Ying Wang , Guangliang Liu , Yingying Fang , Peng Liu , Yanwei Liu , Yingying Guo , Jianbo Shi , Ligang Hu , Yong Cai , Yongguang Yin , Guibin Jiang
{"title":"汞滴的暗氧化：汞[Hg（I）]物质控制转化动力学。","authors":"Ying Wang , Guangliang Liu , Yingying Fang , Peng Liu , Yanwei Liu , Yingying Guo , Jianbo Shi , Ligang Hu , Yong Cai , Yongguang Yin , Guibin Jiang","doi":"10.1016/j.watres.2023.120472","DOIUrl":null,"url":null,"abstract":"<div><p>Liquid elemental mercury droplet (Hg(0)<sub>l</sub>) is an important species in heavy Hg-contaminated environments. The oxidation processes of Hg(0)<sub>l</sub><span> and its related mechanisms are still poorly understood. Herein, for the first time, it was verified that mercurous species [Hg(I)] was an important species in natural water contaminated by Hg(0)</span><sub>l</sub> as well as in the simulated dark oxidation of Hg(0)<sub>l</sub>. The formation and further transformation of Hg(I) controlled the overall oxidation process of Hg(0)<sub>l</sub> and were affected by different environmental factors. Through kinetic modeling using ACUCHEM program, oxidation of Hg(0) to Hg(I) (Hg(0) → Hg(I)) was determined to be the rate-limiting step in Hg(0)<sub>l</sub> oxidation because its <em>k</em> value ((8.7 ± 0.21) × 10<sup>−11</sup> <em>s</em><sup>−1</sup>) is seven orders of magnitude lower than that of Hg(I) oxidation (Hg(I) → Hg(II), (4.7 ± 0.15) × 10<sup>−4</sup> <em>s</em><sup>−1</sup>). Ligands like OH<sup>−</sup>, Cl<sup>−</sup>, and natural organic matter enhanced the formation of Hg(I) via promoting the constants of comproportionation (up to (9.5 ± 0.78) × 10<sup>−4</sup> <em>s</em><sup>−1</sup>). These findings highlight the importance of Hg(I) in Hg(0)<sub>l</sub> oxidation process by controlling the transformation kinetics of Hg species, facilitating an improved understanding of the environmental redox cycles of Hg.</p></div>","PeriodicalId":443,"journal":{"name":"Water Research","volume":"244 ","pages":"Article 120472"},"PeriodicalIF":11.4000,"publicationDate":"2023-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Dark oxidation of mercury droplet: Mercurous [Hg(I)] species controls transformation kinetics\",\"authors\":\"Ying Wang , Guangliang Liu , Yingying Fang , Peng Liu , Yanwei Liu , Yingying Guo , Jianbo Shi , Ligang Hu , Yong Cai , Yongguang Yin , Guibin Jiang\",\"doi\":\"10.1016/j.watres.2023.120472\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>Liquid elemental mercury droplet (Hg(0)<sub>l</sub>) is an important species in heavy Hg-contaminated environments. The oxidation processes of Hg(0)<sub>l</sub><span> and its related mechanisms are still poorly understood. Herein, for the first time, it was verified that mercurous species [Hg(I)] was an important species in natural water contaminated by Hg(0)</span><sub>l</sub> as well as in the simulated dark oxidation of Hg(0)<sub>l</sub>. The formation and further transformation of Hg(I) controlled the overall oxidation process of Hg(0)<sub>l</sub> and were affected by different environmental factors. Through kinetic modeling using ACUCHEM program, oxidation of Hg(0) to Hg(I) (Hg(0) → Hg(I)) was determined to be the rate-limiting step in Hg(0)<sub>l</sub> oxidation because its <em>k</em> value ((8.7 ± 0.21) × 10<sup>−11</sup> <em>s</em><sup>−1</sup>) is seven orders of magnitude lower than that of Hg(I) oxidation (Hg(I) → Hg(II), (4.7 ± 0.15) × 10<sup>−4</sup> <em>s</em><sup>−1</sup>). Ligands like OH<sup>−</sup>, Cl<sup>−</sup>, and natural organic matter enhanced the formation of Hg(I) via promoting the constants of comproportionation (up to (9.5 ± 0.78) × 10<sup>−4</sup> <em>s</em><sup>−1</sup>). These findings highlight the importance of Hg(I) in Hg(0)<sub>l</sub> oxidation process by controlling the transformation kinetics of Hg species, facilitating an improved understanding of the environmental redox cycles of Hg.</p></div>\",\"PeriodicalId\":443,\"journal\":{\"name\":\"Water Research\",\"volume\":\"244 \",\"pages\":\"Article 120472\"},\"PeriodicalIF\":11.4000,\"publicationDate\":\"2023-10-01\",\"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/S0043135423009120\",\"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/S0043135423009120","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}
Dark oxidation of mercury droplet: Mercurous [Hg(I)] species controls transformation kinetics
Liquid elemental mercury droplet (Hg(0)l) is an important species in heavy Hg-contaminated environments. The oxidation processes of Hg(0)l and its related mechanisms are still poorly understood. Herein, for the first time, it was verified that mercurous species [Hg(I)] was an important species in natural water contaminated by Hg(0)l as well as in the simulated dark oxidation of Hg(0)l. The formation and further transformation of Hg(I) controlled the overall oxidation process of Hg(0)l and were affected by different environmental factors. Through kinetic modeling using ACUCHEM program, oxidation of Hg(0) to Hg(I) (Hg(0) → Hg(I)) was determined to be the rate-limiting step in Hg(0)l oxidation because its k value ((8.7 ± 0.21) × 10−11s−1) is seven orders of magnitude lower than that of Hg(I) oxidation (Hg(I) → Hg(II), (4.7 ± 0.15) × 10−4s−1). Ligands like OH−, Cl−, and natural organic matter enhanced the formation of Hg(I) via promoting the constants of comproportionation (up to (9.5 ± 0.78) × 10−4s−1). These findings highlight the importance of Hg(I) in Hg(0)l oxidation process by controlling the transformation kinetics of Hg species, facilitating an improved understanding of the environmental redox cycles of Hg.
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.
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