1. School of Chemical Engineering, Northwest University, Xi’an 710069, China 2. International Science & Technology Cooperation Base for Clean Utilization of Hydrocarbon Resources, Chemical Engineering Research Center of the Ministry of Education for Advanced Use Technology of Shanbei Energy, Collaborative Innovation Center for Development of Energy and Chemical Industry in Northern Shaanxi, Northwest University, Xi’an 710069, China
A facile synthesis of hierarchical ZSM-5 with the three-dimensionally ordered mesoporosity (3DOm ZSM-5) was achieved by solid conversion (SC) of SiO2 colloidal crystals to high-crystalline ZSM-5. The products of 3DZ5_S/C and 3DZ5_S, which were severally transformed from the carbon-padded SiO2 colloidal crystals and the initial SiO2 colloidal crystals, exhibited not only a similar ordered structure and acidity but also higher crystallinity and more balanced meso-/micropore combination in comparison with 3DZ5_C obtained by the conventional confined space crystallization approach. All three synthesized 3DZ5 catalysts showed improved methanol-to-propylene performance than the commercially microporous ZSM-5 (CZ5), embodied in five times longer lifetime, higher propylene selectivity and Spropylene/Sethylene ratio (P/E), and superior coke toleration with lower formation rate of coke (Rcoke). Moreover, the 3DZ5_S catalyst in situ converted from SiO2 colloidal crystals presented the highest selectivities of propylene (42.51%) and light olefins (74.6%) among all three 3DZ5 catalysts. The high efficiency in synthesis and in situ utilization of SiO2 colloidal crystals demonstrate the proposed SC strategy to be more efficiently and eco-friendly for the high-yield production of not only 3DOm ZSM-5 but also other types of hierarchical zeolites.
M Shamzhy , M Opanasenko , P Concepción , A Martínez . New trends in tailoring active sites in zeolite-based catalysts. Chemical Society Reviews, 2019, 48(4): 1095–1149 https://doi.org/10.1039/C8CS00887F
3
Q M Sun , N Wang , J H Yu . Advances in catalytic applications of zeolite-supported metal catalysts. Advanced Materials, 2021, 33(51): 2104442 https://doi.org/10.1002/adma.202104442
4
X L Liu , C M Wang , J Zhou , C Liu , Z C Liu , J Shi , Y D Wang , J W Teng , Z K Xie . Molecular transport in zeolite catalysts: depicting an integrated picture from macroscopic to microscopic scales. Chemical Society Reviews, 2022, 51(19): 8174–8200 https://doi.org/10.1039/D2CS00079B
5
A J Mallette , S Seo , J D Rimer . Synthesis strategies and design principles for nanosized and hierarchical zeolites. Nature Synthesis, 2022, 1(7): 521–534 https://doi.org/10.1038/s44160-022-00091-8
6
J Pérez-Ramírez , C H Christensen , K Egeblad , C H Christensen , J C Groen . Hierarchical zeolites: enhanced utilisation of microporous crystals in catalysis by advances in materials design. Chemical Society Reviews, 2008, 37(11): 2530–2542 https://doi.org/10.1039/b809030k
7
S Xu , X Zhang , D G Cheng , F Chen , X Ren . Effect of hierarchical ZSM-5 zeolite crystal size on diffusion and catalytic performance of n-heptane cracking. Frontiers of Chemical Science and Engineering, 2018, 12(4): 780–789 https://doi.org/10.1007/s11705-018-1733-8
8
S Mintova , M Jaber , V Valtchev . Nanosized microporous crystals: emerging applications. Chemical Society Reviews, 2015, 44(20): 7207–7233 https://doi.org/10.1039/C5CS00210A
9
L H Chen , M H Sun , Z Wang , W Yang , B L Su . Hierarchically structured zeolites: from design to application. Chemical Reviews, 2020, 120(20): 11194–11294 https://doi.org/10.1021/acs.chemrev.0c00016
