Stable single-unit-cell nanosheets of zeolite MFI as active and long-lived catalysts

被引:1945
作者
Choi, Minkee [1 ]
Na, Kyungsu [1 ]
Kim, Jeongnam [1 ,2 ]
Sakamoto, Yasuhiro [5 ,6 ]
Terasaki, Osamu [4 ,6 ]
Ryoo, Ryong [1 ,2 ,3 ]
机构
[1] Korea Adv Inst Sci & Technol, Dept Chem, Ctr Funct Nanomat, Taejon 305701, South Korea
[2] Korea Adv Inst Sci & Technol, Grad Sch Nanosci & Technol WCU, Taejon 305701, South Korea
[3] Korea Adv Inst Sci & Technol, Inst NanoCentury, Taejon 305701, South Korea
[4] Korea Adv Inst Sci & Technol, Grad Sch EEWS WCU, Taejon 305701, South Korea
[5] Stockholm Univ, Arrhenius Lab, S-10691 Stockholm, Sweden
[6] Osaka Prefecture Univ, Nanosci & Nanotechnol Res Ctr, Sakai, Osaka 5998570, Japan
基金
瑞典研究理事会; 日本科学技术振兴机构;
关键词
COKE FORMATION;
D O I
10.1038/nature08288
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
Zeolites-microporous crystalline aluminosilicates-are widely used in petrochemistry and fine-chemical synthesis(1-3) because strong acid sites within their uniform micropores enable size- and shape-selective catalysis. But the very presence of the micropores, with aperture diameters below 1 nm, often goes hand-in-hand with diffusion limitations(3-5) that adversely affect catalytic activity. The problem can be overcome by reducing the thickness of the zeolite crystals, which reduces diffusion path lengths and thus improves molecular diffusion(4,5). This has been realized by synthesizing zeolite nanocrystals(6), by exfoliating layered zeolites(7-9), and by introducing mesopores in the microporous material through templating strategies(10-17) or demetallation processes(18-22). But except for the exfoliation, none of these strategies has produced 'ultrathin' zeolites with thicknesses below 5 nm. Here we show that appropriately designed bifunctional surfactants can direct the formation of zeolite structures on themesoporous and microporous length scales simultaneously and thus yield MFI (ZSM-5, one of the most important catalysts in the petrochemical industry) zeolite nanosheets that are only 2 nm thick, which corresponds to the b-axis dimension of a single MFI unit cell. The large number of acid sites on the external surface of these zeolites renders them highly active for the catalytic conversion of large organic molecules, and the reduced crystal thickness facilitates diffusion and thereby dramatically suppresses catalyst deactivation through coke deposition during methanol-to-gasoline conversion. We expect that our synthesis approach could be applied to other zeolites to improve their performance in a range of important catalytic applications.
引用
收藏
页码:246 / U120
页数:5
相关论文
共 28 条
  • [1] MOLECULAR OR SUPRAMOLECULAR TEMPLATING - DEFINING THE ROLE OF SURFACTANT CHEMISTRY IN THE FORMATION OF MICROPOROUS AND MESOPOROUS MOLECULAR-SIEVES
    BECK, JS
    VARTULI, JC
    KENNEDY, GJ
    KRESGE, CT
    ROTH, WJ
    SCHRAMM, SE
    [J]. CHEMISTRY OF MATERIALS, 1994, 6 (10) : 1816 - 1821
  • [2] COKE FORMATION IN HIGH-SILICA ZEOLITES
    BIBBY, DM
    HOWE, RF
    MCLELLAN, GD
    [J]. APPLIED CATALYSIS A-GENERAL, 1992, 93 (01) : 1 - 34
  • [3] COKE FORMATION IN ZEOLITE ZSM-5
    BIBBY, DM
    MILESTONE, NB
    PATTERSON, JE
    ALDRIDGE, LP
    [J]. JOURNAL OF CATALYSIS, 1986, 97 (02) : 493 - 502
  • [4] Amphiphilic organosilane-directed synthesis of crystalline zeolite with tunable mesoporosity
    Choi, Minkee
    Cho, Hae Sung
    Srivastava, Rajendra
    Venkatesan, Chithravel
    Choi, Dae-Heung
    Ryoo, Ryong
    [J]. NATURE MATERIALS, 2006, 5 (09) : 718 - 723
  • [5] State of the art and future challenges of zeolites as catalysts
    Corma, A
    [J]. JOURNAL OF CATALYSIS, 2003, 216 (1-2) : 298 - 312
  • [6] From microporous to mesoporous molecular sieve materials and their use in catalysis
    Corma, A
    [J]. CHEMICAL REVIEWS, 1997, 97 (06) : 2373 - 2419
  • [7] Delaminated zeolites:: Combining the benefits of zeolites and mesoporous materials for catalytic uses
    Corma, A
    Fornés, V
    Martínez-Triguero, J
    Pergher, SB
    [J]. JOURNAL OF CATALYSIS, 1999, 186 (01) : 57 - 63
  • [8] Delaminated zeolite precursors as selective acidic catalysts
    Corma, A
    Fornes, V
    Pergher, SB
    Maesen, TLM
    Buglass, JG
    [J]. NATURE, 1998, 396 (6709) : 353 - 356
  • [9] New aluminosilicate and titanosilicate delaminated materials active for acid catalysis, and oxidation reactions using H2O2
    Corma, A
    Diaz, U
    Domine, ME
    Fornés, V
    [J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2000, 122 (12) : 2804 - 2809
  • [10] The hydrothermal synthesis of zeolites: History and development from the earliest days to the present time
    Cundy, CS
    Cox, PA
    [J]. CHEMICAL REVIEWS, 2003, 103 (03) : 663 - 701