气液脉冲调制等离子体与气泡伴随等离子体衍生热增强十八胺和4-十二烷基啉的降解:性能和机制洞察

IF 9.1 1区 工程技术 Q1 ENGINEERING, CHEMICAL Separation and Purification Technology Pub Date : 2025-07-30 Epub Date: 2025-01-25 DOI:10.1016/j.seppur.2025.131758
Xuri Li , Siyuan Zhang , Liang Ma , Miao Lu , Jingbao Liu , Haining Liu , Zhijian Wu , Xiangmei Cui , Xiushen Ye
{"title":"气液脉冲调制等离子体与气泡伴随等离子体衍生热增强十八胺和4-十二烷基啉的降解:性能和机制洞察","authors":"Xuri Li ,&nbsp;Siyuan Zhang ,&nbsp;Liang Ma ,&nbsp;Miao Lu ,&nbsp;Jingbao Liu ,&nbsp;Haining Liu ,&nbsp;Zhijian Wu ,&nbsp;Xiangmei Cui ,&nbsp;Xiushen Ye","doi":"10.1016/j.seppur.2025.131758","DOIUrl":null,"url":null,"abstract":"<div><div>A gas–liquid pulse-modulated plasma with bubbling coupled with plasma-derived heat system was developed for efficient degradation of octadecylamine (ODA) and 4-dodecylmorpholine (DMP). The structure–activity relationship between high-voltage electrode structures and the degradation activity of ODA and DMP was delved into using fluid dynamics simulations. The crucial role of bubbling is evident in the enhancement of ODA and DMP degradation efficiencies by 100% and 47% within 30 min, respectively. ODA and DMP degradation efficiencies reached 96% and 100% with treatment of 30 min, respectively, accompanied by a high mineralization efficiency of 80 %. An in-depth analysis was performed on the evolution of the physicochemical properties of the reaction solution during degradation. The plasma coupled with plasma-derived heat system exhibited remarkable synergistic effects, achieving synergistic intensities of 0.96 for ODA and 1.28 for DMP, with energy efficiencies increased by 31% and 16%. Analysis of the evolution of total nitrogen and nitrogen-containing species revealed that ODA and DMP degradation commenced with the decomposition of amino groups, ultimately converting them into <span><math><mrow><mi>N</mi><msubsup><mi>O</mi><mrow><mn>3</mn></mrow><mo>-</mo></msubsup></mrow></math></span> and <span><math><mrow><mi>N</mi><msubsup><mi>H</mi><mrow><mn>4</mn></mrow><mo>+</mo></msubsup></mrow></math></span>. Quenching tests and electron spin resonance characterization confirmed the generation of <span><math><mrow><mo>·</mo><mi>O</mi><mi>H</mi></mrow></math></span>, <span><math><mrow><msup><mrow><mspace></mspace></mrow><mo>·</mo></msup><msubsup><mi>O</mi><mrow><mn>2</mn></mrow><mo>-</mo></msubsup></mrow></math></span> and <span><math><mrow><msup><mrow><mspace></mspace></mrow><mn>1</mn></msup><msub><mi>O</mi><mn>2</mn></msub></mrow></math></span>, with <span><math><mrow><mo>·</mo><mi>O</mi><mi>H</mi></mrow></math></span> playing a pivotal role in the degradation process. Furthermore, the possible degradation pathways of ODA and DMP were elucidated by the theoretical calculations and gas chromatography-mass spectrometry results, respectively. The toxicity evaluation of degradation intermediates demonstrated a consistent decrease in toxicity during the degradation process. This study advances our understanding of the synergistic potential of plasma-plasma-derived heat systems for pollutant degradation and paves the way for the development of more effective pollutant degradation technologies.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"362 ","pages":"Article 131758"},"PeriodicalIF":9.1000,"publicationDate":"2025-07-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Gas-liquid pulse-modulated plasma with bubbling concomitant with plasma-derived heat enhanced degradation of the octadecylamine and 4-dodecylmorpholine: Performance and mechanism insight\",\"authors\":\"Xuri Li ,&nbsp;Siyuan Zhang ,&nbsp;Liang Ma ,&nbsp;Miao Lu ,&nbsp;Jingbao Liu ,&nbsp;Haining Liu ,&nbsp;Zhijian Wu ,&nbsp;Xiangmei Cui ,&nbsp;Xiushen Ye\",\"doi\":\"10.1016/j.seppur.2025.131758\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>A gas–liquid pulse-modulated plasma with bubbling coupled with plasma-derived heat system was developed for efficient degradation of octadecylamine (ODA) and 4-dodecylmorpholine (DMP). The structure–activity relationship between high-voltage electrode structures and the degradation activity of ODA and DMP was delved into using fluid dynamics simulations. The crucial role of bubbling is evident in the enhancement of ODA and DMP degradation efficiencies by 100% and 47% within 30 min, respectively. ODA and DMP degradation efficiencies reached 96% and 100% with treatment of 30 min, respectively, accompanied by a high mineralization efficiency of 80 %. An in-depth analysis was performed on the evolution of the physicochemical properties of the reaction solution during degradation. The plasma coupled with plasma-derived heat system exhibited remarkable synergistic effects, achieving synergistic intensities of 0.96 for ODA and 1.28 for DMP, with energy efficiencies increased by 31% and 16%. Analysis of the evolution of total nitrogen and nitrogen-containing species revealed that ODA and DMP degradation commenced with the decomposition of amino groups, ultimately converting them into <span><math><mrow><mi>N</mi><msubsup><mi>O</mi><mrow><mn>3</mn></mrow><mo>-</mo></msubsup></mrow></math></span> and <span><math><mrow><mi>N</mi><msubsup><mi>H</mi><mrow><mn>4</mn></mrow><mo>+</mo></msubsup></mrow></math></span>. Quenching tests and electron spin resonance characterization confirmed the generation of <span><math><mrow><mo>·</mo><mi>O</mi><mi>H</mi></mrow></math></span>, <span><math><mrow><msup><mrow><mspace></mspace></mrow><mo>·</mo></msup><msubsup><mi>O</mi><mrow><mn>2</mn></mrow><mo>-</mo></msubsup></mrow></math></span> and <span><math><mrow><msup><mrow><mspace></mspace></mrow><mn>1</mn></msup><msub><mi>O</mi><mn>2</mn></msub></mrow></math></span>, with <span><math><mrow><mo>·</mo><mi>O</mi><mi>H</mi></mrow></math></span> playing a pivotal role in the degradation process. Furthermore, the possible degradation pathways of ODA and DMP were elucidated by the theoretical calculations and gas chromatography-mass spectrometry results, respectively. The toxicity evaluation of degradation intermediates demonstrated a consistent decrease in toxicity during the degradation process. This study advances our understanding of the synergistic potential of plasma-plasma-derived heat systems for pollutant degradation and paves the way for the development of more effective pollutant degradation technologies.</div></div>\",\"PeriodicalId\":427,\"journal\":{\"name\":\"Separation and Purification Technology\",\"volume\":\"362 \",\"pages\":\"Article 131758\"},\"PeriodicalIF\":9.1000,\"publicationDate\":\"2025-07-30\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Separation and Purification Technology\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S1383586625003557\",\"RegionNum\":1,\"RegionCategory\":\"工程技术\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"2025/1/25 0:00:00\",\"PubModel\":\"Epub\",\"JCR\":\"Q1\",\"JCRName\":\"ENGINEERING, CHEMICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Separation and Purification Technology","FirstCategoryId":"5","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S1383586625003557","RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"2025/1/25 0:00:00","PubModel":"Epub","JCR":"Q1","JCRName":"ENGINEERING, CHEMICAL","Score":null,"Total":0}
引用次数: 0