10
H Y Chen , M F Yang , W J Shang , Y Tong , B Y Liu , X L Han , J B Zhang , Q Q Hao , M Sun , X X Ma . Organosilane surfactant-directed synthesis of hierarchical ZSM-5 zeolites with improved catalytic performance in methanol-to-propylene reaction. Industrial & Engineering Chemistry Research, 2018, 57(32): 10956–10966 https://doi.org/10.1021/acs.iecr.8b00849
11
M J Mendoza-castro , E D O Jardim , C A Trujillo , N Linares , J Garciamartinez . Hierarchical catalysts prepared by interzeolite transformation. Journal of the American Chemical Society, 2022, 144(11): 5163–5171 https://doi.org/10.1021/jacs.2c00665
12
C T Wang , W Fang , Z Q Liu , L Wang , Z W Liao , Y R Yang , H J Li , L Liu , H Zhou , X D Qin . et al.. Fischer-tropsch synthesis to olefins boosted by MFI zeolite nanosheets. Nature Nanotechnology, 2022, 17(7): 714–720 https://doi.org/10.1038/s41565-022-01154-9
13
D Verboekend , M Milina , S Mitchell , J Pérez-Ramírez . Hierarchical zeolites by desilication: occurrence and catalytic impact of recrystallization and restructuring. Crystal Growth & Design, 2013, 13(11): 5025–5035 https://doi.org/10.1021/cg4010483
14
J J Li , M Liu , X W Guo , S T Xu , Y X Wei , Z M Liu , C S Song . Interconnected hierarchical ZSM-5 with tunable acidity prepared by a dealumination-realumination process: a superior MTP catalyst. ACS Applied Materials & Interfaces, 2017, 9(31): 26096–26106 https://doi.org/10.1021/acsami.7b07806
15
I I Ivanova , E E Knyazeva . Micro-mesoporous materials obtained by zeolite recrystallization: synthesis, characterization and catalytic applications. Chemical Society Reviews, 2013, 42(9): 3671–3688 https://doi.org/10.1039/C2CS35341E
16
Z P Wang , C Li , H J Cho , S C Kung , M A Snyder , W Fan . Direct, single-step synthesis of hierarchical zeolites without secondary templating. Journal of Materials Chemistry. A, Materials for Energy and Sustainability, 2015, 3(3): 1298–1305 https://doi.org/10.1039/C4TA05031B
17
M Choi , H S Cho , R Srivastava , C Venkatesan , D H Choi , R Ryoo . Amphiphilic organosilane-directed synthesis of crystalline zeolite with tunable mesoporosity. Nature Materials, 2006, 5(9): 718–723 https://doi.org/10.1038/nmat1705
18
M Choi , K Na , J Kim , Y Sakamoto , R Ryoo . Stable single-unit-cell nanosheets of zeolite MFI as active and long-lived catalysts. Nature, 2009, 461(7261): 246–249 https://doi.org/10.1038/nature08288
19
M Hartmann . Hierarchical zeolites: a proven strategy to combine shape selectivity with efficient mass transport. Angewandte Chemie International Edition, 2004, 43(44): 5880–5882 https://doi.org/10.1002/anie.200460644
20
H Dai , Y F Shen , T M Yang , C S Lee , D L Fu , A Agarwal , T T Le , M Tsapatsis , J C Palmer , B M Weckhuysen . et al.. Finned zeolite catalysts. Nature Materials, 2020, 19(10): 1074–1080 https://doi.org/10.1038/s41563-020-0753-1
21
X Y Zhang , D X Liu , D D Xu , S Asahina , K A Cychosz , K V Agrawal , Y Al Wahedi , A Bhan , S Al Hashimi , O Terasaki . et al.. Synthesis of self-pillared zeolite nanosheets by repetitive branching. Science, 2012, 336(6089): 1684–1687 https://doi.org/10.1126/science.1221111
22
W Fan , M A Snyder , S Kumar , P S Lee , W C Yoo , A V Mccormick , R L Penn , A Stein , M Tsapatsis . Hierarchical nanofabrication of microporous crystals with ordered mesoporosity. Nature Materials, 2008, 7(12): 984–991 https://doi.org/10.1038/nmat2302
23
V Valtchev , G Majano , S Mintova , J Pérez-Ramírez . Tailored crystalline microporous materials by post-synthesis modification. Chemical Society Reviews, 2013, 42(1): 263–290 https://doi.org/10.1039/C2CS35196J
