丙烷直接脱氢催化剂的研究进展

doi:10.1016/S1872-2067(19)63360-7

催化学报 ›› 2019, Vol. 40 ›› Issue (9): 1233-1254.DOI: 10.1016/S1872-2067(19)63360-7

丙烷直接脱氢催化剂的研究进展

胡忠攀^a, 杨丹丹^a, 王政^b, 袁忠勇^a

a 南开大学材料科学与工程学院新催化材料科学研究所, 先进能源材料化学教育部重点实验室, 天津 300350;
b 宁夏大学化学化工学院, 省部共建煤炭高效利用与绿色化工国家重点实验室, 宁夏银川 750021

收稿日期:2019-01-28 出版日期:2019-09-18 发布日期:2019-07-06
通讯作者: 袁忠勇
基金资助:
国家自然科学基金（21421001，21573115）；中央高校基本科研业务费专项资金（63185015）；煤炭高效利用与绿色化工国家重点实验室基金（2017-K13）.

State-of-the-art catalysts for direct dehydrogenation of propane to propylene

Zhong-Pan Hu^a, Dandan Yang^a, Zheng Wang^b, Zhong-Yong Yuan^a

a Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), Institute of New Catalytic Materials Science, School of Materials Science and Engineering, Nankai University, Tianjin 300350, China;
b State Key Laboratory of High-Efficiency Utilization of Coal and Green Chemical Engineering, College of Chemistry and Chemical Engineering, Ningxia University, Yinchuan 750021, Ningxia, China

Received:2019-01-28 Online:2019-09-18 Published:2019-07-06
Contact: S1872-2067(19)63360-7
Supported by:
This work was supported by the National Natural Science Foundation of China (21421001, 21573115), the Fundamental Research Funds for the Central Universities (63185015), and the Foundation of State Key Laboratory of High-Efficiency Utilization of Coal and Green Chemical Engineering (2017-K13).

摘要/Abstract

摘要： 丙烯是一种重要化工原料，可以用于生产聚丙烯、丙烯腈、丙烯酸、甘油及异丙醇等化学品.近年来，随着丙烯下游产品需求量的增加，传统丙烯生产技术（石油催化裂解、石脑油催化裂化）难以满足日益增长的丙烯需求，寻求新的丙烯生产技术成为石油化工行业的重要趋势.另外，由于美国页岩气开采技术日益成熟，大量廉价的丙烷被开采出来.丙烷直接脱氢制丙烯成本大大降低，并逐渐成为丙烯生产来源的一个重要方面.丙烷脱氢工艺中最重要的就是催化剂的制备和研究，常见的丙烷脱氢催化剂为CrO_x基催化剂和Pt基催化剂体系，并被广泛应用于工业丙烷脱氢体系.但是，Cr基催化剂积碳严重，需要反复再生；而Pt基催化剂价格昂贵，且Pt颗粒容易发生团聚而发生不可逆失活.因此，提高现有CrO_x基和Pt基催化剂的稳定性或开发新型替代型丙烷脱氢催化剂成为提高丙烷脱氢工艺的关键.
本文综述了近年来丙烷直接脱氢制丙烯催化剂的研究进展，详细讨论了不同催化剂（包括Pt，CrO_x，VO_x，GaO_x，ZnO，FeO_x，CoO_x，SnO_x，ZrO₂基催化剂和碳基催化剂）的活性位点、催化机理及助剂类型和载体种类等对催化剂性能的影响.研究表明，丙烷脱氢催化剂的催化性能与活性物种的分散性和催化剂酸性关系很大.一般而言，活性物种分散性越高，催化剂的催化性能越好.而酸性过高会影响丙烯的脱附过程，因而会导致丙烷的深度脱氢、裂解或积碳的形成.因此，提高活性位的分散性和调节催化剂酸性是目前丙烷脱氢催化剂研究的重要方面.最近的一些研究主要集中在制备单分散（单原子）或双原子合金催化剂用于丙烷脱氢，大大提高催化剂的稳定性.
目前，CrO_x基和Pt基催化剂仍是丙烷脱氢反应的主要催化剂，提高它们的活性、稳定性、选择性和抗积碳能力仍是丙烷脱氢工艺研究的重要方面.另外，一些新型负载型金属氧化物（如VO_x，GaO_x，FeO_x，CoO_x，SnO_x，ZnO_x，ZrO_x）和纳米碳材料（介孔碳、碳纳米管和生物质碳）被发现是良好的丙烷脱氢催化剂.但是，这些催化剂也面临失活严重和循环性差等问题.因此，未来的研究目标需要集中在以下几方面：（1）开发新型制备工艺，提高催化剂稳定性；（2）明确催化剂活性位点、催化机理和构效关系；（3）明确催化剂失活和再生循环机制；（4）发展原位或operando技术监测丙烷脱氢催化剂的实时变化情况.

关键词: 丙烷脱氢, 丙烯, 非均相催化剂, 活性位, 催化机理

Abstract: With growing demand for propylene and increasing production of propane from shale gas, the technologies of propylene production, including direct dehydrogenation and oxidative dehydrogenation of propane, have drawn great attention in recent years. In particular, direct dehydrogenation of propane to propylene is regarded as one of the most promising methods of propylene production because it is an on-purpose technique that exclusively yields propylene instead of a mixture of products. In this critical review, we provide the current investigations on the heterogeneous catalysts (such as Pt, CrO_x, VO_x, GaO_x-based catalysts, and nanocarbons) used in the direct dehydrogenation of propane to propylene. A detailed comparison and discussion of the active sites, catalytic mechanisms, influencing factors (such as the structures, dispersions, and reducibilities of the catalysts and promoters), and supports for different types of catalysts is presented. Furthermore, rational designs and preparation of high-performance catalysts for propane dehydrogenation are proposed and discussed.

Key words: Propane dehydrogenation, Propylene, Heterogeneous catalyst, Active site, Catalytic mechanism

胡忠攀, 杨丹丹, 王政, 袁忠勇. 丙烷直接脱氢催化剂的研究进展[J]. 催化学报, 2019, 40(9): 1233-1254.

Zhong-Pan Hu, Dandan Yang, Zheng Wang, Zhong-Yong Yuan. State-of-the-art catalysts for direct dehydrogenation of propane to propylene[J]. Chinese Journal of Catalysis, 2019, 40(9): 1233-1254.

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丙烷直接脱氢催化剂的研究进展

State-of-the-art catalysts for direct dehydrogenation of propane to propylene

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