摘要

研究了一种鼓泡气液脉冲调制等离子体-等离子体衍生热耦合系统,用于高效降解十八烷基胺(ODA)和4-十二烷基啉(DMP)。采用流体动力学模拟方法研究了高压电极结构与ODA和DMP降解活性之间的构效关系。在30 min内,鼓泡对ODA和DMP的降解效率分别提高了100% %和47% %,其关键作用是明显的。处理时间为30 min时,ODA和DMP的降解效率分别达到96 %和100 %,矿化效率高达80 %。对反应溶液在降解过程中理化性质的演变进行了深入分析。等离子体与等离子体衍生热系统的耦合表现出显著的协同效应,ODA的协同强度为0.96,DMP的协同强度为1.28,能量效率分别提高了31% %和16% %。对总氮和含氮物种的演化分析表明,ODA和DMP的降解始于氨基的分解,最终转化为NO3-NO3-和NH4+NH4+。淬火实验和电子自旋共振表征证实了·OH·OH、·O2-·O2-和1021o2的生成,其中·OH·OH在降解过程中起着关键作用。此外,通过理论计算和气相色谱-质谱分析结果分别阐明了ODA和DMP可能的降解途径。降解中间体的毒性评价表明,在降解过程中毒性持续下降。这项研究促进了我们对等离子体衍生热系统对污染物降解的协同潜力的理解,并为开发更有效的污染物降解技术铺平了道路。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

