文献类型：期刊文献

中文题名：富氧空位的非晶/晶态铁锰氧化物催化PET解聚

英文题名：Amorphous/crystalline Fe-Mn oxides with abundant oxygen vacancies for PET glycolysis

作者：贺昊[1];杨太顺[1];范庆明[1];王勃然[1];徐晶[1,2]

机构：[1]广西大学化学化工学院,广西石化资源加工与过程强化技术重点实验室,广西南宁530004;[2]华东理工大学化工学院,绿色化工与工业催化全国重点实验室,上海200237

年份：2026

卷号：45

期号：4

起止页码：2065

中文期刊名：化工进展

外文期刊名：Chemical Industry and Engineering Progress

收录：;EI(收录号：20262621019954);北大核心:【北大核心2023】；

基金：广西科技重大专项(桂科AA23062018);广西科技基地和人才专项(桂科AD23026311)。

语种：中文

中文关键词：聚对苯二甲酸乙二醇酯;催化;糖酵解;废物处理;氧空位;多相反应

外文关键词：polyethylene terephthalate;catalysis;glycolysis;waste treatment;oxygen vacancies;multiphase reaction

摘要：金属氧化物因其结构稳定、环境相容性好及制备简易性等优势,在催化聚对苯二甲酸乙二醇酯(PET)的乙二醇醇解(即PET糖酵解)过程中具有重要应用价值。然而,当前研究多聚焦于金属位点的构效关系,而对氧空位在催化过程中的作用机制尚未明晰。本文采用共沉淀与低温无氧煅烧合成了富含氧空位的非晶/晶态复合铁锰氧化物催化剂(MFO-1),并系统考察了其催化PET糖酵解的性能。通过多维度物化表征证实,MFO-1催化剂相较结晶态氧化物(MFO-2、MFO-3)与单金属氧化物(FFO),具有显著增强的比表面积(108m^(2)/g)与酸性位密度(1.41mmol/g)。其非晶/晶态异质界面通过结构畸变构筑氧空位缺陷,并与金属活性位点共同作用,实现了聚酯解聚路径的精准调控。在优化条件(催化剂∶PET=1∶100,乙二醇∶PET=10∶1,190℃反应1.5h)下,PET转化率达100%,对苯二甲酸双(2-羟乙基)酯产率达97.6%。催化剂借助本征磁响应机制可实现高效固液分离,经4次循环稳定性测试后,活性保持率超95%。本文通过调控催化剂电子微环境实现聚酯PET的高效解聚,为塑料升级回收催化剂设计提供了新范式。
Metal oxides,owing to their structural robustness,environmental compatibility,and facile synthesis protocols,exhibit significant potential in catalytic polyethylene terephthalate(PET)glycolysis.Current studies predominantly focus on the structure-activity relationships of metal sites,while the role of oxygen vacancies remains unclear.Herein,this article developed an oxygen vacancy-rich amorphous/crystalline Fe-Mn oxide(MFO-1)via coprecipitation and low-temperature oxygen-free calcination,and demonstrated its superior catalytic performance in PET glycolysis.Characterizations revealed that MFO-1 had higher specific surface area(108m^(2)/g)and surface acid site density(1.41mmol/g)than the crystalline oxides(MFO-2,MFO-3)and monometallic oxides(FFO).The unique amorphous-crystalline heterointerface promoted the oxygen vacancy formation via structural distortion,which could precisely regulate PET depolymerization pathways by synergizing with the metallic active sites.Under optimized conditions(catalyst∶PET=1∶100,EG∶PET=10∶1,190℃for 1.5h),100%PET conversion and 97.6%bis(2-hydroxyethyl)terephthalate selectivity were achieved.MOF-1 exhibited magnetic separability and retained over 95%of its initial catalytic activity after four consecutive operational cycles,demonstrating exceptional stability.This work achieved PET depolymerization by engineering the catalyst’s electronic microenvironment,which provided a novel paradigm for plastic upcycling catalyst design.