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Catalytic upgrading of coal pyrolysis volatiles by Ga-substituted mesoporous ZSM-5

机译：GA-替代的介孔ZSM-5催化升级煤热解挥发物

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摘要

Five MFI-type zeolite catalysts, which were aluminosilicate ZSM-5 (Z5), gallium-substituted silicalite-1 (Ga-S1), mesoporous ZSM-5 (MZ5), gallium-substituted mesoporous silicalite-1 (Ga-MS1) and gallium-substituted mesoporous ZSM-5 (Ga-MZ5), were hydrothermally synthesized with combined using of TPAOH and TPOAC as micropore and mesopore structure-directing agents respectively, followed by the application in the catalytic upgrading of volatiles from low-rank coal fast pyrolysis. The obtained results indicated that significant improvements with the yield of high value-added products of BTEXN (benzene, toluene, ethylbenzene, xylene and naphthalene) increased from 5.4 mg.g(-1 )to 11.9-26.4 mg.g(-1), as well as the content of light fractions ( 300 degrees C) in coal tars increased from 51% to 65-88% were realized by using the representative MFI-type zeolite catalysts in contrast to non-catalyst pyrolysis. Moreover, the possible mechanism for catalytic upgrading over the best-performing catalyst of gallium-substituted mesoporous ZSM-5 (Ga-MZ5) with the highest yield of aromatics and effective reduction of phenols was proposed on the basis of systematic comparison of structural features and catalytic performances of various MFI-type zeolite catalysts and fundamental study of the synergetic effects dominated by acidity, ratio of Bronsted/Lewis acid sites, intra-/extra-framework gallium species and hierarchical meso-/microporosity.
机译：五种MFI型沸石催化剂，其是铝硅酸盐ZSM-5（Z5），镓取代的硅沸石-1（Ga-S1），中孔ZSM-5（MZ5），镓取代的介孔硅沸石-1（GA-MS1）和镓取代的介孔ZSM-5（GA-MZ5）分别用TPAOH和TPOAC作为微孔和中孔结构引导剂的组合使用，然后在低级煤快速热解中的催化升级中的应用。所得结果表明，对Btexn（苯，甲苯，乙苯，二甲苯和萘）的高附加值产物的产率显着改善，从5.4 mg.g（-1）增加到11.9-26.4 mg.g（-1）并且通过使用代表性MFI型沸石催化剂与非催化剂热解对比，煤焦油中的光级分（<300℃）的含量从51％增加到65-88％。此外，基于结构性特征的系统比较，提出了在结构特征的系统比较和催化促进最佳性溶解的介孔ZSM-5（GA-MZ5）和有效减少酚类催化剂的最佳性能催化催化机制。各种MFI型沸石催化剂的催化性能和由酸度，耐骨架/路易斯酸盐酸的比例，/超框架内镓物种和分级式/微孔占的协同作用的基本研究。

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  • 来源
    《Fuel》 |2020年第may1期|117217.1-117217.11|共11页
  • 作者

    Bi Chenyao; Wang Xu; You Qing; Liu Baoyu; Li Zhuo; Zhang Jianbo; Hao Qingqing; Sun Ming; Chen Huiyong; Ma Xiaoxun;

  • 作者单位

    Northwest Univ Sch Chem Engn Xian 710069 Shaanxi Peoples R China;

    Northwest Univ Sch Chem Engn Xian 710069 Shaanxi Peoples R China;

    Northwest Univ Sch Chem Engn Xian 710069 Shaanxi Peoples R China;

    Guangdong Univ Technol Sch Chem Engn & Light Ind Guangzhou 510006 Guangdong Peoples R China;

    Northwest Univ Sch Chem Engn Xian 710069 Shaanxi Peoples R China;

    Northwest Univ Sch Chem Engn Xian 710069 Shaanxi Peoples R China|Northwest Univ Chem Engn Res Ctr Shaanxi Res Ctr Engn Technol Clean Coal Convers Minist Educ Adv Use Technol Shanbei Energy Xian 710069 Shaanxi Peoples R China|Collaborat Innovat Ctr Dev Energy & Chem Ind Nort Int Sci & Technol Cooperat Base MOST Clean Utiliz Xian 710069 Shaanxi Peoples R China;

    Northwest Univ Sch Chem Engn Xian 710069 Shaanxi Peoples R China|Northwest Univ Chem Engn Res Ctr Shaanxi Res Ctr Engn Technol Clean Coal Convers Minist Educ Adv Use Technol Shanbei Energy Xian 710069 Shaanxi Peoples R China|Collaborat Innovat Ctr Dev Energy & Chem Ind Nort Int Sci & Technol Cooperat Base MOST Clean Utiliz Xian 710069 Shaanxi Peoples R China;

    Northwest Univ Sch Chem Engn Xian 710069 Shaanxi Peoples R China|Northwest Univ Chem Engn Res Ctr Shaanxi Res Ctr Engn Technol Clean Coal Convers Minist Educ Adv Use Technol Shanbei Energy Xian 710069 Shaanxi Peoples R China|Collaborat Innovat Ctr Dev Energy & Chem Ind Nort Int Sci & Technol Cooperat Base MOST Clean Utiliz Xian 710069 Shaanxi Peoples R China;

    Northwest Univ Sch Chem Engn Xian 710069 Shaanxi Peoples R China|Northwest Univ Chem Engn Res Ctr Shaanxi Res Ctr Engn Technol Clean Coal Convers Minist Educ Adv Use Technol Shanbei Energy Xian 710069 Shaanxi Peoples R China|Collaborat Innovat Ctr Dev Energy & Chem Ind Nort Int Sci & Technol Cooperat Base MOST Clean Utiliz Xian 710069 Shaanxi Peoples R China;

    Northwest Univ Sch Chem Engn Xian 710069 Shaanxi Peoples R China|Northwest Univ Chem Engn Res Ctr Shaanxi Res Ctr Engn Technol Clean Coal Convers Minist Educ Adv Use Technol Shanbei Energy Xian 710069 Shaanxi Peoples R China|Collaborat Innovat Ctr Dev Energy & Chem Ind Nort Int Sci & Technol Cooperat Base MOST Clean Utiliz Xian 710069 Shaanxi Peoples R China;

  • 收录信息 美国《科学引文索引》(SCI);美国《工程索引》(EI);
  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类
  • 关键词

    Coal volatiles; Catalytic upgrading; Mesoporous zeolite; MFI; Gallium substitution;

    机译：煤挥发物;催化升级;中孔沸石;MFI;镓替代;

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