{"title":"超快类芬顿反应的单原子铁锚定管状g-C3N4催化剂:高价铁氧和有机自由基的作用","authors":"Fei Chen, Lian-Lian Liu, Jing-Hang Wu, Xian-Hong Rui, Jie-Jie Chen, Yan Yu","doi":"10.1002/adma.202202891","DOIUrl":null,"url":null,"abstract":"<p>Single-atom catalysts have emerged as an efficient oxidant activator for eliminating organic pollutants in Fenton-like systems. However, the complex preparation, single active site, lack of understanding of the fundamental mechanism, and harsh pH conditions currently limit their practical applications. In this work, single-atom iron anchored nitrogen-rich g-C<sub>3</sub>N<sub>4</sub> nanotubes (FeCNs) are designed and synthesized by a facile approach, and eco-friendly peracetic acid (PAA) is selected as the oxidant for Fenton-like reactions. The constructed heterogenous system achieves an enhanced degradation of various organic contaminants over a wide pH range of 3.0–9.0, exhibiting an ultrahigh and stable catalytic activity, outperforming equivalent quantities of pristine g-C<sub>3</sub>N<sub>4</sub> by 75 times. The <sup>18</sup>O isotope-labeling technique, probe method, and theoretical calculations demonstrate that the efficient catalytic activity relies on the high-valency iron-oxo species coupled with organic radicals generated by PAA. An increase in electron transport from the contaminant to the formed “metastable PAA/FeCN catalyst surface complex” is detected. A double driving mechanism for the tubular g-C<sub>3</sub>N<sub>4</sub> regulated by a single Fe site and PAA activation is proposed. This work opens an avenue for developing novel catalysts with the coexistence of multiple active units and providing opportunities for significantly improving catalytic efficiency.</p>","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":null,"pages":null},"PeriodicalIF":27.4000,"publicationDate":"2022-06-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"79","resultStr":"{\"title\":\"Single-Atom Iron Anchored Tubular g-C3N4 Catalysts for Ultrafast Fenton-Like Reaction: Roles of High-Valency Iron-Oxo Species and Organic Radicals\",\"authors\":\"Fei Chen, Lian-Lian Liu, Jing-Hang Wu, Xian-Hong Rui, Jie-Jie Chen, Yan Yu\",\"doi\":\"10.1002/adma.202202891\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p>Single-atom catalysts have emerged as an efficient oxidant activator for eliminating organic pollutants in Fenton-like systems. However, the complex preparation, single active site, lack of understanding of the fundamental mechanism, and harsh pH conditions currently limit their practical applications. In this work, single-atom iron anchored nitrogen-rich g-C<sub>3</sub>N<sub>4</sub> nanotubes (FeCNs) are designed and synthesized by a facile approach, and eco-friendly peracetic acid (PAA) is selected as the oxidant for Fenton-like reactions. The constructed heterogenous system achieves an enhanced degradation of various organic contaminants over a wide pH range of 3.0–9.0, exhibiting an ultrahigh and stable catalytic activity, outperforming equivalent quantities of pristine g-C<sub>3</sub>N<sub>4</sub> by 75 times. The <sup>18</sup>O isotope-labeling technique, probe method, and theoretical calculations demonstrate that the efficient catalytic activity relies on the high-valency iron-oxo species coupled with organic radicals generated by PAA. An increase in electron transport from the contaminant to the formed “metastable PAA/FeCN catalyst surface complex” is detected. A double driving mechanism for the tubular g-C<sub>3</sub>N<sub>4</sub> regulated by a single Fe site and PAA activation is proposed. This work opens an avenue for developing novel catalysts with the coexistence of multiple active units and providing opportunities for significantly improving catalytic efficiency.</p>\",\"PeriodicalId\":114,\"journal\":{\"name\":\"Advanced Materials\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":27.4000,\"publicationDate\":\"2022-06-09\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"79\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Advanced Materials\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://onlinelibrary.wiley.com/doi/10.1002/adma.202202891\",\"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}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Advanced Materials","FirstCategoryId":"88","ListUrlMain":"https://onlinelibrary.wiley.com/doi/10.1002/adma.202202891","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}
Single-Atom Iron Anchored Tubular g-C3N4 Catalysts for Ultrafast Fenton-Like Reaction: Roles of High-Valency Iron-Oxo Species and Organic Radicals
Single-atom catalysts have emerged as an efficient oxidant activator for eliminating organic pollutants in Fenton-like systems. However, the complex preparation, single active site, lack of understanding of the fundamental mechanism, and harsh pH conditions currently limit their practical applications. In this work, single-atom iron anchored nitrogen-rich g-C3N4 nanotubes (FeCNs) are designed and synthesized by a facile approach, and eco-friendly peracetic acid (PAA) is selected as the oxidant for Fenton-like reactions. The constructed heterogenous system achieves an enhanced degradation of various organic contaminants over a wide pH range of 3.0–9.0, exhibiting an ultrahigh and stable catalytic activity, outperforming equivalent quantities of pristine g-C3N4 by 75 times. The 18O isotope-labeling technique, probe method, and theoretical calculations demonstrate that the efficient catalytic activity relies on the high-valency iron-oxo species coupled with organic radicals generated by PAA. An increase in electron transport from the contaminant to the formed “metastable PAA/FeCN catalyst surface complex” is detected. A double driving mechanism for the tubular g-C3N4 regulated by a single Fe site and PAA activation is proposed. This work opens an avenue for developing novel catalysts with the coexistence of multiple active units and providing opportunities for significantly improving catalytic efficiency.
期刊介绍:
Advanced Materials, one of the world's most prestigious journals and the foundation of the Advanced portfolio, is the home of choice for best-in-class materials science for more than 30 years. Following this fast-growing and interdisciplinary field, we are considering and publishing the most important discoveries on any and all materials from materials scientists, chemists, physicists, engineers as well as health and life scientists and bringing you the latest results and trends in modern materials-related research every week.