Sulfate Radical-based Advanced Oxidation Processes Research Articles

Bimetallic iron-nickel phosphide as efficient peroxymonosulfate activator for tetracycline hydrochloride degradation: Performance and mechanism

Sulfate radical-based advanced oxidation processes with (SR-AOPs) are widely employed to degrade organic pollutants due to their high efficiency, cost-effectiveness and safety. In this study, a highly active and stable FeNiP was successfully prepared by reduction and heat treatment. FeNiP exhibited high performance of peroxymonosulfate (PMS) activation for tetracycline hydrochloride (TC) removal. Over a wide pH range, an impressive TC degaradation efficiency 97.86% was achieved within 60 min employing 0.1 g/L FeNiP and 0.2 g/L PMS at room temperature. Both free radicals of SO4·-, ·OH, ·O2− and non-free radicals of 1O2 participated the TC degradation in the FeNiP/PMS system. The PMS activation ability was greatly enhanced by the cycling between Ni and Fe bimetal, and the active site regeneration was achieved due to the existence of the negatively charged Pn−. Moreover, the FeNiP/PMS system exhibited substantial TC degradation levels in both simulated real-world disturbance scenarios and practical water tests. Cycling experiments further affirmed the robust stability of FeNiP catalyst, demonstrating sustained degradation efficiency of approximately 80% even after four cycles. These findings illuminate its promising potential across natural water bodies, presenting an innovative catalyst construction approach for PMS activation in the degradation of antibiotic pollutants.

Enhanced antibiotic degradation via photo-assisted peroxymonosulfate over graphitic carbon nitride nanosheets/CuBi2O4: Highly efficiency of oxygen activation and interfacial charge transfer

Improving the activation capacity of peroxymonosulfate (PMS) to increase radical and non-radical production is critical for antibiotic degradation. However, how to boost reactive oxygen species (ROS) and speed interfacial charge transfer remains an essential challenge. We report a coupling system of 10 %CNNS/CuBi2O4 photocatalyst and sulfate radical-based advanced oxidation processes (SO4−-AOPs) to enhance the activation of PMS and improve antibiotic degradation. Owing to highly efficient oxygen activation and interfacial charge transfer, the degradation efficiency of the photo-assisted PMS system was as high as 51.6 times and 2.8 times that of photocatalyst and SO4−-AOPs alone, respectively. Importantly, the highly efficient oxygen activation resulted in the production of O2−, which in turn could utilize the excess electrons generated through efficient interfacial charge transfer to convert into non-radical 1O2. The total organic carbon (TOC) elimination effectiveness of the photo-assisted PMS system reached 82 % via the synergy of radicals and non-radicals (O2−, OH, 1O2, SO4−, h+). This system also had excellent potential for reducing the generation and toxicity of disinfection by-products (DBPs), as evidenced through significant reductions in concentrations of trichloromethane (TCM), dichloroacetic acid (DCAA), and trichloronitromethane (TCNM) by 76 %, 64 %, and 35 %, respectively, providing an effective and eco-friendly strategy for antibiotic treatment.

Photocatalytic Degradation of Rhodamine B via Fe-g-C3N4 Activated Sulfate Radical-Based Advanced Oxidation Processes and the Synergistic Mechanism

Photocatalytic Degradation of Rhodamine B via Fe-g-C3N4 Activated Sulfate Radical-Based Advanced Oxidation Processes and the Synergistic Mechanism

Green rGO/FeNPs nanocomposites activated peroxydisulfate for the removal of mixed 17β-estradiol and estriol

Reduced graphene oxide/iron nanoparticles (rGO/FeNPs) synthesized by the chemical method have been used in Fenton oxidation of organic contaminants, yet little is known about biosynthesized rGO/FeNPs using green tea extract (GT) as how to activate persulfate in sulfate radical-based advanced oxidation processes. In this study, rGO/FeNPs were used to activate peroxydisulfate (PDS) for 17β-estradiol (βE2) and estriol (E3) removal. The rGO/FeNPs-PDS system removed 83.6% of βE2 and 62.5% of E3 within 240 min, which was confirmed by a combination of adsorption and degradation via both radical and non-radical pathways. Four main reactive species in βE2 and E3 degradation were observed, i.e., hydroxyl radical (·OH), sulfate radical (SO4·−), singlet oxygen (1O2) and electron transfer, with the respective contributions of ·OH (32.9 and 34.7%), SO4·− (16.1 and 19.7%), 1O2 (12.2 and 14.1%) and electron transfer (8.0 and 7.2%). Analysis of X-ray photoelectron spectroscopy (XPS), Fourier transform infrared (FTIR), Electron Paramagnetic Resonance (EPR) and electrochemical measurements all indicated that beside the well-known role of Fe, CO from rGO through the generation of ·OH, SO4·−, 1O2 and electron transfer, as well as GT through electron transfer also participated in the activation of PDS. Finally, the degradation pathways of βE2/E3 were proposed. Overall, this study provides a new insight into the biosynthesis of rGO/FeNPs to activate PDS for the oxidation of mixed emerging contaminants.

