{"title":"锰掺杂产生氧空位,提高了氢氧化钴活化过氧单硫酸盐的性能","authors":"Wenchao Zhang , Yufei Han , Yiting Guo , Wenhao Zhang , Fei Xu , Weizhi Zhou","doi":"10.1016/j.jece.2024.115042","DOIUrl":null,"url":null,"abstract":"<div><div>A process for activating peroxymonosulfate using Mn-doped cobalt oxyhydroxide (CoOOH) was developed, achieving efficient removal of organic pollutant. Targeting sulfamethoxazole (SMX) as the pollutant, the reaction rate of cobalt hydroxide with a 10 % manganese doping (CoMn10) increased by more than tenfold compared to undoped CoOOH. Under conditions of 0.3 g/L catalyst and 0.5 mM PMS, 10 mg/L SMX was removed within 10 min. The activation of PMS to degrade SMX is mainly based on heterogeneous catalytic reaction. Quenching experiments, electron paramagnetic resonance spectra and methyl phenyl sulfoxide <strong>(</strong>PMSO) probe confirmed the presence of multiple reactive oxygen species in the CoMn10/PMS system, including sulfate radicals, singlet oxygen, high-valent metals, and electron transfer. It was resistant to multiple anions (Cl<sup>−</sup>, NO<sub>3</sub><sup>−</sup>, SO<sub>4</sub><sup>2−</sup>) and has catalytic stability in real water. CoMn10/PMS system has the ability to degrade a variety of pollutants efficiently. The introduction of manganese facilitates the formation of oxygen vacancies. The density functional theory (DFT) computation showed that manganese increased the adsorption energy and electron transport flux of CoOOH, enhanced the chemical activity of CoOOH, and the structure of PMS adsorbed on CoMn10 was more easily adsorbed and cleavaged.</div></div>","PeriodicalId":15759,"journal":{"name":"Journal of Environmental Chemical Engineering","volume":"13 1","pages":"Article 115042"},"PeriodicalIF":7.2000,"publicationDate":"2025-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Manganese doping generates oxygen vacancies to enhance the performance of cobalt oxyhydroxide in activating peroxymonosulfate\",\"authors\":\"Wenchao Zhang , Yufei Han , Yiting Guo , Wenhao Zhang , Fei Xu , Weizhi Zhou\",\"doi\":\"10.1016/j.jece.2024.115042\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>A process for activating peroxymonosulfate using Mn-doped cobalt oxyhydroxide (CoOOH) was developed, achieving efficient removal of organic pollutant. Targeting sulfamethoxazole (SMX) as the pollutant, the reaction rate of cobalt hydroxide with a 10 % manganese doping (CoMn10) increased by more than tenfold compared to undoped CoOOH. Under conditions of 0.3 g/L catalyst and 0.5 mM PMS, 10 mg/L SMX was removed within 10 min. The activation of PMS to degrade SMX is mainly based on heterogeneous catalytic reaction. Quenching experiments, electron paramagnetic resonance spectra and methyl phenyl sulfoxide <strong>(</strong>PMSO) probe confirmed the presence of multiple reactive oxygen species in the CoMn10/PMS system, including sulfate radicals, singlet oxygen, high-valent metals, and electron transfer. It was resistant to multiple anions (Cl<sup>−</sup>, NO<sub>3</sub><sup>−</sup>, SO<sub>4</sub><sup>2−</sup>) and has catalytic stability in real water. CoMn10/PMS system has the ability to degrade a variety of pollutants efficiently. The introduction of manganese facilitates the formation of oxygen vacancies. The density functional theory (DFT) computation showed that manganese increased the adsorption energy and electron transport flux of CoOOH, enhanced the chemical activity of CoOOH, and the structure of PMS adsorbed on CoMn10 was more easily adsorbed and cleavaged.