{"title":"改良气化-熔渣驱动的过硫酸盐活化技术用于高效降解对乙酰氨基酚:N/O 活性位点调节和非自由基氧化","authors":"Wenhao Si, Fei Qi, Kangjun Wang, Qiang Wang, Zequan Zeng, Yuting Niu, Zhanggen Huang","doi":"10.3390/catal13121512","DOIUrl":null,"url":null,"abstract":"With the development of coal chemical technology, a large amount of gasification slag and wastewater are produced through coal gasification. Efficient gasification slag utilization and wastewater treatment have attracted much attention. In this study, gasification slag was modified and used as a low-cost and efficient catalyst to activate persulfate for acetaminophen degradation. Via the analysis of high-resolution X-ray photoelectron spectroscopy, the surfaces of nitric acid and calcined modified gasification slag retained a considerable number of carbonyl and graphite N functional groups. These proved to be effective active sites for the activation of persulfate. X-ray diffraction analysis revealed that the gasification slag was composed of carbon and SiO2. The evaluation of catalytic activity and application of density functional theory proved that the interaction between carbonyl and graphitic nitrogen significantly affected the catalyst activity. When the ratio of graphitic nitrogen to carbonyl was 1:3, the adsorption and activation of persulfate were significantly enhanced. The results of the quenching experiments also confirmed that the non-free radical pathway is the main pathway to activate persulfate using the gasification slag. This study provides a new approach to industrial waste utilization in wastewater treatment.","PeriodicalId":9794,"journal":{"name":"Catalysts","volume":"12 19","pages":""},"PeriodicalIF":3.8000,"publicationDate":"2023-12-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Modified Gasification-Slag-Driven Persulfate Activation for Highly Efficient Degradation of Acetaminophen: N/O Active Site Regulation and Nonradical Oxidation\",\"authors\":\"Wenhao Si, Fei Qi, Kangjun Wang, Qiang Wang, Zequan Zeng, Yuting Niu, Zhanggen Huang\",\"doi\":\"10.3390/catal13121512\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"With the development of coal chemical technology, a large amount of gasification slag and wastewater are produced through coal gasification. Efficient gasification slag utilization and wastewater treatment have attracted much attention. In this study, gasification slag was modified and used as a low-cost and efficient catalyst to activate persulfate for acetaminophen degradation. Via the analysis of high-resolution X-ray photoelectron spectroscopy, the surfaces of nitric acid and calcined modified gasification slag retained a considerable number of carbonyl and graphite N functional groups. These proved to be effective active sites for the activation of persulfate. X-ray diffraction analysis revealed that the gasification slag was composed of carbon and SiO2. The evaluation of catalytic activity and application of density functional theory proved that the interaction between carbonyl and graphitic nitrogen significantly affected the catalyst activity. When the ratio of graphitic nitrogen to carbonyl was 1:3, the adsorption and activation of persulfate were significantly enhanced. The results of the quenching experiments also confirmed that the non-free radical pathway is the main pathway to activate persulfate using the gasification slag. This study provides a new approach to industrial waste utilization in wastewater treatment.\",\"PeriodicalId\":9794,\"journal\":{\"name\":\"Catalysts\",\"volume\":\"12 19\",\"pages\":\"\"},\"PeriodicalIF\":3.8000,\"publicationDate\":\"2023-12-15\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Catalysts\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://doi.org/10.3390/catal13121512\",\"RegionNum\":3,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Catalysts","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.3390/catal13121512","RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0
摘要
随着煤化工技术的发展,煤气化过程中会产生大量气化渣和废水。气化渣的高效利用和废水处理备受关注。本研究将气化渣改性并用作一种低成本、高效的催化剂,以激活对乙酰氨基酚降解过程中的过硫酸盐。通过高分辨率 X 射线光电子能谱分析,硝酸和煅烧改性气化炉渣表面保留了大量的羰基和石墨 N 官能团。事实证明,这些都是活化过硫酸盐的有效活性位点。X 射线衍射分析表明,气化渣由碳和二氧化硅组成。催化活性评估和密度泛函理论的应用证明,羰基和石墨氮之间的相互作用对催化剂活性有显著影响。当石墨氮与羰基的比例为 1:3 时,过硫酸盐的吸附和活化能力明显增强。淬火实验结果也证实,非自由基途径是利用气化渣活化过硫酸盐的主要途径。这项研究为废水处理中的工业废物利用提供了一种新方法。
Modified Gasification-Slag-Driven Persulfate Activation for Highly Efficient Degradation of Acetaminophen: N/O Active Site Regulation and Nonradical Oxidation
With the development of coal chemical technology, a large amount of gasification slag and wastewater are produced through coal gasification. Efficient gasification slag utilization and wastewater treatment have attracted much attention. In this study, gasification slag was modified and used as a low-cost and efficient catalyst to activate persulfate for acetaminophen degradation. Via the analysis of high-resolution X-ray photoelectron spectroscopy, the surfaces of nitric acid and calcined modified gasification slag retained a considerable number of carbonyl and graphite N functional groups. These proved to be effective active sites for the activation of persulfate. X-ray diffraction analysis revealed that the gasification slag was composed of carbon and SiO2. The evaluation of catalytic activity and application of density functional theory proved that the interaction between carbonyl and graphitic nitrogen significantly affected the catalyst activity. When the ratio of graphitic nitrogen to carbonyl was 1:3, the adsorption and activation of persulfate were significantly enhanced. The results of the quenching experiments also confirmed that the non-free radical pathway is the main pathway to activate persulfate using the gasification slag. This study provides a new approach to industrial waste utilization in wastewater treatment.
期刊介绍:
Catalysts (ISSN 2073-4344) is an international open access journal of catalysts and catalyzed reactions. Catalysts publishes reviews, regular research papers (articles) and short communications. Our aim is to encourage scientists to publish their experimental and theoretical results in as much detail as possible. Therefore, there is no restriction on the length of the papers. The full experimental details must be provided so that the results can be reproduced.