Pilot-scale sulfate radical-based advanced oxidation for wastewater reuse: simultaneous disinfection, removal of contaminants of emerging concern, and antibiotic resistance genes

Wastewater reuse addresses water scarcity, but contaminants of emerging concern (CECs), pathogens and antibiotic resistance genes (ARGs) pose health and environmental risks. The European Union (EU) has enacted Regulation (EU) 2020/741, establishing wastewater reuse standards for agriculture. This study evaluates for the first time the effectiveness of four sulfate radical-based advanced oxidation processes (SR-AOPs), based on the combination of peroxymonosulfate (PMS) with O3 and H2O2, applied at pilot plant, for the simultaneous elimination of microorganisms, CECs, and ARGs, in actual urban wastewater treatment plant (UWWTP) effluents. The system PMS/H2O2/UV-A improved the disinfection effectiveness, compared to PMS/UV-A, especially using a molar ratio 1:3 (0.5 mM PMS:1.5 mM H2O2), achieving complete elimination of total aerobic microorganisms in 90 min. However, this double oxidation system, does not improve CECs removal compared to PMS/UV-A in neither of the two molar ratios studied (1:1 or 1:3), and none of these treatments significantly reduced the prevalence of ARGs. However, the PMS/O3 system demonstrated the ability to remove total aerobic microorganisms in 20 min and Escherichia coli in 5 min, 94 % of CECs, and 6 out of the 8 ARGs, demonstrating to be the most effective treatment. However, the system showed phytotoxicity, inhibiting seed growth by 10–30 %, probably associated with the by-products formed in the reaction between organic matter and ozone. This result highlights that SR-AOPs are promising processes with the capability to achieve the simultaneous removal of different contaminant groups, reducing the risks associated with wastewater reuse. Their application at larger scales is increasingly closer.

Single‐Atom Catalysts Originated from Metal–Organic Frameworks for Sulfate Radical‐Based Advanced Oxidation Processes: Critical Insights into Mechanisms

AbstractThe widely discussed single‐atom catalysts (SACs) are regarded as a kind of attractive material for sulfate radical‐based advanced oxidation processes (SR‐AOPs) owing to their maximum atomic utilization efficiency and outstanding stability. Currently, metal–organic frameworks (MOFs) have appeared as prospective precursors for building SACs due to extensive chelating sites, functional adjustability, and structural tunability. However, there are few critical and systematic reviews about the application of MOF‐derived SACs in SR‐AOPs, especially in‐depth analysis of the mechanisms. Therefore, this review seeks to offer a thorough summary of the development of MOF‐derived SACs in SR‐AOPs. First, the unique advantages of MOFs as derivative precursors for SACs are discussed thoroughly. Afterward, the current synthesis strategies are elaborated categorically to unveil the formation process of single atoms and their coordination environments. Notably, the roles of different reaction sites including the generation of reactive species and mediating electron transfer are further analyzed to explain mechanisms comprehensively. Thereafter, the characterization techniques and theoretical calculations for mechanisms studies are also highlighted. Eventually, critical insights into present challenges and future developments are proposed, which are expected to enhance the catalytic efficiency of MOF‐derived SACs in SR‐AOPs.

