{"title":"Identification and Regulation of Active Sites on Nanodiamonds: Establishing a Highly Efficient Catalytic System for Oxidation of Organic Contaminants","authors":"Penghui Shao, Jiayu Tian, Feng Yang, Xiaoguang Duan, Shanshan Gao, Wenxin Shi, Xubiao Luo, Fuyi Cui, Shenglian Luo, Shaobin Wang","doi":"10.1002/adfm.201705295","DOIUrl":null,"url":null,"abstract":"<p>Nanodiamonds exhibit great potential as green catalysts for remediation of organic contaminants. However, the specific active site and corresponding oxidative mechanism are unclear, which retard further developments of high-performance catalysts. Here, an annealing strategy is developed to accurately regulate the content of ketonic carbonyl groups on nanodiamonds; meanwhile other structural characteristics of nanodiamonds remain almost unchanged. The well-defined nanodiamonds with well-controlled ketonic carbonyl groups exhibit excellent catalytic activity in activation of peroxymonosulfate for oxidation of organic pollutants. Based on the semi-quantitative and quantitative correlations of ketonic carbonyl groups and the reaction rate constants, it is conclusively determined that ketonic carbonyl groups are the catalytically active sites. Different from conventional oxidative systems, reactive oxygen species in nanodiamonds@peroxymonosulfate system are revealed to be singlet oxygen with high selectivity, which can effectively oxidize and mineralize the target contaminants. Impressively, the singlet-oxygen-mediated oxidation system significantly outperforms the classical radicals-based oxidation system in remediation of actual wastewater. This work not only provides a valuable insight for the design of new nanocarbon catalysts with abundant active sites but also establishes a very promising catalytic oxidation system for the green remediation of actual contaminated water.</p>","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":null,"pages":null},"PeriodicalIF":18.5000,"publicationDate":"2018-01-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1002/adfm.201705295","citationCount":"462","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Advanced Functional Materials","FirstCategoryId":"88","ListUrlMain":"https://onlinelibrary.wiley.com/doi/10.1002/adfm.201705295","RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 462
Abstract
Nanodiamonds exhibit great potential as green catalysts for remediation of organic contaminants. However, the specific active site and corresponding oxidative mechanism are unclear, which retard further developments of high-performance catalysts. Here, an annealing strategy is developed to accurately regulate the content of ketonic carbonyl groups on nanodiamonds; meanwhile other structural characteristics of nanodiamonds remain almost unchanged. The well-defined nanodiamonds with well-controlled ketonic carbonyl groups exhibit excellent catalytic activity in activation of peroxymonosulfate for oxidation of organic pollutants. Based on the semi-quantitative and quantitative correlations of ketonic carbonyl groups and the reaction rate constants, it is conclusively determined that ketonic carbonyl groups are the catalytically active sites. Different from conventional oxidative systems, reactive oxygen species in nanodiamonds@peroxymonosulfate system are revealed to be singlet oxygen with high selectivity, which can effectively oxidize and mineralize the target contaminants. Impressively, the singlet-oxygen-mediated oxidation system significantly outperforms the classical radicals-based oxidation system in remediation of actual wastewater. This work not only provides a valuable insight for the design of new nanocarbon catalysts with abundant active sites but also establishes a very promising catalytic oxidation system for the green remediation of actual contaminated water.
期刊介绍:
Firmly established as a top-tier materials science journal, Advanced Functional Materials reports breakthrough research in all aspects of materials science, including nanotechnology, chemistry, physics, and biology every week.
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