Construction and extension of carbon network conjugated systems under high temperature regeneration for cycling degradation of Naproxen by activating peroxymonosulfate: mechanisms of active sites self-cycling and reactive oxygen species regulation
{"title":"Construction and extension of carbon network conjugated systems under high temperature regeneration for cycling degradation of Naproxen by activating peroxymonosulfate: mechanisms of active sites self-cycling and reactive oxygen species regulation","authors":"Zexin Zhu, Meng Li, Yintao Shi, Hao Zhang, Huiyuan Deng, Dongsheng Xia","doi":"10.1016/j.jclepro.2024.144510","DOIUrl":null,"url":null,"abstract":"The development of metal-free catalysts with excellent reusability and the research of effects for carbon network structures in activation process are great challenges in non-metallic catalysis today. In this study, a regenerated metal-free biochar (Re-TBC-800) was prepared by pyrolyzing multi-use black tea biochar (TBC-800) to activate peroxymonosulfate (PMS) for cycling degradation of naproxen (NPX) up to 48 times (only 6 times before regeneration). It was demonstrated by Raman and DFT calculations that the rearrangement of carbon networks during thermal regeneration resulted in the formation of a higher conjugated structure. After regeneration, C−O changed from electron acceptor to electron donor to achieve self-cycling between C=O and C−O. The reaction pathways changed from a non-radical (<sup>1</sup>O<sub>2</sub> and electron transfer) effect to a synergistic (•OH, SO<sub>4</sub><sup>•−</sup>, <sup>1</sup>O<sub>2</sub> and electron transfer) effect. Re-TBC-800 provided new insights into the structural design of functional catalysts.","PeriodicalId":349,"journal":{"name":"Journal of Cleaner Production","volume":"46 1","pages":""},"PeriodicalIF":9.7000,"publicationDate":"2024-12-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Cleaner Production","FirstCategoryId":"93","ListUrlMain":"https://doi.org/10.1016/j.jclepro.2024.144510","RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENGINEERING, ENVIRONMENTAL","Score":null,"Total":0}
引用次数: 0
Abstract
The development of metal-free catalysts with excellent reusability and the research of effects for carbon network structures in activation process are great challenges in non-metallic catalysis today. In this study, a regenerated metal-free biochar (Re-TBC-800) was prepared by pyrolyzing multi-use black tea biochar (TBC-800) to activate peroxymonosulfate (PMS) for cycling degradation of naproxen (NPX) up to 48 times (only 6 times before regeneration). It was demonstrated by Raman and DFT calculations that the rearrangement of carbon networks during thermal regeneration resulted in the formation of a higher conjugated structure. After regeneration, C−O changed from electron acceptor to electron donor to achieve self-cycling between C=O and C−O. The reaction pathways changed from a non-radical (1O2 and electron transfer) effect to a synergistic (•OH, SO4•−, 1O2 and electron transfer) effect. Re-TBC-800 provided new insights into the structural design of functional catalysts.
期刊介绍:
The Journal of Cleaner Production is an international, transdisciplinary journal that addresses and discusses theoretical and practical Cleaner Production, Environmental, and Sustainability issues. It aims to help societies become more sustainable by focusing on the concept of 'Cleaner Production', which aims at preventing waste production and increasing efficiencies in energy, water, resources, and human capital use. The journal serves as a platform for corporations, governments, education institutions, regions, and societies to engage in discussions and research related to Cleaner Production, environmental, and sustainability practices.