Qing Zhang , Yuting He , Jing Zhang , Yadong Li , Yanfen Fang , Yunzhi Tan
{"title":"Construction of Brönsted sites on pyrite surface via plasma technology for efficient hydrolysis of microcystins-LR","authors":"Qing Zhang , Yuting He , Jing Zhang , Yadong Li , Yanfen Fang , Yunzhi Tan","doi":"10.1016/j.jes.2025.01.016","DOIUrl":null,"url":null,"abstract":"<div><div>Enhancing the catalytic hydrolysis efficiency of microcystins (MCs) at ambient temperature has been a persistent challenge in water treatment. We employed N<sub>2</sub>/low-temperature plasma technology to modify the surface of natural pyrites (NP), and the resulting nitrogen-modified pyrites (NP<sub>N</sub>) with a nanorod structure and new Fe-N<sub>x</sub> sites are more efficient for the hydrolysis of microcystins-LR (MC-LR). Kinetic experiments revealed that NP<sub>N</sub> exhibited significantly higher hydrolysis activity (<em>k</em><sub>obs</sub> = 0.1471 h<sup>−1</sup>) than NP (0.0914 h<sup>−1</sup>). Liquid chromatography-mass spectrometry (LC/MS) for the intermediates produced by hydrolyzing MC-LR, in situ attenuated total reflectance Fourier transform infrared spectroscopy (in situ ATR-FTIR) and X-ray photoelectron spectroscopy (XPS) analysis unfolded that the Fe and N atoms of Fe-N<sub>x</sub> sites on the surface act of NP<sub>N</sub> as Lewis acid and Brönsted basic respectively, selectively breaking amide bond on MC-LR molecule. This study demonstrates the effectiveness of plasma technology in modifying mineral materials to enhance their catalytic activity, providing a new method for eliminating MCs in practical water treatment.</div></div>","PeriodicalId":15788,"journal":{"name":"Journal of Environmental Sciences-china","volume":"155 ","pages":"Pages 622-632"},"PeriodicalIF":5.9000,"publicationDate":"2025-01-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Environmental Sciences-china","FirstCategoryId":"93","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S1001074225000233","RegionNum":2,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENVIRONMENTAL SCIENCES","Score":null,"Total":0}
引用次数: 0
Abstract
Enhancing the catalytic hydrolysis efficiency of microcystins (MCs) at ambient temperature has been a persistent challenge in water treatment. We employed N2/low-temperature plasma technology to modify the surface of natural pyrites (NP), and the resulting nitrogen-modified pyrites (NPN) with a nanorod structure and new Fe-Nx sites are more efficient for the hydrolysis of microcystins-LR (MC-LR). Kinetic experiments revealed that NPN exhibited significantly higher hydrolysis activity (kobs = 0.1471 h−1) than NP (0.0914 h−1). Liquid chromatography-mass spectrometry (LC/MS) for the intermediates produced by hydrolyzing MC-LR, in situ attenuated total reflectance Fourier transform infrared spectroscopy (in situ ATR-FTIR) and X-ray photoelectron spectroscopy (XPS) analysis unfolded that the Fe and N atoms of Fe-Nx sites on the surface act of NPN as Lewis acid and Brönsted basic respectively, selectively breaking amide bond on MC-LR molecule. This study demonstrates the effectiveness of plasma technology in modifying mineral materials to enhance their catalytic activity, providing a new method for eliminating MCs in practical water treatment.
期刊介绍:
The Journal of Environmental Sciences is an international journal started in 1989. The journal is devoted to publish original, peer-reviewed research papers on main aspects of environmental sciences, such as environmental chemistry, environmental biology, ecology, geosciences and environmental physics. Appropriate subjects include basic and applied research on atmospheric, terrestrial and aquatic environments, pollution control and abatement technology, conservation of natural resources, environmental health and toxicology. Announcements of international environmental science meetings and other recent information are also included.