载体还原处理提高Ru/CeO_(2)催化对苯二甲酸加氢转化性能  

Enhancing Catalytic Activity of Ru/CeO_(2) in Terephthalic Acid Hydro-Conversion via Reduction Pre-Treatment of CeO_(2) Support

作　　者：彭宇轩 汪啸[3,4] 纪红艳[1,2] 吴雪婷 宋术岩 张洪杰 PENG Yu-Xuan;WANG Xiao;JI Hong-Yan;WU Xue-Ting;SONG Shu-Yan;ZHANG Hong-Jie(School of Rare Earths,University of Science and Technology of China,Hefei 230026,China;Ganjiang Innovation Academy,Chinese Academy of Sciences,Ganzhou 341119,China;School of Applied Chemistry and Engineering,University of Science and Technology of China,Hefei 230026,China;State Key Laboratory of Rare Earth Resource Utilization,Changchun Institute of Applied Chemistry,Chinese Academy of Sciences,Changchun 130022,China)

机构地区：[1]中国科学技术大学稀土学院,合肥230026 [2]中国科学院赣江创新研究院,赣州341119 [3]中国科学技术大学应用化学与工程学院,合肥230026 [4]中国科学院长春应用化学研究所,稀土资源利用国家重点实验室,长春130022

出　　处：《应用化学》2023年第11期1494-1503,共10页Chinese Journal of Applied Chemistry

基　　金：国家科技重大专项(No.2022YFB3504000);国家自然科学基金(Nos.22020102003,22025506,22271274);吉林省科技发展计划(Nos.20230101035JC,20230101022JC)资助。

摘　　要：聚对苯二甲酸乙二醇酯(PET)塑料可通过水解反应回收成对苯二甲酸(PTA)与乙二醇单体,后续PTA的综合利用具有一定的研究意义。本文以Ru/CeO_(2)多相催化PTA加氢转化为主要研究对象,通过将可变价氧化物CeO_(2)载体进行高温氢气还原预处理,尝试使其表面形成更多的氧缺陷与Lewis酸位点,以增强其催化PTA加氢转化反应中的活性。结果表明,经过高温氢气还原的CeO_(2)载体负载的Ru基催化剂在该反应中的催化活性显著优于未经过处理的样品,其在200~250℃下PTA转化率提高179%~300%,初步推测是由于高温氢气还原处理在载体表面构建了更多的氧缺陷与Lewis酸位点,增强了其对含有富电子芳环的反应物分子的吸附。本工作对于铈基氧化物多相催化剂的优化设计与表面调控具有一定的借鉴意义。Polyethylene terephthalate(PET)plastics can be recovered into terephthalic acid(PTA)and ethylene glycol monomers through hydrolysis reactions,and the comprehensive utilization of terephthalic acid has certain research significance.In this paper,Ru/CeO_(2) catalyzed PTA hydro-conversion reaction is researched.Attempts of generating more oxygen vacancies and Lewis acid sites on Ru/CeO_(2) by high-temperature reduction in H_(2) are made for boosting the catalytic activity in PTA hydro-conversion.Ru-based catalysts with pre-reduced CeO_(2) support exhibits significant enhanced activity in PTA hydro-conversion,as the PTA conversion is raised by 179%~300% under 200~250℃.The enhancement in catalytic activity by reduction pretreatment of CeO_(2) support is attributed to enhanced adsorption of PTA reactant due to newly generated Lewis acid sites.This work provides useful insights for rational design and precise surface regulation for Ce-based heterogeneous catalysts.

关 键 词：塑料升级回收 催化加氢 表面调控 稀土催化 

分 类 号：O611[理学—无机化学]