CuFeS2 supported on dendritic mesoporous silica-titania for persulfate-assisted degradation of sulfamethoxazole under visible light

Sulfamethoxazole (SMX) is a prevalent sulfonamide antibiotic found in the environment, and it has a variety of detrimental effects on environmental sustainability and water safety. Recently, the combination of photocatalysis and sulfate radical-based advanced oxidation processes (SR-AOPs) has attracted a lot of interest as a viable technique for degradation of refractory pollutants. In this study, a visible light active CuFeS2 supported on dendritic mesoporous silica-titania (CuFeS2-DMST) photocatalyst was synthesized to improve the ability of TiO2 to activate persulfate (PS) by introducing CuFeS2 (Fe2+/Fe3+, Cu+/Cu2+ redox cycles). The CuFeS2-DMST/PS/Vis system demonstrated superior SMX degradation efficiency (88.9%, 0.0146 min−1) than TiO2 because of reduced e-/h+ recombination, excellent charge separation and mobility, and a greater surface area than TiO2. Furthermore, after four consecutive photocatalytic cycles, the system demonstrated moderate stability. From chemical quenching tests, O2●-, h+, 1O2, SO4●- and ●OH were found to be the main reactive oxidizing species. The formed intermediates during the degradation process were identified, and degradation mechanisms were proposed. This study proposes a viable technique for activating PS using a low-cost, stable, and high-surface-area TiO2-based photocatalyst, and this concept can be applied to design photocatalysts for water treatment.

Towards removal of PPCPs by advanced oxidation processes: A review

The continuous influx of emerging contaminants (ECs) into water bodies poses a significant threat to human health. Among these contaminants, pharmaceuticals and personal care products (PPCPs) are of particular concern due to their potential to exert adverse effects even at low concentrations. Therefore, it is imperative to explore methods for their effective removal or reduction to safeguard both human health and the ecological environment. Advanced oxidation processes (AOPs) have received substantial attention as promising treatment methods. AOPs are capable of efficiently treating water by generating reactive oxygen species (ROS) with potent oxidation properties, which can effectively eliminate various contaminants. This review delves into the diverse range of AOPs available, including ozonation, photocatalytic oxidation, the Fenton process, electrochemical oxidation, sulfate radicals-based advanced oxidation processes (SR-AOPs), and more. It also discusses the respective limitations and future prospects of these processes, aiming to provide insights into their potential for addressing the pressing issue of PPCP contamination in water bodies.

Ultrafast degradation of organic pollutants in an Fe3O4-CoS2-x activated persulfate catalytic system with an Fe-Co catalytic cycle involving oxygen and sulfur vacancies

Processes that ensure the rapid degradation of organic pollutants are urgently required in wastewater treatment. Heterogeneous catalysts in sulfate radical-based advanced oxidation processes (SR-AOPs) have a low catalytic efficiency, long reaction time, and are difficult to recover. Rationally designed magnetically separable Fe3O4-CoS2-0.4 that was rich in sulfur and oxygen vacancies was used as an efficient catalyst for peroxymonosulfate (PMS) activation to rapidly degrade various dyes and antibiotics. The synergistic effect of Fe, Co and S on the activation of PMS and the sulfur and oxygen vacancy generated by the composite greatly promoted the catalytic performance, in which the singlet oxygen (1O2) generated was the main active species in the degradation process. Fe3O4-CoS2-0.4 is easily separated from the reaction solution by magnets and shows good recyclability and stability in removing MB, achieving removal rates of 100%, 100% and 96.07% in the first, second and third cycles, respectively. Fe3O4-modified CoS2 also greatly reduces the ion leaching of cobalt ions and the secondary pollution. In addition, for several other typical dyes and antibiotics (metronidazole, phenol, tetracycline, levofloxacin, crystal violet, malachite green, and rhodamine B), high removal rates (100%, 100%, 88.3%, 90.3%, 100%, 100%, and 100%, respectively) were achieved in a short time.

Sulfate radical-based advanced oxidation process effects on tire wear particles aging and ecotoxicity

