{"title":"Hydroxyl Spillover in Fe–Se Dual-Site Catalysts for Mixed Plastics Assay","authors":"Yu Wu, Wenxuan Jiang, Weiqing Xu, Fan Lv, Shaojia Song, Liuyong Hu, Canglong Wang, Lirong Zheng, Wenling Gu, Riguang Zhang, Shaojun Guo, Chengzhou Zhu","doi":"10.1021/jacs.4c16655","DOIUrl":null,"url":null,"abstract":"The complex composition of real plastic wastes poses a significant challenge for their large-scale disposal. A responsive on-site compositional analysis of plastics is informative in choosing downstream processing methods. Nanocatalyst-based assay kit is highly qualified for this scene; however, there remain no efficient nanocatalysts for plastics due to their highly inert chemistry. Herein, we first unveiled the hydroxyl spillover effect in an Fe–Se dual-site catalyst (FeSe/NC) and devised a prototype colorimetric assay kit for mixed plastics. Experimental and theoretical results unveiled that Fe sites acted as the main active sites for H<sub>2</sub>O<sub>2</sub> activation to produce adsorbed hydroxyl (*OH) intermediates, which subsequently desorb as hydroxyl radicals (<sup>•</sup>OH) and transfer to Se sites, supports, and even plastics for further catalysis. Specifically, <sup>•</sup>OH transferred to different plastics shows varying activities, where signal outputs were hereby used as the fingerprint for plastic identification. Moreover, the remaining *OH could respond to redox interferences in the samples for enhanced accuracy. In contrast to traditional techniques involving precise apparatus and complex pretreatments, our approach enables a rapid assay (∼10 min) of raw powdery mixed plastic wastes with an ultralow cost (0.0012 $). This discovery fills a crucial gap in the plastic assay, offering new technical guidance for diverse upcycling and recycling strategies to tackle the global plastic waste crisis.","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":"124 1","pages":""},"PeriodicalIF":14.4000,"publicationDate":"2024-12-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of the American Chemical Society","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1021/jacs.4c16655","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0
Abstract
The complex composition of real plastic wastes poses a significant challenge for their large-scale disposal. A responsive on-site compositional analysis of plastics is informative in choosing downstream processing methods. Nanocatalyst-based assay kit is highly qualified for this scene; however, there remain no efficient nanocatalysts for plastics due to their highly inert chemistry. Herein, we first unveiled the hydroxyl spillover effect in an Fe–Se dual-site catalyst (FeSe/NC) and devised a prototype colorimetric assay kit for mixed plastics. Experimental and theoretical results unveiled that Fe sites acted as the main active sites for H2O2 activation to produce adsorbed hydroxyl (*OH) intermediates, which subsequently desorb as hydroxyl radicals (•OH) and transfer to Se sites, supports, and even plastics for further catalysis. Specifically, •OH transferred to different plastics shows varying activities, where signal outputs were hereby used as the fingerprint for plastic identification. Moreover, the remaining *OH could respond to redox interferences in the samples for enhanced accuracy. In contrast to traditional techniques involving precise apparatus and complex pretreatments, our approach enables a rapid assay (∼10 min) of raw powdery mixed plastic wastes with an ultralow cost (0.0012 $). This discovery fills a crucial gap in the plastic assay, offering new technical guidance for diverse upcycling and recycling strategies to tackle the global plastic waste crisis.
期刊介绍:
The flagship journal of the American Chemical Society, known as the Journal of the American Chemical Society (JACS), has been a prestigious publication since its establishment in 1879. It holds a preeminent position in the field of chemistry and related interdisciplinary sciences. JACS is committed to disseminating cutting-edge research papers, covering a wide range of topics, and encompasses approximately 19,000 pages of Articles, Communications, and Perspectives annually. With a weekly publication frequency, JACS plays a vital role in advancing the field of chemistry by providing essential research.