Fuqiang Liu, Yang Liu, Hongyu Dong, Huixin Shao, Bin Su, Tianshu Zhou, Xiaohong Guan
{"title":"以过氧化二硫酸盐和对苯二酚为核心反应物的硫酸根自由基介导的化学发光:机理与环境应用","authors":"Fuqiang Liu, Yang Liu, Hongyu Dong, Huixin Shao, Bin Su, Tianshu Zhou, Xiaohong Guan","doi":"10.1021/acsestengg.4c00219","DOIUrl":null,"url":null,"abstract":"Chemiluminescence (CL) is an attractive method for real-time quantification of toxic contaminants or intermediates generated during advanced oxidation processes due to its high sensitivity, low detection limit, and wide linear range. In this study, we present an unprecedented intrinsic CL phenomenon observed in an alkaline aqueous solution containing hydroquinone (HQ) and peroxydisulfate (PDS, S<sub>2</sub>O<sub>8</sub><sup>2–</sup>). Mechanistic investigations unveil a two-stage process for CL production: sulfate radical (SO<sub>4</sub><sup>•–</sup>) generation and CL emission. Initially, the highly oxidizing SO<sub>4</sub><sup>•–</sup> are formed via the decomposition of PDS by semiquinone radicals, originating from the comproportionation reaction of HQ with benzoquinone that is generated by the reaction of HQ with OH<sup>–</sup> in the presence of dissolved oxygen. Subsequently, SO<sub>4</sub><sup>•–</sup> promptly oxidizes the residual HQ to an excited-state light-emitting species, which returns to its ground-state, accompanied by a transient and intense light emission. Notably, HQ plays dual roles in the CL process by both participating in the generation of SO<sub>4</sub><sup>•–</sup> and serving as the precursor of the light-emitting substrate. The proposed CL system is developed to quantify trace amounts of HQ and real-time monitor the degradation kinetics of phenols. These findings hold considerable significance in chemical analysis, intermediate identification, and advanced oxidation processes.","PeriodicalId":7008,"journal":{"name":"ACS ES&T engineering","volume":null,"pages":null},"PeriodicalIF":7.4000,"publicationDate":"2024-06-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Sulfate Radicals-Mediated Chemiluminescence Production with Peroxydisulfate and Hydroquinone as Coreactants: Mechanism and Environmental Applications\",\"authors\":\"Fuqiang Liu, Yang Liu, Hongyu Dong, Huixin Shao, Bin Su, Tianshu Zhou, Xiaohong Guan\",\"doi\":\"10.1021/acsestengg.4c00219\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Chemiluminescence (CL) is an attractive method for real-time quantification of toxic contaminants or intermediates generated during advanced oxidation processes due to its high sensitivity, low detection limit, and wide linear range. In this study, we present an unprecedented intrinsic CL phenomenon observed in an alkaline aqueous solution containing hydroquinone (HQ) and peroxydisulfate (PDS, S<sub>2</sub>O<sub>8</sub><sup>2–</sup>). Mechanistic investigations unveil a two-stage process for CL production: sulfate radical (SO<sub>4</sub><sup>•–</sup>) generation and CL emission. Initially, the highly oxidizing SO<sub>4</sub><sup>•–</sup> are formed via the decomposition of PDS by semiquinone radicals, originating from the comproportionation reaction of HQ with benzoquinone that is generated by the reaction of HQ with OH<sup>–</sup> in the presence of dissolved oxygen. Subsequently, SO<sub>4</sub><sup>•–</sup> promptly oxidizes the residual HQ to an excited-state light-emitting species, which returns to its ground-state, accompanied by a transient and intense light emission. Notably, HQ plays dual roles in the CL process by both participating in the generation of SO<sub>4</sub><sup>•–</sup> and serving as the precursor of the light-emitting substrate. The proposed CL system is developed to quantify trace amounts of HQ and real-time monitor the degradation kinetics of phenols. 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Sulfate Radicals-Mediated Chemiluminescence Production with Peroxydisulfate and Hydroquinone as Coreactants: Mechanism and Environmental Applications
Chemiluminescence (CL) is an attractive method for real-time quantification of toxic contaminants or intermediates generated during advanced oxidation processes due to its high sensitivity, low detection limit, and wide linear range. In this study, we present an unprecedented intrinsic CL phenomenon observed in an alkaline aqueous solution containing hydroquinone (HQ) and peroxydisulfate (PDS, S2O82–). Mechanistic investigations unveil a two-stage process for CL production: sulfate radical (SO4•–) generation and CL emission. Initially, the highly oxidizing SO4•– are formed via the decomposition of PDS by semiquinone radicals, originating from the comproportionation reaction of HQ with benzoquinone that is generated by the reaction of HQ with OH– in the presence of dissolved oxygen. Subsequently, SO4•– promptly oxidizes the residual HQ to an excited-state light-emitting species, which returns to its ground-state, accompanied by a transient and intense light emission. Notably, HQ plays dual roles in the CL process by both participating in the generation of SO4•– and serving as the precursor of the light-emitting substrate. The proposed CL system is developed to quantify trace amounts of HQ and real-time monitor the degradation kinetics of phenols. These findings hold considerable significance in chemical analysis, intermediate identification, and advanced oxidation processes.
期刊介绍:
ACS ES&T Engineering publishes impactful research and review articles across all realms of environmental technology and engineering, employing a rigorous peer-review process. As a specialized journal, it aims to provide an international platform for research and innovation, inviting contributions on materials technologies, processes, data analytics, and engineering systems that can effectively manage, protect, and remediate air, water, and soil quality, as well as treat wastes and recover resources.
The journal encourages research that supports informed decision-making within complex engineered systems and is grounded in mechanistic science and analytics, describing intricate environmental engineering systems. It considers papers presenting novel advancements, spanning from laboratory discovery to field-based application. However, case or demonstration studies lacking significant scientific advancements and technological innovations are not within its scope.
Contributions containing experimental and/or theoretical methods, rooted in engineering principles and integrated with knowledge from other disciplines, are welcomed.