| 无溶剂路线制备分子筛封装的钴基催化剂及其在费托合成制汽油反应中的应用（英文） |
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| 引用本文： | Mudassar Javeda,程世林,张桂华,Cederick Cyril Amooa,汪婧妍,吕鹏,吕成学,邢闯,孙剑,椿范立.无溶剂路线制备分子筛封装的钴基催化剂及其在费托合成制汽油反应中的应用（英文）[J].催化学报,2020(4):604-612. |
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| 作者姓名： | Mudassar Javeda 程世林 张桂华 Cederick Cyril Amooa 汪婧妍 吕鹏 吕成学 邢闯 孙剑 椿范立 |
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| 作者单位： | 浙江科技学院生物与化学工程学院;北京兴高化学技术有限公司;富山大学工学部;中国科学院大连化学物理研究所洁净能源国家实验室（筹） |
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| 基金项目： | the financial support from the Zhejiang Province Natural Science Foundation(LY19B060001);the Foundation of State Key Laboratory of High-efficiency Utilization of Coal and Green Chemical Engineering(2018-K25);the Foundation of Zhejiang University of Science and Technology(2019QN18,2019QN23)~~ |
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| 摘 要： | 自2012年浙江大学肖丰收教授(J.Am.Chem.Soc.,2012,134,15173-15176)首次提出无溶剂法合成分子筛以来,该路线已备受关注.无溶剂合成分子筛方法具有废液少、产率高、安全系数高等优点.本文针对合成气经费托路线(FTS)一步法制备富含异构烷烃汽油馏分的研究,通过无溶剂研磨法制备了分子筛封装金属催化剂.一般来说,烷烃异构化催化剂的性能主要取决于分子筛的孔道结构及其酸性,其次是分子筛晶粒大小、结晶度和表面性质等因素.本文对比了三种具有相同拓扑结构的MFI分子筛(Silicalite-1,HZSM-5和NaZSM-5)对汽油和异构烷烃选择性的影响规律.结果显示,在CO转化率(~30%)近似相同的情况下,具有最弱酸性的Silicalite-1封装的Co颗粒表现出最高的汽油选择性(~70%)和异构烷烃选择性(~30.7%).这意味着正构烷烃异构化反应只需要弱酸即可实现,较强的酸性则会使其发生过度裂解反应.Py-IR谱图显示,Silicalite-1在1445 cm-1附近的L酸是区别于NaZSM-5和HZSM-5的一个重要酸性位,可作为FTS路线制备富含异构烷烃汽油的一个关键参数.另外,与封装型(Co@MFI)催化剂相比,浸渍型催化剂(Co/MFI)的汽油选择性明显偏低,可能与金属活性位与分子筛酸性位之间的距离有直接关系.因此,无溶剂合成分子筛是一条具有前景和适宜放大的催化剂合成路线.对于合成气经费托路线制取富含异构烷烃汽油反应,正构烷烃在分子筛催化剂上的裂解和异构化之间的竞争反应是核心问题.未来有待突破的研究方向包括:(1)多支链异构烷烃的合成,目前对于有效调控多支链烷烃的生成关注较少;(2)反应路线的设计,合成气经甲醇路线,联合甲醇制汽油(MTG)反应获得异构烷烃;(3)裂解反应的抑制;(4)分子筛孔道/笼对异构烷烃选择性的调控机制.
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| 关 键 词： | 无溶剂合成 分子筛封装 钴催化剂 费托合成 汽油 异构烷烃 |
A facile solvent-free synthesis strategy for Co-imbedded zeolite-based Fischer-Tropsch catalysts for direct gasoline production |
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| Institution: | (School of Biological and Chemical Engineering,Zhejiang University of Science and Technology,Hangzhou 310023,Zhejiang,China;Dalian National Laboratory for Clean Energy,Dalian Institute of Chemical Physics,Chinese Academy of Sciences,Dalian 116023,Liaoning,China;Beijing Booming Highchem Technology Co.,LTD,Beijing 100005,China;Department of Applied Chemistry,Graduate School of Engineering,University of Toyama,Gofuku 3190,Toyama 9308555,Japan) |
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| Abstract: | A series of Co-imbedded zeolite-based catalysts were synthesized following a facile solvent-free grinding route.The catalytic performance for direct syngas conversion to gasoline range hydrocarbons was compared with their counterpart Co-impregnated zeolite-based catalysts.Successful transformation of solid raw materials to targeted zeolite was confirmed by XRD,SEM,STEM,and N2 physisorption analysis.An in-depth study of acidic strength and acidic site distribution was conducted by NH3-TPD and Py-IR spectroscopy.Acidic strength showed a pivotal role in defining product range.Co@S1,with the weakest acidic strength of silicalite-1 among three types of zeolites,evaded over-cracking of product and exhibited the highest gasoline and isoparaffin selectivity(≈70%and 30.7%,respectively).Moreover,the solvent-free raw material grinding route for zeolite synthesis accompanies several advantages like the elimination of production of wastewater,high product yield within confined crystallization space,and elimination of safety concerns regarding high pressure due to the absence of the solvent.Facileness and easiness of the solvent-free synthesis route together with promising catalytic performance strongly support its application on the industrial scale. |
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| Keywords: | Solvent-free synthesis Co-imbedded zeolite catalyst Fischer-Tropsch synthesis Gasoline Isoparaffin |
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