面向工业应用的焦炉煤气预加氢脱硫催化剂失活机理

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中文摘要：以焦炉煤气深度净化过程使用的预加氢转化新鲜催化剂和失活催化剂为研究对象，利用微型固定床反应装置对新鲜催化剂和再生催化剂进行加氢脱硫(HDS)活性评价，并采用N2-吸脱附仪、X射线衍射、Raman光谱、热重分析仪、扫描电子显微镜、电子能谱仪、紫外可见分光光度计和高频红外碳硫仪进行表征，深入研究了预加氢转化催化剂的积炭失活机理。研究结果发现，积炭覆盖催化剂表面活性位和堵塞催化剂孔道是导致预加氢转化催化剂失活的主要原因，同时积炭过程伴随活性组分(Fe和Mo)流失及再生过程中催化剂的烧结对催化剂失活也有贡献;积炭的形态以球形石墨化碳为主，其分布形式从催化剂内部向外逐渐增加;除异形条状和五齿球的失活催化剂外，其他催化剂再生(600℃，空气气氛)后可继续使用，再生后催化剂加氢活性下降，这主要是因为催化剂比表面积、孔容的下降及活性组分的流失。

外文标题：Deactivation mechanism of coke oven gas prehydrogenation desulfurization catalyst for industrial application

外文摘要：Taking the pre-hydrogenation conversion fresh catalyst and deactivated catalyst used in the deep purification process of coke oven gas as the research object,we used a micro-fixed-bed reaction device to carry out the hydrodesulfurization(HDS)activity evaluation.The carbon deposition and deactivation mechanisms of pre-hydrogenation reforming catalyst were explored by characterizations using N2-sorption desorption apparatus,X-ray diffraction(XRD),Raman spectroscopy,thermo-gravimetric analysis(TG-DTG),scanning electron microscope with energy dispersive spectrometer(SEM-EDS),UV-Vis spectroscopy and high-frequency infrared carbon-sulfur analyzer.The research result showed that the carbon deposition covering the active sites on the catalyst surface and the catalyst pore blocking were the main deactivation reasons.Meanwhile,the loss of active components(Fe and Mo)during the process of carbon deposition and the catalyst sintering during regeneration process also contributed to the deactivation of the catalysts.Secondly,the form of carbon deposition is dominated by spherical graphitic carbon,increasing gradually from the inside of the catalyst to outside.Finally,except for the catalysts of anisotropic strips and pentagonal spheres,other deactivated catalysts can be reused after regeneration(600℃,air atmosphere).However,the hydrotreating activity of the catalysts decreased after regeneration,mainly due to the reduction of the catalysts'surface,pore volume and the loss of active components.

外文关键词：

coke oven gasFeMo/Al2O3 catalysthydrodesulfurizationcatalyst cokingdeactivation mechanism

作者：

谭天兵、秦志峰、李乃珍、常丽萍、武蒙蒙、于峰、吴琼笑、陷艳莉、景建宁

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作者单位：

太原理工大学化学工程与技术学院,省部共建煤基能源清洁高效利用国家重点实验室,山西太原 030024

山西浙大新材料与化工研究院,山西太原 030002

山西道生鑫宇清洁能源有限公司,山西岢岚 036300

东莞市能源投资集团有限公司,广东东莞 523000

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关键词：

焦炉煤气 FeMo/Al2O3催化剂加氢脱硫催化剂积炭失活机理

基金：

2016年度山西省科技重大专项2018年度山西省优秀人才科技创新项目山西浙大新材料与化工研究院研发项目东莞市能源投资集团有限公司攻关项目

项目编号：

MJH2016-03201805D2110372021ST-AT-002RH2000004464

出版年：

2024

DOI：

10.16085/j.issn.1000-6613.2023-1656

化工进展

中国化工学会,化学工业出版社

化工进展

CSTPCD北大核心

影响因子：1.062

ISSN：1000-6613

年,卷(期)：2024.43(10)