合成气直接转化制取芳烃研究进展

doi:10.1016/S1872-2067(19)63346-2

催化学报 ›› 2020, Vol. 41 ›› Issue (4): 561-573.DOI: 10.1016/S1872-2067(19)63346-2

• 中国科学院青年创新促进会专栏 • 上一篇下一篇

合成气直接转化制取芳烃研究进展

杨晓丽^a,b,c, 苏雄^a, 陈德^c, 张涛^a,b, 黄延强^a

a 中国科学院大连化学物理研究所, 辽宁大连 116023, 中国;
b 中国科学院大学, 北京 100049, 中国;
c 挪威科技大学化学工程系, 特隆赫姆7494, 挪威

收稿日期:2019-09-17 修回日期:2019-10-17 出版日期:2020-04-18 发布日期:2019-12-12
通讯作者: 黄延强
基金资助:
国家重点研发计划（2016YFA0202804）；中国科学院战略性先导科技专项（XDB17020400）；国家自然科学基金（21506204，21476226）；大连市杰出青年科学基金（2016RJ04）；中国科学院青年创新促进会.

Direct conversion of syngas to aromatics: A review of recent studies

Xiaoli Yang^a,b,c, Xiong Su^a, De Chen^c, Tao Zhang^a,b, Yanqiang Huang^a

a State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, Liaoning, China;
b University of Chinese Academy of Sciences, Beijing 100049, China;
c Department of Chemical Engineering, Norwegian University of Science and Technology, 7494 Trondheim, Norway

Received:2019-09-17 Revised:2019-10-17 Online:2020-04-18 Published:2019-12-12
Supported by:
The authors gratefully acknowledge the National Key R&D Program of China (2016YFA0202804), the Strategic Priority Research Program of the Chinese Academy of Sciences (XDB17020400), the National Natural Science Foundation of China (21506204, 21476226), Dalian Science Foundation for Distinguished Young Scholars (2016RJ04), and the Youth Innovation Promotion Association CAS for financial support.

摘要/Abstract

摘要： 芳烃类化合物是石化行业重要的基础原料.非石油基碳资源经合成气直接转化制取芳烃具有重要的应用前景，但该过程仍存在着芳烃收率低以及催化剂稳定性差等难题.近年来相关工作取得重要进展，研究人员尝试通过高效催化剂的设计和操作条件的优化以获得更好的催化反应性能.本综述首先对该过程进行了热力学分析，并根据催化剂体系对相关研究成果进行分类总结，主要包括改性FT催化剂和复合催化剂.然后，对各类催化剂体系的反应性能特点和机理进行了深入探讨.
改性FT催化剂常采用添加助剂或引入分子筛载体的方法调变反应中间体在传统FT催化剂上的反应路径，以促进芳烃的生成.但是，该过程倾向于生成链烃而致使芳烃选择性受到限制，而且容易形成积炭，催化剂稳定性差.复合催化剂可分为氧化物-分子筛和FT-分子筛催化剂，合成气首先在氧化物或者FT催化剂上生成某些亚稳态中间物种，随后扩散至分子筛孔道内经芳构化转化为芳烃.对于氧化物-分子筛复合催化剂，CO在氧化物上活化并生成醇类（主要是甲醇），随后在分子筛上进行C-C偶联、环化、芳构，生成芳烃.在该串联反应中，由于中间产物的不断转化，不仅使CO加氢反应的平衡右移，提升转化率，而且增加了芳烃的收率与反应的稳定性.另外，该过程CH₄产物的选择性极低.对于FT-分子筛复合催化剂，合成气首先在高温FT催化剂上生成低碳烃类，然后转移至分子筛孔道内进行芳构化，该方法可以获得较高的CO转化率但芳烃选择性仍比较低.
文章还详细描述了针对不同过程的反应器设计，包括单反应器和双反应器.在单反应器中可装填改性FT催化剂或物理混合的复合催化剂.对于复合催化剂，存在两种活性组分的优化反应条件不一致以及混合方式影响反应活性和产物分布等问题.因此，探索更佳的反应工艺条件对于实现合成气直接转化制芳烃的工业应用具有重要意义.双反应器则是将复合催化剂的两种功能组分分开装填，使分步过程分别在各自最佳反应条件下进行，从而避免了不匹配的问题.最后，该综述展望了合成气直接转化制芳烃过程存在的挑战和应用前景，为更好地设计催化剂、构建反应路径和优化工艺条件提供指导.

关键词: 合成气, 芳烃, 改性FT催化剂, 复合型催化剂, 反应器

Abstract: The direct catalytic conversion of syngas to aromatics offers a promising route to manufacture fine chemicals by employing non-petroleum carbon resources, because aromatic constituents are the key platform for producing polymers. However, this remains a great challenge due to the low yield of aromatics and poor catalyst stability, which restrict further development. In recent years, extensive research has been reported on the design of effective catalysts and the optimization of operating conditions to obtain better catalytic performance. In this review, we focus on these related achievements and present a comprehensive overview of different kinds of catalysts, mainly including modified Fischer-Tropsch (FT) catalysts and composite catalysts, as well as their performance and reaction mechanisms. The thermodynamic analysis of the reactions involved in this innovative conversion process and the comparison of different methods are also described in detail in this updated review. Finally, the challenges and prospects for direct syngas conversion are discussed to provide general guidelines for the construction of a well-designed reaction route.

Key words: Syngas, Aromatics, Modified FT catalyst, Composite catalyst, Reactor

中图分类号:

杨晓丽, 苏雄, 陈德, 张涛, 黄延强. 合成气直接转化制取芳烃研究进展[J]. 催化学报, 2020, 41(4): 561-573.

Xiaoli Yang, Xiong Su, De Chen, Tao Zhang, Yanqiang Huang. Direct conversion of syngas to aromatics: A review of recent studies[J]. Chinese Journal of Catalysis, 2020, 41(4): 561-573.

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合成气直接转化制取芳烃研究进展

Direct conversion of syngas to aromatics: A review of recent studies

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