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材料导报  2022, Vol. 36 Issue (17): 20080196-9    https://doi.org/10.11896/cldb.20080196
  无机非金属及其复合材料 |
有机硫水解催化剂研究进展
王明飞, 陈鹏, 陶雷, 薛宇, 刘敬业, 王学谦, 马懿星*, 王郎郎, 李佳奇
昆明理工大学环境科学与工程学院, 昆明 650500
Research Progress of Organic Sulfur Hydrolysis Catalyst
WANG Mingfei, CHEN Peng, TAO Lei, XUE Yu, LIU Jingye, WANG Xueqian, MA Yixing*, WANG Langlang, LI Jiaqi
Faculty of Environmental Science and Engineering, Kunming University of Science and Technology, Kunming 650500, China
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摘要 有机硫是焦炉煤气、天然气、黄磷尾气、合成氨等气体净化的重点和难点,其中羰基硫(COS)和CS2占主要部分。催化水解法被认为是净化工业气体中有机硫的有效途径之一,是一种低成本高效净化技术,能够在较低温度下将COS和CS2催化水解为H2S,进而对H2S进行高效脱除。催化水解法应用于工业精脱硫中具有两大优势:(1)转化率高,反应温度低,不消耗氢源;(2)水解产物H2S的净化工艺成熟,可进行硫资源的回收。
催化水解法已有较成熟的研究和工业应用,然而水解过程中的氧化反应是导致水解剂效率降低和寿命缩短的重要原因。因此,开发出廉价高效的水解催化剂成为本领域的研究热点,H2S的高选择性是有机硫催化水解的重要指标。
以γ-Al2O3、活性炭作为载体制备的水解催化剂是目前应用效果较好的催化剂,且γ-Al2O3的应用最早、最广泛,但其抗氧能力较差、催化剂易中毒等特点使其在应用过程中受到一定限制。TiO2、ZrO2等载体在近几年的研究工作受到关注,不同活性组分的添加为突破水解催化剂对H2S的低选择性和抗毒性提供了可能。此外有机硫水解机理的探究也为水解催化剂的开发提供了理论依据,在此基础上调控反应路径,改善水解过程中多种影响因素,也有助于有机硫水解催化剂活性和寿命的双提升。
本文介绍了COS和CS2催化水解的主要载体和活性组分的研究和应用情况,分别对有机硫水解机理和水解催化剂失活原因进行了总结和归纳,分析了催化水解法在应用中面临的问题并展望其前景,以期为新型高效水解催化材料的设计提供参考。
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王明飞
陈鹏
陶雷
薛宇
刘敬业
王学谦
马懿星
王郎郎
李佳奇
关键词:  有机硫  催化水解  催化剂  水解机理  失活    
Abstract: Organic sulfur is the key and difficult point in the purification of coke oven gas, natural gas, yellow phosphorus tail gas, synthetic ammonia and other gases, among which COS and CS2 account for the main part. Catalytic hydrolysis is considered to be one of the most effective ways to purify organic sulfur in industrial gases, which is a low-cost and high-efficiency purification technology. COS and CS2 can be converted to H2S by catalytic hydrolysis at lower temperature, and H2S can be then removed efficiently. There are two major advantages for refined desulfurization by catalytic hydrolysis: (i) high conversion rate, low reaction temperature, and no hydrogen source consumption; (ii) mature purification process of the hydrolysate H2S, which can be used for the recovery of sulfur resources.
Catalytic hydrolysis has been well studied and applied in industry, but the oxidation reaction in the hydrolysis process is an important reason for the reduction of the efficiency and life of the hydrolysis catalyst. Therefore, the development of cheap and efficient hydrolysis catalysts has become a research hotspot in this field. Moreover, high selectivity of H2S is a core indicator of organic sulfur hydrolysis catalysis.
The hydrolysis catalysts prepared with γ-Al2O3 and activated carbon as support are the catalysts with a better application effect at present. Besides, the application of γ-Al2O3 is the earliest and most extensive, but its poor antioxidant capacity and catalyst poisoning characteristics make it limited in the application process. Supports such as TiO2 and ZrO2 have been followed with interest in recent years, and the addition of different active components provides the possibility to break through the low selectivity of H2S and anti-toxicity. In addition, the study on the mechanism of organic sulfur hydrolysis also provides a theoretical basis for the development of hydrolytic catalysts. On this basis, the activity and life of organic sulfur hydrolysis catalysts can be improved by adjusting the reaction path and improving influencing factors in the hydrolysis process.
This review introduces the research and application of the main supports and active components on COS and CS2 catalytic hydrolysis. The hydrolysis mechanism of organic sulfur and hydrolysis catalyst deactivation reason has also been summarized, and the problems faced and future prospect of the catalytic hydrolysis method are analyzed. It is hoped that this paper can provide reference for the design of new high efficiency hydrolytic catalytic materials.
Key words:  organic sulfur    catalytic hydrolysis    catalyst    hydrolysis mechanism    deactivation
出版日期:  2022-09-10      发布日期:  2022-09-10
ZTFLH:  X511  
基金资助: 国家自然科学基金(21876071;51868030);云南省科技厅科技计划项目(2019FD043)
通讯作者:  *mayixing99@kust.edu.cn   
作者简介:  王明飞,2019年6月毕业于河南城建学院,获得工学学士学位。现为昆明理工大学环境科学与工程学院硕士研究生,在马懿星教授的指导下进行研究。目前主要研究领域为工业废气净化。
马懿星,昆明理工大学环境科学与工程学院副教授、研究生导师,主要从事大气污染控制研究。2011年本科毕业于华中科技大学环境科学与工程学院,2016年博士毕业于昆明理工大学环境科学与工程学院,发表论文30余篇,申请专利20余项,曾获中国有色金属工业技术发明奖等奖项。
引用本文:    
王明飞, 陈鹏, 陶雷, 薛宇, 刘敬业, 王学谦, 马懿星, 王郎郎, 李佳奇. 有机硫水解催化剂研究进展[J]. 材料导报, 2022, 36(17): 20080196-9.
WANG Mingfei, CHEN Peng, TAO Lei, XUE Yu, LIU Jingye, WANG Xueqian, MA Yixing, WANG Langlang, LI Jiaqi. Research Progress of Organic Sulfur Hydrolysis Catalyst. Materials Reports, 2022, 36(17): 20080196-9.
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http://www.mater-rep.com/CN/10.11896/cldb.20080196  或          http://www.mater-rep.com/CN/Y2022/V36/I17/20080196
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