重新考虑过氧化氢在基于过氧一碳酸盐的污染物控制氧化系统中的作用

IF 11.4 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Water Research Pub Date : 2024-11-05 DOI:10.1016/j.watres.2024.122750
Zihan Yang , Yi Zhou , Yiqian Jiang , Peiqing Zhao , Xu Meng
{"title":"重新考虑过氧化氢在基于过氧一碳酸盐的污染物控制氧化系统中的作用","authors":"Zihan Yang ,&nbsp;Yi Zhou ,&nbsp;Yiqian Jiang ,&nbsp;Peiqing Zhao ,&nbsp;Xu Meng","doi":"10.1016/j.watres.2024.122750","DOIUrl":null,"url":null,"abstract":"<div><div>Advanced oxidation processes that utilize peroxymonocarbonate (HCO<sub>4</sub><sup>-</sup>), generated in-situ through the reaction of HCO<sub>3</sub><sup>-</sup> and H<sub>2</sub>O<sub>2</sub>, are employed for the removal of pollutants in water. Nevertheless, the precise role of H<sub>2</sub>O<sub>2</sub> in these processes remains a subject of debate. This study established a HCO<sub>4</sub><sup>-</sup>-based oxidation system using NaHCO<sub>3</sub> and H<sub>2</sub>O<sub>2</sub> for the degradation of acetaminophen and investigated the activation mechanisms of coexisting oxidants. Under thermal activation conditions, the O<img>O bond in HCO<sub>4</sub><sup>-</sup> (HO<img>OCOO<sup>-</sup>) was more readily cleaved than the O<img>O bond in the co-existing oxidant H<sub>2</sub>O<sub>2</sub> (HO<img>OH), leading to the generation of reactive oxygen species (ROS). Based on kinetics and ROS evaluation, H<sub>2</sub>O<sub>2</sub> primarily served to form HCO<sub>4</sub><sup>-</sup> rather than converting to ·OH or O<sub>2</sub>, with HCO<sub>4</sub><sup>-</sup> acting as the primary oxidant for degradation through the formation of <span><math><msubsup><mtext>CO</mtext><mrow><mn>3</mn></mrow><mrow><mo>·</mo><mo>−</mo></mrow></msubsup></math></span>and <strong>·</strong>OH. In this oxidation system, H<sub>2</sub>O<sub>2</sub> utilization efficiency for <strong>·</strong>OH production reached 27.34 %, <strong>·</strong>OH yield reached 24.15 % and acetaminophen degradation efficiency realized 83 % at 60 °C with 20 mM HCO<sub>3</sub><sup>-</sup> and 20 mM H<sub>2</sub>O<sub>2</sub>. The apparent activation energy of acetaminophen degradation and HCO<sub>4</sub><sup>-</sup> activation were calculated as 90.83 kJ mol<sup>-1</sup> and 18.81 kJ mol<sup>-1</sup>, respectively. Moreover, a novel CO<sub>2</sub>-derived HCO<sub>4</sub><sup>-</sup>-based system led to a comparable acetaminophen degradation efficiency of 82 % and a higher k<em><sub>obs</sub></em> of 0.028 min<sup>-1</sup>. The system optimization and ROS evaluation suggest that high concentration of H<sub>2</sub>O<sub>2</sub> inhibited the degradation and quenched <span><math><msubsup><mtext>CO</mtext><mrow><mn>3</mn></mrow><mrow><mo>·</mo><mo>−</mo></mrow></msubsup></math></span> and <strong>·</strong>OH to yield <strong>·</strong>O<sub>2</sub><sup>-</sup> and <sup>1</sup>O<sub>2</sub>. Furthermore, EPR analysis and quenching experiments indicate that <span><math><msubsup><mtext>CO</mtext><mrow><mn>3</mn></mrow><mrow><mo>·</mo><mo>−</mo></mrow></msubsup></math></span> was mainly responsible for acetaminophen degradation. This work provides fundamental understanding of the HCO<sub>4</sub><sup>-</sup>-based oxidation system.</div></div>","PeriodicalId":443,"journal":{"name":"Water Research","volume":"268 ","pages":"Article 122750"},"PeriodicalIF":11.4000,"publicationDate":"2024-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Reconsideration of the role of hydrogen peroxide in peroxymonocarbonate-based oxidation system for pollutant control\",\"authors\":\"Zihan Yang ,&nbsp;Yi Zhou ,&nbsp;Yiqian Jiang ,&nbsp;Peiqing Zhao ,&nbsp;Xu Meng\",\"doi\":\"10.1016/j.watres.2024.122750\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>Advanced oxidation processes that utilize peroxymonocarbonate (HCO<sub>4</sub><sup>-</sup>), generated in-situ through the reaction of HCO<sub>3</sub><sup>-</sup> and H<sub>2</sub>O<sub>2</sub>, are employed for the removal of pollutants in water. Nevertheless, the precise role of H<sub>2</sub>O<sub>2</sub> in these processes remains a subject of debate. This study established a HCO<sub>4</sub><sup>-</sup>-based oxidation system using NaHCO<sub>3</sub> and H<sub>2</sub>O<sub>2</sub> for