Understanding the Role of Internal Diffusion Barriers in Pt/Beta Zeolite Catalyzed Isomerization of n-Heptane

被引:55
作者
Guo, Zhongyuan [1 ]
Li, Xin [1 ]
Hu, Shen [1 ]
Ye, Guanghua [1 ]
Zhou, Xinggui [1 ]
Coppens, Marc-Olivier [2 ]
机构
[1] East China Univ Sci & Technol, State Key Lab Chem Engn, Shanghai 200237, Peoples R China
[2] UCL, Dept Chem Engn, London WC1E 7JE, England
基金
中国国家自然科学基金; 英国工程与自然科学研究理事会;
关键词
diffusion barriers; interfaces; n-heptane; Pt; Beta; zeolite catalysis; MFI-TYPE ZEOLITES; SURFACE BARRIERS; TRANSPORT; INTERGROWTH; HYDROISOMERIZATION; EXISTENCE; CRYSTALS;
D O I
10.1002/anie.201913660
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Applications of zeolites in catalysis are plagued by strong diffusion resistance, which results from limitations to molecular transport in micropores, across external crystal surfaces, but also across internal interfaces. The first type of diffusion resistance is well understood, the second is receiving increasing attention, while the diffusion barriers at internal interfaces remain largely unclear. We take Pt/Beta catalyzed isomerization of n-heptane as the model system to explore the role of internal diffusion barriers in zeolite catalysis. The two as-synthesized Pt/Beta catalysts have an identical Pt loading, similar Beta particle size and acidity, but different internal structures. A Pt/Beta crystal with no observable internal interfaces can be 180 % higher in activity and 22 % higher in selectivity than its counterpart with numerous internal interfaces. This can only be attributed to the strong transport barriers across internal interfaces, as supported by directly comparing the apparent diffusivities of the two Beta samples.
引用
收藏
页码:1548 / 1551
页数:4
相关论文
共 36 条
[1]  
[Anonymous], 2008, ANGEW CHEM-GER EDIT
[2]   Particular properties of the coke formed on nano-sponge *BEA zeolite during ethanol-to-hydrocarbons transformation [J].
Astafan, A. ;
Benghalem, M. A. ;
Pouilloux, Y. ;
Patarin, J. ;
Bats, N. ;
Bouchy, C. ;
Daou, T. J. ;
Pinard, L. .
JOURNAL OF CATALYSIS, 2016, 336 :1-10
[3]   Understanding Diffusion in Hierarchical Zeolites with House-of-Cards Nanosheets [J].
Bai, Peng ;
Haldoupis, Emmanuel ;
Dauenhauer, Paul J. ;
Tsapatsis, Michael ;
Siepmann, J. Ilja .
ACS NANO, 2016, 10 (08) :7612-7618
[4]   Synthesis and characterization of the all-silica pure polymorph C and an enriched polyrnorph B intergrowth of zeolite beta [J].
Cantin, Angel ;
Corma, Avelino ;
Diaz-Cabanas, Maria J. ;
Jorda, Jose L. ;
Moliner, Manuel ;
Rey, Fernando .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2006, 45 (47) :8013-8015
[5]   Enhanced Molecular Transport in Hierarchical Silicalite-1 [J].
Chang, Chun-Chih ;
Teixeira, Andrew R. ;
Li, Chao ;
Dauenhauer, Paul J. ;
Fan, Wei .
LANGMUIR, 2013, 29 (45) :13943-13950
[6]   From microporous to mesoporous molecular sieve materials and their use in catalysis [J].
Corma, A .
CHEMICAL REVIEWS, 1997, 97 (06) :2373-2419
[7]   A NEW EXPERIMENTAL-TECHNIQUE FOR MEASUREMENT OF INTRACRYSTALLINE DIFFUSIVITY [J].
EIC, M ;
RUTHVEN, DM .
ZEOLITES, 1988, 8 (01) :40-45
[8]   Intracrystalline Transport Resistances in Nanoporous Zeolite X [J].
Feldhoff, Armin ;
Caro, Juergen ;
Jobic, Herve ;
Ollivier, Jacques ;
Krause, Cordula B. ;
Galvosas, Petrik ;
Kaerger, Joerg .
CHEMPHYSCHEM, 2009, 10 (14) :2429-2433
[9]   Direct quantification of surface barriers for mass transfer in nanoporous crystalline materials [J].
Gao, Mingbin ;
Li, Hua ;
Yang, Miao ;
Gao, Shushu ;
Wu, Pengfei ;
Tian, Peng ;
Xu, Shutao ;
Ye, Mao ;
Liu, Zhongmin .
COMMUNICATIONS CHEMISTRY, 2019, 2 (1)
[10]   Cavity-controlled diffusion in 8-membered ring molecular sieve catalysts for shape selective strategy [J].
Gao, Shushu ;
Liu, ZhiQiang ;
Xu, Shuta ;
Zheng, Anmin ;
Wu, Pengfei ;
Li, Bing ;
Yuan, Xiaoshuai ;
Wei, Yingxu ;
Liu, Zhongmin .
JOURNAL OF CATALYSIS, 2019, 377 :51-62