24
H Y Chen , W J Shang , C B Yang , B Y Liu , C Y Dai , J B Zhang , Q Q Hao , M Sun , X X Ma . Epitaxial growth of layered-bulky ZSM-5 hybrid catalysts for the methanol-to-propylene process. Industrial & Engineering Chemistry Research, 2019, 58(4): 1580–1589 https://doi.org/10.1021/acs.iecr.8b05472
25
S Kim , G Park , M H Woo , G Kwak , S K Kim . Control of hierarchical structure and framework-Al distribution of ZSM-5 via adjusting crystallization temperature and their effects on methanol conversion. ACS Catalysis, 2019, 9(4): 2880–2892 https://doi.org/10.1021/acscatal.8b04493
26
H O Mohamed , R K Parsapur , I Hita , A Ramírez , K W Huang , J Gascon , P Castaño . Stable and reusable hierarchical ZSM-5 zeolite with superior performance for olefin oligomerization when partially coked. Applied Catalysis B: Environmental, 2022, 316: 121582 https://doi.org/10.1016/j.apcatb.2022.121582
27
H Y Chen , J Wydra , X Y Zhang , P S Lee , Z P Wang , W Fan , M Tsapatsis . Hydrothermal synthesis of zeolites with three-dimensionally ordered mesoporous-imprinted structure. Journal of the American Chemical Society, 2011, 133(32): 12390–12393 https://doi.org/10.1021/ja2046815
28
J Wang , M F Yang , W J Shang , X P Su , Q Q Hao , H Y Chen , X X Ma . Synthesis, characterization, and catalytic application of hierarchical SAPO-34 zeolite with three-dimensionally ordered mesoporous-imprinted structure. Microporous and Mesoporous Materials, 2017, 252: 10–16 https://doi.org/10.1016/j.micromeso.2017.06.012
29
H J Cho , P Dornath , W Fan . Synthesis of hierarchical Sn-MFI as lewis acid catalysts for isomerization of cellulosic sugars. ACS Catalysis, 2014, 4(6): 2029–2037 https://doi.org/10.1021/cs500295u
30
Q You , X Wang , Y S Wu , C Y Bi , X Yang , M Sun , J B Zhang , Q Q Hao , H Y Chen , X X Ma . Hierarchical Ti-beta with a three-dimensional ordered mesoporosity for catalytic epoxidation of bulky cyclic olefins. New Journal of Chemistry, 2021, 45(23): 10303–10314 https://doi.org/10.1039/D1NJ00736J
31
H Y Chen , P S Lee , X Y Zhang , D Lu . Structure replication and growth development of three-dimensionally ordered mesoporous-imprinted zeolites during confined growth. Journal of Materials Research, 2013, 28(10): 1356–1364 https://doi.org/10.1557/jmr.2013.106
32
Z P Wang , P Dornath , C C Chang , H Y Chen , W Fan . Confined synthesis of three-dimensionally ordered mesoporous-imprinted zeolites with tunable morphology and Si/Al ratio. Microporous and Mesoporous Materials, 2013, 181: 8–16 https://doi.org/10.1016/j.micromeso.2013.07.010
33
R Khare , A Bhan . Mechanistic studies of methanol-to-hydrocarbons conversion on diffusion-free MFI samples. Journal of Catalysis, 2015, 329: 218–228 https://doi.org/10.1016/j.jcat.2015.05.012
34
B Fernández-Reyes , S Morales-Jiménez , G Sánchez-Marrero , J C Muñoz-Senmache , A J Hernández-Maldonado . Hierarchical three-dimensionally ordered mesoporous carbon (3DOm) zeolite composites for the adsorption of contaminants of emerging concern. Journal of Hazardous Materials Letters, 2021, 2: 100017 https://doi.org/10.1016/j.hazl.2021.100017
35
P S Lee , X Y Zhang , J A Stoeger , A Malek , W Fan , S Kumar , W C Yoo , S Al Hashimi , R L Penn , A Stein . et al.. Sub-40 nm zeolite suspensions via disassembly of three-dimensionally ordered mesoporous-imprinted silicalite-1. Journal of the American Chemical Society, 2011, 133(3): 493–502 https://doi.org/10.1021/ja107942n
36
