Fe(III)-Doped g-C₃N₄ Mediated Peroxymonosulfate Activation for Selective Degradation of Phenolic Compounds via High-Valent Iron-Oxo Species

Abstract

Herein, we proposed a new peroxymonosulfate (PMS) activation system employing the Fe(III) doped g-CN (CNF) as catalyst. Quite different from traditional sulfate radical-based advanced oxidation processes (SR-AOPs), the PMS/CNF system was capable of selectively degrading phenolic compounds (e.g., p-chlorophenol, 4-CP) in a wide pH range (3-9) via nonradical pathway. The generated singlet oxygen (O) in the PMS/CNF3 (3.46 wt % Fe) system played negligible role in removing 4-CP, and high-valent iron-oxo species fixated in the nitrogen pots of g-CN (≡Fe═O) was proposed as the dominant reactive species by using dimethyl sulfoxide as a probe compound. The mechanism was hypothesized that PMS was first bound to the Fe(III)-N moieties to generate ≡Fe═O, which effectively reacted with 4-CP via electron transfer. GC-MS analysis indicated that 4-chlorocatechol and 1,4-benzoquinone were the major intermediates, which could be further degraded to carboxylates. The kinetic results suggested that the formation of ≡Fe═O was proportional to the dosages of PMS and CNF3 under the experimental conditions. Also, the PMS/CNF3 system exhibited satisfactory removal of 4-CP in the presence of inorganic anions and natural organic matters. We believe that this study will provide a new routine for effective PMS activation by heterogeneous iron-complexed catalysts to efficiently degrade organic contaminants via nonradical pathway.

Modulating the Electronic Structure of Single‐Atom Catalysts on 2D Nanomaterials for Enhanced Electrocatalytic Performance

“…When incorporating a small amount of metal into the precursors, the g‐C 3 N 4 nanosheets doped with individual metal atoms can be facilely obtained. For instance, Sr, Co, and Fe doped g‐C 3 N 4 have been synthesized without defining the structure of the metal atoms in g‐C 3 N 4 matrix . In a modified strategy reported by Chen et al, the as‐prepared silver tricyanomethanide was used as a miscible and reactive metal precursor to cocondensation with cyanamide, which ensured the homogeneity of the single atom dispersed Ag coordinated with g‐C 3 N 4 .…”

Adsorption Characteristics of Phenolic Compounds on Graphene Oxide and Reduced Graphene Oxide: A Batch Experiment Combined Theory Calculation

“…A large number of studies have focused on waste water purification contaminated by phenols, and various techniques have been developed to efficiently remove them. At present, the most widely used methods for phenol removal have included biological degradation [2,3], photocatalytic decomposition [4,5], chemical oxidation [6,7], 2 of 13 hydrodynamic cavitation [8,9] and adsorption [10][11][12][13]. Among these approaches, adsorption seem to have a particular advantage due to its relatively low cost, speed and convenience of operation.…”

Fine‐Tuning Surface Properties of Perovskites via Nanocompositing with Inert Oxide toward Developing Superior Catalysts for Advanced Oxidation

“…The reactive species generated in L 1.15 FO/H 2 O 2 system were confirmed by the quenching tests and in situ EPR technique as shown in Figure a–c. Ethanol (EtOH) and furfuryl alcohol (FFA) were chosen as the scavengers of hydroxyl radical ( • OH) and singlet oxygen ( 1 O 2 ), respectively . Figure a witnessed that FFA (0.05 m ) exhibited more serious inhibition on MO degradation and only 72% of MO was removed in 70 min, compared with EtOH (0.05 m ).…”