在介孔HZSM-5负载的钌催化剂上对PET降解化学品中的苯环进行氢化。

Hydrogenation of the benzene rings in PET degraded chemicals over meso-HZSM-5 supported Ru catalyst.

作者信息

Ou Weitao, Wang Han, Ye Yingdan, Zhao Huaiyuan, Zhang Yibin, Hou Zhaoyin

机构信息

Key Laboratory of Biomass Chemical Engineering of Ministry of Education, Department of Chemistry, Zhejiang University, Hangzhou 310028, China.

Zhejiang Hengyi Petrochemical Research Institute Co., Ltd., Hangzhou 311200, China.

出版信息

J Hazard Mater. 2024 Sep 5;476:134964. doi: 10.1016/j.jhazmat.2024.134964. Epub 2024 Jun 19.

DOI:10.1016/j.jhazmat.2024.134964

PMID:38901261

Abstract

Chemical upcycling of waste polyethylene terephthalate (PET) to value-added products can reduce the emission of CO, microplastics and toxic chemicals. In this work, mesoporous H-type Zeolite Socony Mobil-5 (HZSM-5) supported Ru catalyst (Ru/m-HZSM-5) was synthesized and tested in the hydrogenation of PET degraded chemicals (bis(2-hydroxyethyl) terephthalate, dimethyl terephthalate, diethyl terephthalate, and terephthalic acid). Characterizations disclosed that Ru/m-HZSM-5 catalyst possesses mesopores (a dominant channel of 5.32 nm), enlarged specific surface area (404 m·g), and Ru NPs dispersed highly (40.6 %) compared to that of Ru/HZSM-5. And also, it was found that Ru/m-HZSM-5 was capable for the hydrogenation of benzene rings in these PET degraded chemicals with large sizes (1.09-1.82 nm). In particular, the conversion of BHET and the selectivity of BHCD over Ru/m-HZSM-5 reached 95.5 % and 95.6 % at 120 °C within 2 h. And Ru/m-HZSM-5 could be recycled at least five times without obvious loss of activity and selectivity.

摘要

将废弃聚对苯二甲酸乙二酯（PET）化学升级循环转化为增值产品可以减少一氧化碳、微塑料和有毒化学品的排放。在这项工作中，合成了介孔H型ZSM-5分子筛（HZSM-5）负载的Ru催化剂（Ru/m-HZSM-5），并对PET降解产物（对苯二甲酸双（2-羟乙基）酯、对苯二甲酸二甲酯、对苯二甲酸二乙酯和对苯二甲酸）进行了加氢测试。表征结果表明，与Ru/HZSM-5相比，Ru/m-HZSM-5催化剂具有介孔（主导通道为5.32 nm）、更大的比表面积（404 m²/g）以及高度分散的Ru纳米颗粒（40.6%）。此外，发现Ru/m-HZSM-5能够对这些尺寸较大（1.09 - 1.82 nm）的PET降解产物中的苯环进行加氢反应。特别是，在120℃、2小时内，Ru/m-HZSM-5上BHET的转化率和BHCD的选择性分别达到95.5%和95.6%。并且Ru/m-HZSM-5至少可以循环使用五次，而活性和选择性没有明显损失。