Tire wear particles (TWPs) are widely distributed in natural water and pose as major pollutants in aquatic environments. In this study, heat-activated persulfate (HPT) and ultraviolet-activated persulfate treatments (UPT) were employed to investigate the influence of sulfate radical (SO4−•)-based advanced oxidation process (SAOPs) on TWP physicochemical properties and to clarify their ecotoxic effects in laboratory-level studies. Results showed that the specific surface areas of TWPs increased after UPT but decreased after HPT. In terms of chemical properties, the increase of oxygen-containing functional groups on the surfaces of TWPs was more evident in UPT than that in HPT. The atrazine (ATZ) adsorption capacity of TWPs after HPT and UPT was increased compared with the untreated TWPs. Atrazine adsorbed by TWPs was easily resolved and released in artificial intestinal fluid (1.89–2.08 mg/g) and artificial gastric fluid (1.60–2.04 mg/g) conditions. Acute toxicity experiments of Photobacterium phosphoreum and SEM-EDS detection results suggested that various heavy metals (e.g., Zn2+, Cu2+) in the TWPs would be released into the water system in SAOPs. ATZ released from TWPs that adsorbed ATZ herbicide, rather than TWPs themselves, had a negative effect on aquatic plant growth (e.g., C. vulgaris). The leaching solution of oxidized TWPs (after HPT and UPT) showed a more significant inhibition effect on the zebrafish survival compared with that of untreated TWPs, which was possibly caused by the generation of oxidation byproducts such as N-(1,3-dimethylbutyl)-N′-phenyl-p-phenylenediamine-quinone.

Dual strategies to construct electrospun NiCo2O4/boron-doped LaCoO3 heterojunction catalysts to activate peroxymonosulfate for organic pollutant degradation

The spinel and perovskite-based heterogeneous catalysts play indispensable roles in the sulfate radical-based advanced oxidation process (SR-AOP). In this study, novel electrospun boron-doped NiCo2O4/LaCo1−xBxO3 (NCO/Bx, 0 ≤ x < 1) catalysts were constructed using defect and interface engineering to accelerate peroxymonosulfate (PMS) activation. Due to the synergistic impacts of oxygen vacancies (OVs) and heterointerfaces, NCO/B0.2 demonstrated improved catalytic performance toward the degradation of Orange II (Org II). The NCO/B0.2 catalyst showed a high degree of pH tolerance, with a range of 5.0–11.0, while maintaining a removal rate of 94.2% even after five cycles. The degradation pathway exhibited a preference for non-radical mechanisms, with singlet oxygen (1O2) being the dominant reactive oxygen species. The synthesis method for NCO/Bx exhibits the potential to facilitate rational design and large-scale production of exceptionally effective heterostructured catalysts.

A Perspective on Removal of Cyanotoxins from Water Through Advanced Oxidation Processes.

This perspective discusses the challenges associated with the removal of cyanotoxins from raw water sources for drinking water treatment and the emergence of sulfate radical-based advanced oxidation processes (SR-AOPs) as an effective treatment technique. The advantage of SR-AOPs is that they can be activated using a variety of methods, including heat, UV radiation, and transition metal catalysts, allowing for greater flexibility in treatment design and optimization. In addition, the byproducts of SR-AOPs are less harmful than those generated by •OH-AOPs, which reduces the risk of secondary contamination. SR-AOPs generate sulfate radicals (SO4 •-) that are highly selective to certain organic contaminants and have lower reactivity to background water constituents, resulting in higher efficiency and selectivity of the process. The presence of natural organic matter and transition metals in the natural water body increases the degradation efficiency of SR-AOPs for the cyanotoxins. The bromate formation is also suppressed when the water contaminated with cyanotoxins is treated with SR-AOPs.

A sustainable solution for organic pollutant degradation: Novel polyethersulfone/carbon cloth/FeOCl composite membranes with electric field-assisted persulfate activation

Sulfate radical-based advanced oxidation processes (SR-AOP) and ultrafiltration (UF) membranes have demonstrated effectiveness in treating wastewater. This investigation illuminated a pioneering two-stage procedure for fabricating polyethersulfone/carbon cloth/FeOCl (PES/CC/FeOCl) composite catalytic membranes, exhibiting proficiency in persulfate activation. Evidenced by their distinctively high degradation rates and superior stability, these innovative composite membranes efficaciously obviate tetracycline (TC), showcasing a striking TC degradation rate, with an unparalleled removal ratio peaking at 93% under applied electrical fields. The process underlying persulfate activation and TC degradation was meticulously explored through electron paramagnetic resonance (EPR) and quenching trials. These evaluations unveil that hydroxyl radicals (•OH) and sulfate radicals (SO4•−) primarily drive the eradication of diminutive organic molecules. Subsequent studies emphasized the noteworthy rejection ratio of the PES/CC/FeOCl composite membranes (90%) for sodium alginate (SA), further revealing their exceptional on-line cleansing efficiency in an electrofiltration-associated in-situ oxidation system. In essence, this study proposed a novel approach for the synthesis of composite membranes adept at the catalytic degradation of organic pollutants. This paradigm-shifting research imparted a unique lens to perceive the integration of membrane separation technology, enriching the domain of advanced wastewater treatment strategies.