摘要图片

摘要图片

查看原文
分享 分享
微信好友 朋友圈 QQ好友 复制链接
本刊更多论文
Gas-liquid pulse-modulated plasma with bubbling concomitant with plasma-derived heat enhanced degradation of the octadecylamine and 4-dodecylmorpholine: Performance and mechanism insight
A gas–liquid pulse-modulated plasma with bubbling coupled with plasma-derived heat system was developed for efficient degradation of octadecylamine (ODA) and 4-dodecylmorpholine (DMP). The structure–activity relationship between high-voltage electrode structures and the degradation activity of ODA and DMP was delved into using fluid dynamics simulations. The crucial role of bubbling is evident in the enhancement of ODA and DMP degradation efficiencies by 100% and 47% within 30 min, respectively. ODA and DMP degradation efficiencies reached 96% and 100% with treatment of 30 min, respectively, accompanied by a high mineralization efficiency of 80 %. An in-depth analysis was performed on the evolution of the physicochemical properties of the reaction solution during degradation. The plasma coupled with plasma-derived heat system exhibited remarkable synergistic effects, achieving synergistic intensities of 0.96 for ODA and 1.28 for DMP, with energy efficiencies increased by 31% and 16%. Analysis of the evolution of total nitrogen and nitrogen-containing species revealed that ODA and DMP degradation commenced with the decomposition of amino groups, ultimately converting them into NO3- and NH4+. Quenching tests and electron spin resonance characterization confirmed the generation of ·OH, ·O2- and 1O2, with ·OH playing a pivotal role in the degradation process. Furthermore, the possible degradation pathways of ODA and DMP were elucidated by the theoretical calculations and gas chromatography-mass spectrometry results, respectively. The toxicity evaluation of degradation intermediates demonstrated a consistent decrease in toxicity during the degradation process. This study advances our understanding of the synergistic potential of plasma-plasma-derived heat systems for pollutant degradation and paves the way for the development of more effective pollutant degradation technologies.
求助全文
通过发布文献求助,成功后即可免费获取论文全文。 去求助
来源期刊
Separation and Purification Technology
Separation and Purification Technology 工程技术-工程:化工
CiteScore
14.00
自引率
12.80%
发文量
2347
审稿时长
43 days
期刊介绍: Separation and Purification Technology is a premier journal committed to sharing innovative methods for separation and purification in chemical and environmental engineering, encompassing both homogeneous solutions and heterogeneous mixtures. Our scope includes the separation and/or purification of liquids, vapors, and gases, as well as carbon capture and separation techniques. However, it's important to note that methods solely intended for analytical purposes are not within the scope of the journal. Additionally, disciplines such as soil science, polymer science, and metallurgy fall outside the purview of Separation and Purification Technology. Join us in advancing the field of separation and purification methods for sustainable solutions in chemical and environmental engineering.
期刊最新文献
Collagen fiber-templated mesoporous potassium titanium phosphate for ultrafast strontium capture Thermodynamic modeling of CO₂ equilibrium in diverse amine systems using an improved activity coefficient model: From single amines to binary blends Sulfation roasting technology: A comprehensive review on its application for extracting valuable metals from mineral and solid waste resources Formation characteristics of chlorinated organic by-products in waste leachate nanofiltration membrane concentrate: a comparative study of Fe2+/H2O2 and Fe0/H2O2 systems Process intensification and multi-criteria evaluation of extractive distillation for the separation of Diisopropylamine/isopropyl alcohol/water system
×
引用
GB/T 7714-2015
复制
MLA
复制
APA
复制
导出至
BibTeX EndNote RefMan NoteFirst NoteExpress
×
×
提示
您的信息不完整,为了账户安全,请先补充。
现在去补充
×
提示
您因"违规操作"
具体请查看互助需知
我知道了
×
提示
现在去查看 取消
×
提示
确定
0
微信
客服QQ
Book学术公众号 扫码关注我们
反馈
×
意见反馈
请填写您的意见或建议
请填写您的手机或邮箱
已复制链接
已复制链接
快去分享给好友吧!
我知道了
×
扫码分享
扫码分享
Book学术官方微信
Book学术官方微信
Book学术文献互助
Book学术文献互助群
群 号:604180095
Book学术
文献互助 智能选刊 最新文献 互助须知 联系我们:info@booksci.cn
Book学术提供免费学术资源搜索服务,方便国内外学者检索中英文文献。致力于提供最便捷和优质的服务体验。
Copyright © 2023 Book学术 All rights reserved.
ghs 京公网安备 11010802042870号 京ICP备2023020795号-1