</div></div>\",\"PeriodicalId\":15759,\"journal\":{\"name\":\"Journal of Environmental Chemical Engineering\",\"volume\":\"13 1\",\"pages\":\"Article 115042\"},\"PeriodicalIF\":7.2000,\"publicationDate\":\"2025-02-01\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of Environmental Chemical Engineering\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S2213343724031749\",\"RegionNum\":2,\"RegionCategory\":\"工程技术\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"2024/12/5 0:00:00\",\"PubModel\":\"Epub\",\"JCR\":\"Q1\",\"JCRName\":\"ENGINEERING, CHEMICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Environmental Chemical Engineering","FirstCategoryId":"5","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S2213343724031749","RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"2024/12/5 0:00:00","PubModel":"Epub","JCR":"Q1","JCRName":"ENGINEERING, CHEMICAL","Score":null,"Total":0}
引用次数: 0
摘要
研究了锰掺杂氧化钴(CoOOH)活化过氧单硫酸盐的工艺,实现了对有机污染物的高效去除。以磺胺甲恶唑(SMX)为污染物,10 %锰掺杂(CoMn10)对氢氧化钴的反应速率比未掺杂的CoOOH提高了10倍以上。在0.3 g/L催化剂和0.5 mM PMS条件下,10 mg/L SMX在10 min内脱除。PMS降解SMX的活化主要基于非均相催化反应。猝灭实验、电子顺磁共振谱和甲基苯基亚砜(PMSO)探针证实了CoMn10/PMS体系中存在多种活性氧,包括硫酸盐自由基、单线态氧、高价金属和电子转移。耐多种阴离子(Cl−、NO3−、SO42−),在实际水中具有催化稳定性。CoMn10/PMS系统具有高效降解多种污染物的能力。锰的引入促进了氧空位的形成。密度泛函理论(DFT)计算表明,锰增加了CoOOH的吸附能和电子传递通量,增强了CoOOH的化学活性,CoMn10吸附的PMS结构更容易被吸附和裂解。
Manganese doping generates oxygen vacancies to enhance the performance of cobalt oxyhydroxide in activating peroxymonosulfate
A process for activating peroxymonosulfate using Mn-doped cobalt oxyhydroxide (CoOOH) was developed, achieving efficient removal of organic pollutant. Targeting sulfamethoxazole (SMX) as the pollutant, the reaction rate of cobalt hydroxide with a 10 % manganese doping (CoMn10) increased by more than tenfold compared to undoped CoOOH. Under conditions of 0.3 g/L catalyst and 0.5 mM PMS, 10 mg/L SMX was removed within 10 min. The activation of PMS to degrade SMX is mainly based on heterogeneous catalytic reaction. Quenching experiments, electron paramagnetic resonance spectra and methyl phenyl sulfoxide (PMSO) probe confirmed the presence of multiple reactive oxygen species in the CoMn10/PMS system, including sulfate radicals, singlet oxygen, high-valent metals, and electron transfer. It was resistant to multiple anions (Cl−, NO3−, SO42−) and has catalytic stability in real water. CoMn10/PMS system has the ability to degrade a variety of pollutants efficiently. The introduction of manganese facilitates the formation of oxygen vacancies. The density functional theory (DFT) computation showed that manganese increased the adsorption energy and electron transport flux of CoOOH, enhanced the chemical activity of CoOOH, and the structure of PMS adsorbed on CoMn10 was more easily adsorbed and cleavaged.
期刊介绍:
The Journal of Environmental Chemical Engineering (JECE) serves as a platform for the dissemination of original and innovative research focusing on the advancement of environmentally-friendly, sustainable technologies. JECE emphasizes the transition towards a carbon-neutral circular economy and a self-sufficient bio-based economy. Topics covered include soil, water, wastewater, and air decontamination; pollution monitoring, prevention, and control; advanced analytics, sensors, impact and risk assessment methodologies in environmental chemical engineering; resource recovery (water, nutrients, materials, energy); industrial ecology; valorization of waste streams; waste management (including e-waste); climate-water-energy-food nexus; novel materials for environmental, chemical, and energy applications; sustainability and environmental safety; water digitalization, water data science, and machine learning; process integration and intensification; recent developments in green chemistry for synthesis, catalysis, and energy; and original research on contaminants of emerging concern, persistent chemicals, and priority substances, including microplastics, nanoplastics, nanomaterials, micropollutants, antimicrobial resistance genes, and emerging pathogens (viruses, bacteria, parasites) of environmental significance.