S Mintova , M Hölzl , V Valtchev , B Mihailova , Y Bouizi , T Bein . Closely packed zeolite nanocrystals obtained via transformation of porous amorphous silica. Chemistry of Materials, 2004, 16(25): 5452–5459 https://doi.org/10.1021/cm030640b
37
D Z Han , D Y Yang , C Y Bi , G Q Zhang , F Yang , Q Q Hao , J B Zhang , H Y Chen , X X Ma . Dry-gel conversion synthesis of SAPO-14 zeolites for the selective conversion of methanol to propylene. Inorganic Chemistry Frontiers, 2023, 10(21): 6193–6203 https://doi.org/10.1039/D3QI00990D
38
T M Davis , M A Snyder , J E Krohn , M Tsapatsis . Nanoparticles in lysine-silica sols. Chemistry of Materials, 2006, 18(25): 5814–5816 https://doi.org/10.1021/cm061982v
39
J Pérez-Ramírez , D Verboekend , A Bonilla , S Abelló . Zeolite catalysts with tunable hierarchy factor by pore-growth moderators. Advanced Functional Materials, 2009, 19(24): 3972–3979 https://doi.org/10.1002/adfm.200901394
40
X B Zhao , Y Hong , L Y Wang , D Fan , N N Yan , X N Liu , P Tian , X W Guo , Z M Liu . External surface modification of as-made ZSM-5 and their catalytic performance in the methanol to propylene reaction. Chinese Journal of Catalysis, 2018, 39(8): 1418–1426 https://doi.org/10.1016/S1872-2067(18)63117-1
41
K Ramesh , C Jie , Y F Han , A Borgna . Synthesis, characterization, and catalytic activity of phosphorus modified H-ZSM-5 catalysts in selective ethanol dehydration. Industrial & Engineering Chemistry Research, 2010, 49(9): 4080–4090 https://doi.org/10.1021/ie901666f
42
J X Zhang , A Zhou , K Gawande , G X Li , S J Shang , C Y Dai , W Fan , Y Han , C S Song , L M Ren . et al.. B-axis-oriented ZSM-5 nanosheets for efficient alkylation of benzene with methanol: synergy of acid sites and diffusion. ACS Catalysis, 2023, 13(6): 3794–3805 https://doi.org/10.1021/acscatal.2c06384
43
J H Li , Y N Wang , W Z Jia , Z W Xi , H H Chen , Z R Zhu , Z H Hu . Effect of external surface of HZSM-5 zeolite on product distribution in the conversion of methanol to hydrocarbons. Journal of Energy Chemistry, 2014, 23(6): 771–780 https://doi.org/10.1016/S2095-4956(14)60211-4
44
C C Chang , A R Teixeira , C Li , P J Dauenhauer , W Fan . Enhanced molecular transport in hierarchical silicalite-1. Langmuir, 2013, 29(45): 13943–13950 https://doi.org/10.1021/la403706r
45
M H Sun , J Zhou , Z Y Hu , L H Chen , L Y Li , Y D Wang , Z K Xie , S Turner , G Van Tendeloo , T Hasan . et al.. Hierarchical zeolite single-crystal reactor for excellent catalytic efficiency. Matter, 2020, 3(4): 1226–1245 https://doi.org/10.1016/j.matt.2020.07.016
46
M S Beheshti , M Behzad , J Ahmadpour , H Arabi . Modification of H-[B]-ZSM-5 zeolite for methanol to propylene (MTP) conversion: investigation of extrusion and steaming treatments on physicochemical characteristics and catalytic performance. Microporous and Mesoporous Materials, 2020, 291: 109699 https://doi.org/10.1016/j.micromeso.2019.109699
47
Y P Zhang , M G Li , E H Xing , Y B Luo , X T Shu . Protective desilication of highly siliceous H-ZSM-5 by sole tetraethylammonium hydroxide for the methanol to propylene (MTP) reaction. RSC Advances, 2018, 8(66): 37842–37854 https://doi.org/10.1039/C8RA06786D
48
X Q Wu , Y X Wei , Z M Liu . Dynamic catalytic mechanism of the methanol-to-hydrocarbons reaction over zeolites. Accounts of Chemical Research, 2023, 56(14): 2001–2014 https://doi.org/10.1021/acs.accounts.3c00187
49
M Z Zhang , S T Xu , Y X Wei , J Z Li , J B Wang , W N Zhang , S S Gao , Z M Liu . Changing the balance of the MTO reaction dual-cycle mechanism: reactions over ZSM-5 with varying contact times. Chinese Journal of Catalysis, 2016, 37(8): 1413–1422 https://doi.org/10.1016/S1872-2067(16)62466-X