the degradation of acetaminophen and investigated the activation mechanisms of coexisting oxidants. Under thermal activation conditions, the O<img>O bond in HCO<sub>4</sub><sup>-</sup> (HO<img>OCOO<sup>-</sup>) was more readily cleaved than the O<img>O bond in the co-existing oxidant H<sub>2</sub>O<sub>2</sub> (HO<img>OH), leading to the generation of reactive oxygen species (ROS). Based on kinetics and ROS evaluation, H<sub>2</sub>O<sub>2</sub> primarily served to form HCO<sub>4</sub><sup>-</sup> rather than converting to ·OH or O<sub>2</sub>, with HCO<sub>4</sub><sup>-</sup> acting as the primary oxidant for degradation through the formation of <span><math><msubsup><mtext>CO</mtext><mrow><mn>3</mn></mrow><mrow><mo>·</mo><mo>−</mo></mrow></msubsup></math></span>and <strong>·</strong>OH. In this oxidation system, H<sub>2</sub>O<sub>2</sub> utilization efficiency for <strong>·</strong>OH production reached 27.34 %, <strong>·</strong>OH yield reached 24.15 % and acetaminophen degradation efficiency realized 83 % at 60 °C with 20 mM HCO<sub>3</sub><sup>-</sup> and 20 mM H<sub>2</sub>O<sub>2</sub>. The apparent activation energy of acetaminophen degradation and HCO<sub>4</sub><sup>-</sup> activation were calculated as 90.83 kJ mol<sup>-1</sup> and 18.81 kJ mol<sup>-1</sup>, respectively. Moreover, a novel CO<sub>2</sub>-derived HCO<sub>4</sub><sup>-</sup>-based system led to a comparable acetaminophen degradation efficiency of 82 % and a higher k<em><sub>obs</sub></em> of 0.028 min<sup>-1</sup>. The system optimization and ROS evaluation suggest that high concentration of H<sub>2</sub>O<sub>2</sub> inhibited the degradation and quenched <span><math><msubsup><mtext>CO</mtext><mrow><mn>3</mn></mrow><mrow><mo>·</mo><mo>−</mo></mrow></msubsup></math></span> and <strong>·</strong>OH to yield <strong>·</strong>O<sub>2</sub><sup>-</sup> and <sup>1</sup>O<sub>2</sub>. Furthermore, EPR analysis and quenching experiments indicate that <span><math><msubsup><mtext>CO</mtext><mrow><mn>3</mn></mrow><mrow><mo>·</mo><mo>−</mo></mrow></msubsup></math></span> was mainly responsible for acetaminophen degradation. This work provides fundamental understanding of the HCO<sub>4</sub><sup>-</sup>-based oxidation system.</div></div>\",\"PeriodicalId\":443,\"journal\":{\"name\":\"Water Research\",\"volume\":\"268 \",\"pages\":\"Article 122750\"},\"PeriodicalIF\":11.4000,\"publicationDate\":\"2024-11-05\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Water Research\",\"FirstCategoryId\":\"93\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S004313542401649X\",\"RegionNum\":1,\"RegionCategory\":\"环境科学与生态学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"ENGINEERING, ENVIRONMENTAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Water Research","FirstCategoryId":"93","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S004313542401649X","RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENGINEERING, ENVIRONMENTAL","Score":null,"Total":0}
引用次数: 0

摘要

利用 HCO3- 和 H2O2 反应生成的过氧化单碳酸盐(HCO4-)的高级氧化工艺,被用于去除水中的污染物。然而,H2O2 在这些过程中的确切作用仍是一个争论的话题。本研究利用 NaHCO3 和 H2O2 建立了一个基于 HCO4 的氧化系统来降解对乙酰氨基酚,并研究了共存氧化剂的活化机制。在热激活条件下,HCO4-(HO-OCOO-)中的O-O键比共存氧化剂H2O2(HO-OH)中的O-O键更容易裂解,从而产生活性氧(ROS)。根据动力学和 ROS 评估,H2O2 主要用于形成 HCO4-,而不是转化为 -OH 或 O2,HCO4- 通过形成 CO3-- 和 -OH 成为降解的主要氧化剂。在该氧化体系中,20 mM HCO3- 和 20 mM H2O2 在 60 °C 条件下,产生 -OH 的 H2O2 利用率达到 27.34%,-OH 产量达到 24.15%,对乙酰氨基酚的降解效率达到 83%。计算得出的对乙酰氨基酚降解表观活化能和 HCO4- 活化表观活化能分别为 90.83 kJ mol-1 和 18.81 kJ mol-1。此外,基于 CO2 衍生 HCO4- 的新型系统的对乙酰氨基酚降解效率为 82%,Kobs 为 0.028 min-1。系统优化和 ROS 评估表明,高浓度 H2O2 可抑制降解,并淬灭 CO3-- 和 -OH 生成 -O2- 和 1O2。此外,EPR 分析和淬灭实验表明 CO3--是对乙酰氨基酚降解的主要原因。这项研究为了解基于 HCO4 的氧化系统提供了基础。
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

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
Reconsideration of the role of hydrogen peroxide in peroxymonocarbonate-based oxidation system for pollutant control
