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现代化工  2019, Vol. 39 Issue (11): 67-72    DOI: 10.16606/j.cnki.issn0253-4320.2019.11.015
  科研与开发 本期目录 | 过刊浏览 | 高级检索 |
碱处理调控ZSM-5孔结构及其在甲醇制芳烃中的性能研究
李政杭, 刘民, 李俊杰, 郭新闻
大连理工大学化工与环境生命学部, 辽宁 大连 116024
Modification of ZSM-5 by alkali treatment and its performance in methanol to aromatics
LI Zheng-hang, LIU Min, LI Jun-jie, GUO Xin-wen
Faculty of Chemical, Environmental and Biological Science and Technology, Dalian University of Technology, Dalian 116024, China
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摘要 采用水热法晶化得到纳米板状孪晶型HZSM-5,通过NaOH或TPAOH处理调变ZSM-5的孔结构。结果表明,NaOH处理将贯通的介孔结构引入微孔ZSM-5中,而TPAOH处理得到多空腔结构,空腔通过微孔与外界连通。对具有不同孔结构的ZSM-5进行Zn改性,并用于甲醇制芳烃反应。通过XRD、SEM、TEM和氩气物理吸附分析不同样品的结构;利用NH3-TPD测定不同样品的酸量;通过XPS分析不同样品的Zn状态。具有多空腔结构的Zn/HZ-TPAOH催化剂的芳烃选择性大幅提升,同时催化剂寿命明显增加,具有连通介孔结构的Zn/HZ-NaOH寿命又明显长于具有多空腔结构的Zn/HZ-TPAOH。
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李政杭
刘民
李俊杰
郭新闻
关键词:  ZSM-5  碱处理  多级孔结构  甲醇制芳烃    
Abstract: Nano-plate twin crystal HZSM-5 is crystallized by hydrothermal method,and the pore structure of ZSM-5 is modified by NaOH or TPAOH.The results show that microporous ZSM-5 gains the perforated mesoporous structure by NaOH treatment and the multi-cavity structure is obtained by TPAOH treatment.The cavity connects to the outside through the micropore.ZSM-5 with different pore structure is modified by Zn and then used in methanol to aromatic reaction.The structures of different samples are analyzed by XRD,SEM,TEM and Argon physical adsorption.NH3-TPD is used to determine the acidic properties of different samples.Zn states in different samples are analyzed by XPS.The results show that Zn/HZ-TPAOH catalyst with multi-cavity structure can significantly improve the selectivity of aromatics,and the catalyst lifetime lengthens significantly.The lifetime of Zn/HZ-NaOH with connected mesoporous structure is significantly longer than that of Zn/HZ-TPAOH with multi-cavity structure.
Key words:  ZSM-5    alkali treatment    multi-stage pore structure    methanol to aromatics
收稿日期:  2019-01-31      修回日期:  2019-09-10           出版日期:  2019-11-20
O643.3  
基金资助: 国际重点研发计划资助项目(2018YFB0604801)
通讯作者:  刘民(1976-),男,博士,副教授,研究方向为环境友好的多孔催化材料设计、表征和应用,通讯联系人,lium@dlut.edu.cn。    E-mail:  lium@dlut.edu.cn
作者简介:  李政杭(1993-),男,硕士研究生,研究方向为ZSM-5的合成及其甲醇芳构化的研究,DUT_lzh@163.com
引用本文:    
李政杭, 刘民, 李俊杰, 郭新闻. 碱处理调控ZSM-5孔结构及其在甲醇制芳烃中的性能研究[J]. 现代化工, 2019, 39(11): 67-72.
LI Zheng-hang, LIU Min, LI Jun-jie, GUO Xin-wen. Modification of ZSM-5 by alkali treatment and its performance in methanol to aromatics. Modern Chemical Industry, 2019, 39(11): 67-72.
链接本文:  
https://www.xdhg.com.cn/CN/10.16606/j.cnki.issn0253-4320.2019.11.015  或          https://www.xdhg.com.cn/CN/Y2019/V39/I11/67
[1] Zhang H,Cheng Y T,Vispute T P,et al.Catalytic conversion of biomass-derived feedstocks into olefins and aromatics with ZSM-5:The hydrogen to carbon effective ratio[J].Energy & Environmental Science,2011,4(6):2297-2307.
[2] Shen X,Kang J,Wei N,et al.Impact of hierarchical pore structure on catalytic performances of MFI zeolites modified by ZnO for the conversion of methanol to aromatics[J].Catalysis Science & Technology,2017,7(16):3598-3612.
[3] Bellussi G,Millini R,Pollesel P.An industrial perspective on the impact of haldor topsøe on research and development in catalysis by zeolites[J].Journal of Catalysis,2015,328:11-18.
[4] Inui T,Makino Y,Okazumi F,et al.Selective aromatization of light paraffins on platinum-ion-exchanged gallium-silicate bifunctional catalysts[J].Cheminform,1987,18(35):no-no.
