2024 04 v.39;No.123 3-12+2
离子热合成ZSM-22分子筛及其晶化机理研究
基金项目(Foundation):
国家自然科学基金（22072174）;;
广东省自然科学基金项目（2023A1515012115）;;
汕头大学卓越人才科研启动项目（NTF22013）
邮箱(Email):
liusuyao@stu.edu.cn;ywfang@stu.edu.cn;
DOI:
中文作者单位:
汕头大学化学化工学院;
摘要(Abstract):
本研究选用离子液体（1-丁基-3-甲基咪唑氯盐，[BMIm]Cl）为模板剂兼溶剂，采用离子热合成法成功制备了结晶度高、孔道开放、形貌规整的ZSM-22分子筛.通过系统调控初始凝胶配比，如NH_4F、[BMIm]Cl、H_2O投料量和晶化时间，实现了对ZSM-22分子筛晶体尺寸和晶化过程的精确控制.研究发现，增加[BMIm]Cl用量、减少水含量可显著提高合成体系的粘度和过饱和度，从而有效促进大量晶核的形成，抑制晶体的生长，制备得到了晶粒长度为700 nm～800 nm，宽度为50 nm～80 nm的ZSM-22分子筛，且与常规合成路线所得分子筛晶粒尺寸相近.经对晶化过程考察认为，[BMIm]Cl和合成温度是缩短ZSM-22分子筛诱导期，加速其成核和晶体生长过程的关键因素.本研究为ZSM-22分子筛的绿色可持续合成提供了新的思路，为其在催化、吸附、分离等领域的应用开辟了广阔前景.
关键词(KeyWords):
离子液体;;合成参数;;晶化机理;;分子筛
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参考文献
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[2]MALLETTE A J,SHILPA K,RIMER J D.The current understanding of mechanistic pathways in zeolite crystallization[J].Chemical Reviews,2024,124(6):3416-3493.
[3]DUSSELIER M,DAVIS M E.Small-pore zeolites:synthesis and catalysis[J].Chemical Reviews,2018,118(11):5265-5329.
[4]PALCIC,VALTCHEV V.Analysis and control of acid sites in zeolites[J].Applied Catalysis A:General,2020,606:117795.
[5]LIU S,REN J,ZHU S,et al.Synthesis and characterization of the Fe-substituted ZSM-22 zeolite catalyst with high n-dodecane isomerization performance[J].Journal of Catalysis,2015,330:485-496.
[6]LIU S,REN J,ZHANG H,et al.Synthesis,characterization and isomerization performance of micro/mesoporous materials based on H-ZSM-22 zeolite[J].Journal of Catalysis,2016,335:11-23.
[7]DYBALLA M,OBENAUS U,ROSENBERGER M,et al.Post-synthetic improvement of H-ZSM-22zeolites for the methanol-to-olefin conversion[J].Microporous and Mesoporous Materials,2016,233:26-30.
[8]DWYER F G.Highly siliceous porous crystalline material ZSM-22 and its use in catalytic dewaxing of petroleum stocks:US4556477A.[P].1984-10-19.
[9]XIONG S,SUN J,LI H,et al.The synthesis of hierarchical ZSM-22 zeolite with only the PHMBtemplate for hydroisomerization of n-hexadecane[J].Microporous and Mesoporous Materials,2024,365:112895.
[10]LIU S,ZHANG H,CHEN H,et al.Fabrication of a core-shell MFI@TON material and its enhanced catalytic performance for toluene alkylation[J].Catalysis Science&Technology,2020,10(5):1281-1291.
[11]CHANG T,LIU S.Role of the mesoporous diameters of hierarchical ZSM-22/MCM-41 zeolite for n-alkane isomerization[J].Molecular Catalysis,2021,503:111420.
[12]AYALA R,IVANOVA S,BLANES J M M,et al.Understanding the role of the cosolvent in the zeolite template function of imidazolium-based ionic liquid[J].The Journal of Physical Chemistry B,2014,118:3650-3660.
[13]COOPER E R,WHEATLEY P S,WEBB P B,et al.Ionic liquids and eutectic mixtures as solvent and template in synthesis of zeolite analogues[J].Nature,2004,430(7003):1012-1016.
[14]J M,SZYJA B M,ROMERO-SARRIA F,et al.Multiple zeolite structures from one ionic liquid template[J].Chemistry-A European Journal,2013,19:122-2130.
[15]LI X,CURNOW O J,CHOI J,et al.Recent advances in the imidazolium-based ionic liquid-templated synthesis of micro-porous zeolites[J].Materials Today Chemistry,2022,26:101133.
[16]WEN H,ZHOU Y,XIE J,et al.Pure-silica ZSM-22 zeolite rapidly synthesized by novel ionic liquiddirected dry-gel conversion[J].RSC Advances,2014,4:49647-49654.
[17]LOPES C W,FINGER P H,MIGNONI M L,et al.Ti O2-TON zeolite synthesis using an ionic liquid as a structure-directing agent[J].Microporous and Mesoporous Materials,2015,213:78-84.
[18]LU P,CHEN L,ZHANG Y,et al.Rapid synthesis of ZSM-22 zeolites using imidazolium-based ionic liquids as OSDAs in fluoride media[J].Microporous and Mesoporous Materials,2016,236:193-201.
[19]LI X,TSAI S T,WU K C W,et al.Morphology control of ionic-liquid-templated ZSM-22 and ZSM-5zeolites using a two-step process and its effect on toluene methylation[J].Microporous and Mesoporous Materials,2021,328:111475.
[20]ARICHI J,LOUIS B.Toward Microscopic design of zeolite crystals:advantages of the fluoridemediated synthesis[J].Crystal Growth&Design,2008,8(11):3999-4005.
[21]JAMIL A K,MURAZA O.Facile control of nanosized ZSM-22 crystals using dynamic crystallization technique[J].Microporous and Mesoporous Materials,2016,227:16-22.
[22]DEL CAMPO P,BEATO P,RAY F,et al.Influence of post-synthetic modifications on the composition,acidity and textural properties of ZSM-22 zeolite[J].Catalysis Today,2018,229:120-134.
[23]CAMBLOR M A,CORMA A,VALENCIA S.Characterization of nanocrystalline zeolite Bet a[J].Microporous and Mesoporous Materials,1998,25(1/3):59-74.
[24]LIU T,LI X,SHIM J,et al.Accelerated crystallization kinetics of MFI zeolite via imidazolium-based synthesis[J].Crystal Growth&Design,2024,24 (10):4122-4130.
[25]LIU B,ZHENG Y,HU N,et al.Synthesis of low-silica CHA zeolite chabazite in fluoride media without organic structural directing agents and zeolites[J].Microporous and Mesoporous Materials,2014,196:270-276.
[26]HU Y,LIU C,ZHANG Y,et al.Microwave-assisted hydrothermal synthesis of nanozeolites with controllable size[J].Microporous and Mesoporous Materials,2009,119(1/3):306-314.
[27]JAIN R,MALLETTE A J,RIMER J D.Controlling nucleation pathways in zeolite crystallization:seeding conceptual methodologies for advanced materials Design[J].Journal of the American Chemical Society,2021,143(51):21446-21460.
基本信息:
DOI：
中图分类号:TQ424.25
引用信息:
[1]周骏峰,顾文瑶,胡心洁等.离子热合成ZSM-22分子筛及其晶化机理研究[J].汕头大学学报(自然科学版),2024,39(04):3-12+2.
基金信息:
国家自然科学基金（22072174）;; 广东省自然科学基金项目（2023A1515012115）;; 汕头大学卓越人才科研启动项目（NTF22013）
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