Advanced oxidation processes that utilize peroxymonocarbonate (HCO4-), generated in-situ through the reaction of HCO3- and H2O2, are employed for the removal of pollutants in water. Nevertheless, the precise role of H2O2 in these processes remains a subject of debate. This study established a HCO4--based oxidation system using NaHCO3 and H2O2 for the degradation of acetaminophen and investigated the activation mechanisms of coexisting oxidants. Under thermal activation conditions, the OO bond in HCO4- (HOOCOO-) was more readily cleaved than the OO bond in the co-existing oxidant H2O2 (HOOH), leading to the generation of reactive oxygen species (ROS). Based on kinetics and ROS evaluation, H2O2 primarily served to form HCO4- rather than converting to ·OH or O2, with HCO4- acting as the primary oxidant for degradation through the formation of CO3·and ·OH. In this oxidation system, H2O2 utilization efficiency for ·OH production reached 27.34 %, ·OH yield reached 24.15 % and acetaminophen degradation efficiency realized 83 % at 60 °C with 20 mM HCO3- and 20 mM H2O2. The apparent activation energy of acetaminophen degradation and HCO4- activation were calculated as 90.83 kJ mol-1 and 18.81 kJ mol-1, respectively. Moreover, a novel CO2-derived HCO4--based system led to a comparable acetaminophen degradation efficiency of 82 % and a higher kobs of 0.028 min-1. The system optimization and ROS evaluation suggest that high concentration of H2O2 inhibited the degradation and quenched CO3· and ·OH to yield ·O2- and 1O2. Furthermore, EPR analysis and quenching experiments indicate that CO3· was mainly responsible for acetaminophen degradation. This work provides fundamental understanding of the HCO4--based oxidation system.
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
Water Research
Water Research 环境科学-工程:环境
CiteScore
20.80
自引率
9.40%
发文量
1307
审稿时长
38 days
期刊介绍: Water Research, along with its open access companion journal Water Research X, serves as a platform for publishing original research papers covering various aspects of the science and technology related to the anthropogenic water cycle, water quality, and its management worldwide. The audience targeted by the journal comprises biologists, chemical engineers, chemists, civil engineers, environmental engineers, limnologists, and microbiologists. The scope of the journal include: •Treatment processes for water and wastewaters (municipal, agricultural, industrial, and on-site treatment), including resource recovery and residuals management; •Urban hydrology including sewer systems, stormwater management, and green infrastructure; •Drinking water treatment and distribution; •Potable and non-potable water reuse; •Sanitation, public health, and risk assessment; •Anaerobic digestion, solid and hazardous waste management, including source characterization and the effects and control of leachates and gaseous emissions; •Contaminants (chemical, microbial, anthropogenic particles such as nanoparticles or microplastics) and related water quality sensing, monitoring, fate, and assessment; •Anthropogenic impacts on inland, tidal, coastal and urban waters, focusing on surface and ground waters, and point and non-point sources of pollution; •Environmental restoration, linked to surface water, groundwater and groundwater remediation; •Analysis of the interfaces between sediments and water, and between water and atmosphere, focusing specifically on anthropogenic impacts; •Mathematical modelling, systems analysis, machine learning, and beneficial use of big data related to the anthropogenic water cycle; •Socio-economic, policy, and regulations studies.
期刊最新文献
Trophic status and metabolic rates of threatened shallow saline lakes in Central Spain: providing diagnostic elements for improving management strategies Seamless observations of chlorophyll-a from OLCI and VIIRS measurements in inland lakes Different Wetting States in Riparian Sediment Ecosystems: Response to Microplastics Exposure Prioritization of monitoring compounds from SNTS identified organic micropollutants in contaminated groundwater using a machine learning optimized ToxPi model Metagenomic insights into nitrite accumulation in sulfur-based denitrification systems utilizing different electron donors: functional microbial communities and metabolic mechanisms
×
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学术文献互助
Book学术文献互助群
群 号:481959085
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