Critical review of advanced oxidation processes in organic wastewater treatment.

What is the role of light in persulfate-based advanced oxidation for water treatment?

Density Functional Theory Calculations for Insight into the Heterocatalyst Reactivity and Mechanism in Persulfate-Based Advanced Oxidation Reactions

Advanced oxidation processes (AOPs) can degrade a wide range of trace organic contaminants (TrOCs) to improve the quality of potable water or discharged wastewater effluents. Their effectiveness is impacted, however, by the dissolved organic matter (DOM) that is ubiquitous in all water sources. During the application of an AOP, DOM can scavenge radicals and/or block light penetration, therefore impacting their effectiveness toward contaminant transformation. The multiple ways in which different types or sources of DOM can impact oxidative water purification processes are critically reviewed. DOM can inhibit the degradation of TrOCs, but it can also enhance the formation and reactivity of useful radicals for contaminants elimination and alter the transformation pathways of contaminants. An in-depth analysis highlights the inhibitory effect of DOM on the degradation efficiency of TrOCs based on DOM's structure and optical properties and its reactivity toward oxidants as well as the synergistic contribution of DOM to the transformation of TrOCs from the analysis of DOM's redox properties and DOM's transient intermediates. AOPs can alter DOM structure properties as well as and influence types, mechanisms, and extent of oxidation byproducts formation. Research needs are proposed to advance practical understanding of how DOM can be exploited to improve oxidative water purification. 

Multiple Roles of Dissolved Organic Matter in Advanced Oxidation Processes

Urbanization and industrialization have exerted significant adverse effects on water quality, resulting in a growing need for reliable and eco-friendly treatment technologies. Persulfate (PS)-based advanced oxidation processes (AOPs) are emerging as viable technologies to treat challenging industrial wastewaters or remediate groundwater impacted by hazardous wastes. While the generated reactive species can degrade a variety of priority organic contaminants through radical and nonradical pathways, there is a lack of systematic and in-depth comparison of these pathways for practical implementation in different treatment scenarios. Our comparative analysis of reaction rate constants for radical vs. nonradical species indicates that radical-based AOPs may achieve high removal efficiency of organic contaminants with relatively short contact time. Nonradical AOPs feature advantages with minimal water matrix interference for complex wastewater treatments. Nonradical species (e.g., singlet oxygen, high-valent metals, and surface activated PS) preferentially react with contaminants bearing electron-donating groups, allowing enhancement of degradation efficiency of known target contaminants. For byproduct formation, analytical limitations and computational chemistry applications are also considered. Finally, we propose a holistically estimated electrical energy per order of reaction (EE/O) parameter and show significantly higher energy requirements for the nonradical pathways. Overall, these critical comparisons help prioritize basic research on PS-based AOPs and inform the merits and limitations of system-specific applications. 

Merits and Limitations of Radical vs. Nonradical Pathways in Persulfate-Based Advanced Oxidation Processes.

Metal-free carbocatalysis for persulfate activation toward nonradical oxidation: Enhanced singlet oxygen generation based on active sites and electronic property

Crucial roles of oxygen and superoxide radical in bisulfite-activated persulfate oxidation of bisphenol AF: Mechanisms, kinetics and DFT studies.

ROS reevaluation for degradation of 4-chloro-3,5-dimethylphenol (PCMX) by UV and UV/persulfate processes in the water: Kinetics, mechanism, DFT studies and toxicity evolution

Staged assessment for the involving mechanism of humic acid on enhancing water decontamination using H2O2-Fe(III) process.

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Papers

Metal-free carbocatalysis for persulfate activation toward nonradical oxidation: Enhanced singlet oxygen generation based on active sites and electronic property

Crucial roles of oxygen and superoxide radical in bisulfite-activated persulfate oxidation of bisphenol AF: Mechanisms, kinetics and DFT studies.

ROS reevaluation for degradation of 4-chloro-3,5-dimethylphenol (PCMX) by UV and UV/persulfate processes in the water: Kinetics, mechanism, DFT studies and toxicity evolution

Staged assessment for the involving mechanism of humic acid on enhancing water decontamination using H2O2-Fe(III) process.