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天然气脱硫工艺羰基硫水解催化剂失活研究 被引量:1

Study on deactivation of carbonyl sulfide hydrolysis catalyst in natural gas desulfurization process
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摘要 为研究羰基硫水解催化剂的失活机理,对PG新剂及旧剂进行了表征。低温氮气吸脱附实验表明:PG新剂比表面积大于330m^(2)/g,使用后催化剂比表面积降低20%以上,平均孔径增大,孔体积略有减小。SEM(扫描电子显微镜)照片表明:新鲜剂表面颗粒形貌均匀,失活催化剂比表面积减小,孔体积减小,孔道变大。XRD(X射线衍射)结果表明:PG新剂主要由AlO(OH)和Al_(2)O_(3)两种晶相构成,使用后催化剂除AlO(OH)相外,均新增Al(OH)_(3)相,且随床层高度下移,Al(OH)_(3)衍射峰强度逐渐削弱。XRF(X射线荧光法)结果表明:PG新剂主要组成为氧化铝和少量氧化钠,反应后催化剂上积聚了一定量的含碳、氮和硫的物质,且氧化钠的含量有所降低。CO_(2)-TPD(CO_(2)程序升温脱附)结果表明:PG新剂上存在丰富的弱碱性中心,而反应后催化剂上硫等杂质的沉积导致弱碱性中心数量显著减少。 In order to study the deactivation mechanism of carbonyl sulfide hydrolysis catalyst, the new and old PG catalyst were characterized. Low temperature nitrogen adsorption and desorption experiments show that the specific surface area of PG new agent is greater than 330 m^(2)/g, and the specific surface area of used catalyst is reduced by more than 20%, the average pore size increased and the pore volume decreased slightly. SEM results show that the surface particle morphology of the fresh agent is uniform, the specific surface area of the deactivated catalyst decreases, the pore volume decreases and the pore channel becomes larger.XRD results show that the PG new agent is mainly composed of two crystalline phases of AlO(OH) and Al_(2)O_(3), Al(OH)_(3)phase is added to the used catalyst except for AlO(OH) phase, and the diffraction peak intensity of Al(OH);decreases gradually with the height of the bed moving down. XRF results show that the PG new agent is mainly composed of Al_(2)O_(3)and a small amount of Na_(2)O, a certain amount of species containing carbon, nitrogen and sulfur are accumulated on the catalyst, and the content of Na_(2)O decreased. The results of CO_(2)-TPD show that there are abundant weak alkaline centers on the PG new agent, and the deposition of sulfur and other impurities on the catalyst after the reaction results in a significant reduction in the number of weak alkaline centers.
作者 刘剑利 朱春蕾 刘爱华 刘增让 徐翠翠 宋宛霖 王国玮 Liu Jianli;Zhu Chunlei;Liu Aihua;Liu Zengrang;Xu Cuicui;Song Wanlin;Wang Guowei(Research Institute of SINOPEC Qilu Petrochemical Company,Zibo,Shandong 255400;State Key Laboratory of Heavy Oil Processing,China University of Petroleum(East China),Qingdao,Shandong 266580)
出处 《炼油技术与工程》 CAS 2022年第6期27-30,63,共5页 Petroleum Refinery Engineering
关键词 天然气脱硫工艺 羰基硫水解 催化剂失活 低温氮气吸脱附 SEM XRD XRF CO -TPD natural gas desulfurization process carbonyl sulfide hydrolysis catalyst deactivation low temperature nitrogen adsorption and desorption SEM XRD XRF CO_(2)-TPD
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