 (04) : 433 - 443
  • [29] Propane reacts with O2 and H2 on gold supported TS-1 to form oxygenates with high selectivity
    Bravo-Suarez, J. J.
    Bando, K. K.
    Akita, T.
    Fujitani, T.
    Fuhrer, T. J.
    Oyama, S. T.
    CHEMICAL COMMUNICATIONS, 2008, (28) : 3272 - 3274
  • [30] Phosphate-Modified Effects on Uncalcined TS-1-Immobilized Au Catalysts for Propylene Epoxidation with H2 and O2
    Xu, Jialun
    Zhang, Zhihua
    Yu, Daiyi
    Du, Wei
    Zheng, Yang
    Song, Nan
    Duan, Xuezhi
    Zhou, Xinggui
    INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 2023, 62 (50) : 21654 - 21665