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Journal ArticleDOI

N-Doping-Induced Nonradical Reaction on Single-Walled Carbon Nanotubes for Catalytic Phenol Oxidation

TLDR
In this paper, N-doped carbon nanotubes (NoCNTs) were employed as metal-free catalysts for phenol catalytic oxidation with sulfate radicals and, more importantly, a detailed mechanism of peroxymonosulfate (PMS) activation and the roles of nitrogen heteroatoms were comprehensively investigated.
Abstract
Metal-free materials have been demonstrated to be promising alternatives to conventional metal-based catalysts. Catalysis on nanocarbons comparable to that of cobalt- or manganese-based catalysts in peroxymonosulfate (PMS) activation has been achieved, yet the catalyst stability has to be addressed and the mechanism also needs to be elucidated. In this study, N-doped carbon nanotubes (NoCNTs) were employed as metal-free catalysts for phenol catalytic oxidation with sulfate radicals and, more importantly, a detailed mechanism of PMS activation and the roles of nitrogen heteroatoms were comprehensively investigated. For the first time, a nonradical pathway accompanied by radical generation (•OH and SO4•–) in phenol oxidation with PMS was discovered upon nitrogen heteroatom doping. The NoCNTs presented excellent stability due to the emerging nonradical processes. The findings can be used for the design of efficient and robust metal-free catalysts with both superior catalytic performance and high stability fo...

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Journal ArticleDOI

Generation of sulfate radical through heterogeneous catalysis for organic contaminants removal: Current development, challenges and prospects

TL;DR: In this paper, the authors provide a state-of-the-art review on the development in heterogeneous catalysts including single metal, mixed metal, and nonmetal carbon catalysts for organic contaminants removal, with particular focus on peroxymonosulfate (PMS) activation.
Journal ArticleDOI

Persulfate-Based Advanced Oxidation: Critical Assessment of Opportunities and Roadblocks.

TL;DR: This Critical Review comparatively examines the activation mechanisms of peroxymonosulfate and peroxydisulfates and the formation pathways of oxidizing species and the impacts of water parameters and constituents such as pH, background organic matter, halide, phosphate, and carbonate on persulfate-driven chemistry.
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Single Cobalt Atoms Anchored on Porous N-Doped Graphene with Dual Reaction Sites for Efficient Fenton-like Catalysis

TL;DR: Dual reaction sites anchored on porous N-doped graphene with dual reaction sites as highly reactive and stable Fenton-like catalysts for efficient catalytic oxidation of recalcitrant organics via activation of peroxymonosulfate (PMS).
Journal ArticleDOI

Metal-free carbocatalysis in advanced oxidation reactions

TL;DR: This Account showcases the recent contributions to metal-free catalysis in advanced oxidation, including design of nanocarbon catalysts, exploration of intrinsic active sites, and identification of reactive species and reaction pathways, and offers perspectives on carbocatalysis for future environmental applications.
Journal ArticleDOI

Activation of peroxymonosulfate by base: Implications for the degradation of organic pollutants.

TL;DR: The results revealed that superoxide anion radical and singlet oxygen other than sulfate radical were the primary reactive oxygen species in the Base/PMS system and presented a new pathway for PMS activation and provide useful information for the treatment of wastewater.
References
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Journal ArticleDOI

Critical Review of rate constants for reactions of hydrated electrons, hydrogen atoms and hydroxyl radicals (⋅OH/⋅O− in Aqueous Solution

TL;DR: In this article, the rate constants for over 3500 reaction are tabulated, including reaction with molecules, ions and other radicals derived from inorganic and organic solutes, and the corresponding radical anions, ⋅O− and eaq−, have been critically pulse radiolysis, flash photolysis and other methods.
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Rate Constants for Reactions of Inorganic Radicals in Aqueous Solution

TL;DR: In this article, rate constants have been compiled for reactions of various inorganic radicals produced by radiolysis or photolysis, as well as by other chemical means in aqueous solutions.
Journal ArticleDOI

Radical generation by the interaction of transition metals with common oxidants.

TL;DR: Nine transition metals were tested for the activation of three oxidants and the generation of inorganic radical species such as sulfate, peroxymonosulfate, and hydroxyl radicals to postulate the rate-determining step of the redox reactions taking place when a metal is coupled with an oxidant in aqueous solution.
Journal ArticleDOI

Catalyst-Free Synthesis of Nitrogen-Doped Graphene via Thermal Annealing Graphite Oxide with Melamine and Its Excellent Electrocatalysis

TL;DR: A facile, catalyst-free thermal annealing approach for large-scale synthesis of NG using low-cost industrial material melamine as the nitrogen source is proposed, which can completely avoid the contamination of transition metal catalysts, and thus the intrinsic catalytic performance of pure NGs can be investigated.
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