负载型过渡金属催化剂催化转移加氢脱氯研究  

Dechlorination by catalytic transfer hydrogenation with supported transition metal catalysts

作　　者：闫紫豪 裴亚宁 唐家璇 任铂洋 刘晨 张伟 张登前 习远兵 YAN Zihao;PEI Yaning;TANG Jiaxuan;REN Boyang;LIU Chen;ZHANG Wei;ZHANG Dengqian;XI Yuanbing(Beijing Key Laboratory of Fuels Cleaning and Advanced Catalytic Emission Reduction Technology,College of New Materials and Chemical Engineering,Beijing Institute of Petrochemical Technology,Beijing 102617;Sinopec Research Institute of Petroleum Processing Co.,Ltd.,Beijing 100083)

机构地区：[1]北京石油化工学院新材料与化工学院,燃料清洁化及高效催化减排技术北京市重点实验室,北京102617 [2]中石化石油化工科学研究院有限公司,北京100083

出　　处：《环境污染与防治》2024年第12期1760-1766,共7页Environmental Pollution & Control

基　　金：国家能源石油炼制技术研发中心(中石化石油化工科学研究院有限公司)开放基金课题(No.202301);北京市大学生科研训练项目(No.2023J00132)。

摘　　要：废塑料热解回收既可以避免“白色污染”,还可以实现其高值化利用,然而塑料热解油中有机氯脱除是亟待解决的问题。以异丙醇为供氢试剂,采用等体积浸渍法制备高活性的负载型过渡金属催化剂进行催化转移加氢(CTH)脱氯,考察催化剂组成、焙烧温度、还原温度、反应温度、供氢试剂用量对CTH脱氯效果的影响。结果表明,对于不同类型的金属催化剂,1Pt/SiO_(2)(SiO_(2)上负载质量分数为1%的Pt)的催化活性最高,脱氯率达到73.3%。向1Pt/SiO_(2)掺杂适量Ni,其催化活性可进一步提高。当1Pt/SiO_(2)中Ni掺杂量为10%(质量分数),催化剂焙烧温度为400℃,还原温度为350℃,反应温度为100℃,异丙醇与有机氯摩尔比为25∶1时,脱氯率最高,达到92.7%。催化剂的表征结果显示,掺杂Ni改变了催化剂表面上Pt的电子结构和活性位点分布,并且Ni对比其他金属,具有更高的加氢活性,从而使催化剂具有较高的催化活性。The pyrolysis recovery of waste plastics can not only avoid“white pollution”,but also realize its high-value utilization.However,the removal of organic chlorine in plastic pyrolysis oil is an urgent problem to be solved.Highly active supported transition metal catalysts were prepared by incipient-wetness impregnation method for dechlorination by catalytic transfer hydrogenation(CTH)using isopropanol as the hydrogen donor,and the effects of catalyst composition,calcination temperature,reduction temperature,reaction temperature and the dosage of isopropanol on the dechlorination performances by CTH were investigated.The results showed that among different types of supported metal catalysts,1Pt/SiO_(2)(Pt with mass fraction of 1%loading on SiO_(2))showed the best catalytic performance and the chlorine removal efficiency reached 73.3%.By doping 1Pt/SiO_(2)with appropriate content of Ni,its catalytic performance could be improved.The highest chlorine removal efficiency of 92.7%was achieved when Ni doping amount was 10%(mass fraction),calcination temperature was 400℃,reduction temperature was 350℃,reaction temperature was 100℃and the molar ratio of isopropanol to organochlorine was 25∶1.The characterization results showed that the doping of Ni changed the electronic structure and dispersion of Pt on the catalyst surface.In addition,Ni had superior hydrogenation activity,which led to higher catalytic activity of the catalyst.

关 键 词：脱氯 PT 催化剂 催化转移加氢 塑料热解油 

分 类 号：TQ426[化学工程] X705[环境科学与工程—环境工程]