[5] Gnep N S,Doyemet J Y,Seco A M,et al.Conversion of light alkanes to aromatic hydrocarbons:Ⅱ.Role of gallium species in propane transformation on GaZSM5 catalysts[J].Applied Catalysis,1988,43(1):155-166.
[6] Kim Y H,Lee K H,Nam C M,et al.Formation of hierarchical pore structures in Zn/ZSM-5 to improve the catalyst stability in the aromatization of branched olefins[J].Chemcatchem,2012,4(8):0-0.
[7] Wei Z,Xia T,Liu M,et al.Alkaline modification of ZSM-5 catalysts for methanol aromatization:The effect of the alkaline concentration[J].Frontiers of Chemical Science & Engineering,2015,9(4):450-460.
[8] Hutchings G J,Johnston P,Lee D F,et al.Acetone conversion to isobutene in high selectivity using zeolite β catalyst[J].Catalysis Letters,1993,21(1-2):49-53.
[9] Zaidi H A,Pant K K.Catalytic conversion of methanol to gasoline range hydrocarbons[J].Catalysis Today,2004,96(3):155-160.
[10] Zeng D,Yang J,Wang J,et al.Solid-state NMR studies of methanol-to-aromatics reaction over silver exchanged HZSM-5 zeolite[J].Microporous & Mesoporous Materials,2007,98(1):214-219.
[11] Adebajo M O,Long M A.The contribution of the methanol-to-aromatics reaction to benzene methylation over ZSM-5 catalysts[J].Catalysis Communications,2003,4(2):71-76.
[12] Zhang J,Qian W,Kong C,et al.Increasing para-xylene selectivity in making aromatics from methanol with a surface-modified Zn/P/ZSM-5 catalyst[J].ACS Catalysis,2015,5(5):2982-2988.
[13] Jia Y,Wang J,Kan Z,et al.Hierarchical ZSM-5 zeolite synthesized via dry gel conversion-steam assisted crystallization process and its application in aromatization of methanol[J].Powder Technology,2018,328:415-429.
[14] Dai C,Zhang A,Liu M,et al.Hollow ZSM-5 with silicon-rich surface,double shells,and functionalized interior with metallic nanoparticles and carbon nanotubes[J].Advanced Functional Materials,2015,25(48):7479-7487.
[15] Li J,Liu M,Guo X,et al.Interconnected hierarchical ZSM-5 with tunable acidity prepared by a dealumination-realumination process:A superior MTP catalyst[J].ACS Applied Materials & Interfaces,2017,9(31):26096-26106.
[16] Stian Svelle,Unni Olsbye,Finn Joensen A,et al.Conversion of methanol to alkenes over medium- and large-pore acidic zeolites:Steric manipulation of the reaction intermediates governs the ethene/propene product selectivity[J].Journal of Physical Chemistry C,2007,111(49):151-157.
[17] Bjørgen M,Svelle S,Joensen F,et al.Conversion of methanol to hydrocarbons over zeolite H-ZSM-5:On the origin of the olefinic species[J].Journal of Catalysis,2007,249(2):195-207.
[18] Milina M,Mitchell S,Crivelli P,et al.Mesopore quality determines the lifetime of hierarchically structured zeolite catalysts[J].Nature Communications,2014,5:3922.
[19] Dai C,Zhang A,Liu M,et al.Hollow alveolus-like nanovesicle assembly with metal-encapsulated hollow zeolite nanocrystals[J].ACS Nano,2016,10(8):7401-7408.
[20] Niu X,Gao J,Miao Q,et al.Influence of preparation method on the performance of Zn-containing HZSM-5 catalysts in methanol-to-aromatics[J].Microporous and Mesoporous Materials,2014,197:252-261.
[21] Chen J T,Chang W C.Effects of tissue culture conditions and explant characteristics on direct somatic embryogenesis in oncidium ‘gower ramsey’[J].Plant Cell Tissue & Organ Culture,2002,69(1):41-44.
[22] Chen J,Feng Z,Ying P,et al.ZnO clusters encapsulated inside micropores of zeolites studied by UV Raman and laser-induced luminescence spectroscopies[J].Journal of Physical Chemistry B,2004,108(34):12669-12676.
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[1] . [J]. Modern Chemical Industry, 2015, 35(8): 105 -108,110 .
[2] . [J]. Modern Chemical Industry, 2015, 35(8): 147 -150,152 .
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[6] . [J]. Modern Chemical Industry, 2015, 35(9): 131 -134 .
[7] . [J]. Modern Chemical Industry, 2015, 35(9): 135 -139 .
[8] . [J]. Modern Chemical Industry, 2015, 35(9): 146 -147 .
[9] . [J]. Modern Chemical Industry, 2015, 35(9): 156 -158 .
[10] . [J]. Modern Chemical Industry, 2015, 35(9): 165 -167,169 .
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