Assessment of sulfate radical-based advanced oxidation and electrocoagulation processes for spent caustic treatment from olefin unit

Assessment of sulfate radical-based advanced oxidation and electrocoagulation processes for spent caustic treatment from olefin unit

Synthesis of metal-free nitrogen-doped mesoporous carbon nanosheets with reference to molecular self-assembly for efficient peroxymonosulfate activation

The application of metal-free carbon materials in Sulfate radical-based advanced oxidation processes (SR-AOPs) has attracted great attention. In SR-AOPs, porosity and active sites are the keys for nitrogen-doped carbon materials to exhibit high catalytic activity. In this paper, melamine and gallic acid were selected as raw materials, preparing metal-free nitrogen-doped carbon materials by using the molecular self-assembly synthesis method. The catalysts with different structural morphology and surface chemistry were obtained by controlling the pyrolysis temperature. It proposed the formation mechanism of nitrogen-doped mesoporous carbon nanosheets (NMC). The pyrolysis temperature was critical for the regulation of surface properties as well as the structure of carbon materials. It was found that NMC-800 exhibited fluffy and porous microstructure, and various active sites on the surface of the catalyst, including graphite N, pyridine N and CO. In the NMC-800/PMS system, the SMX degradation efficiency and corresponding rate constant could achieve 90.3 % and 0.1705 min−1, respectively. Besides, the degradation pathways and intermediate products of SMX were discussed by the analysis of quenching experiments, electron spin resonance (ESR) and liquid chromatography-mass spectrometry (LC-MS).

PH adjustable MgAl@LDH-coated MOFs-derived Co2.25Mn0.75O4 for SMX degradation in PMS activated system

Sulfate radical-based advanced oxidation processes (SR-AOPs) is considered as one of the most promising technologies for antibiotic pollution. In this study, a core-shell catalyst of cobalt-manganese oxide derived from CoMn-MOFs coating by MgAl-LDH (Co/Mn@LDH) was synthesized for peroxymonosulfate (PMS) activation to degrade sulfamethoxazole (SMX). Degradation efficiency of nearly 100% and a mineralization efficiency of 68.3% for SMX were achieved in Co/Mn@LDH/PMS system. Mn species and out shell MgAl-LDH greatly suppressed the cobalt ions leaching, which only 23 μg/L Co ions were detected by ICP after the reaction. SO4·- was identified as dominant reactive species in the system. Furthermore, the possible reactive sites of SMX were predicted by the density functional theory (DFT) calculations. And the intermediates of SMX were detected by LC-MS and the degradation pathway was proposed based on the results above. The ECOSAR results suggested the intermediates of SMX showed a relatively low toxicity compared to SMX, indicating huge potential of utilization of Co/Mn@LDH in SR-AOPs system.

Cobalt cross-linked ordered mesoporous carbon as peroxymonosulfate activator for sulfamethoxazole degradation

Ordered mesoporous carbons (OMCs) functionalized with catalytically-active metals have many potential applications in sulfate radical-based advanced oxidation processes for degrading antibiotics. Cobalt cross-linked ordered mesoporous carbon materials (OMC-Co-Tx) were synthesized through evaporation-induced self-assembly, calcinated at (600 to 800) oC. The OMC-Co-Tx materials were then employed as peroxymonosulfate (PMS) activators for removal of sulfamethoxazole (SMX) from aqueous solutions. OMC-Co-T800 prepared by calcination at 800 °C had a large specific surface area (449 m2/g), uniform pore structure (∼4.5 nm) and showed the best performance for activation of PMS. With a dosage of 0.1 g/L OMC-Co-T800 and 0.4 g/L PMS, the functionalized OMC material allowed SMX (10 mg/L) removal of up to 99% in 30 min. The increase of calcination temperature promoted the reduction of cobalt in OMC materials and increased the defects in their structure, resulting in better catalyst behavior. Quenching experiments and electron paramagnetic resonance analyses showed that reactive species of sulfamethoxazole degradation involved in the OMC-T800/PMS system were SO4•−, OH, O2•− and 1O2. HPLC-MS analyses of degradation intermediates formed in the OMC-Co-T800/PMS system allowed elucidation of four transformation pathways for SMX degradation.

Attenuation effects of ZVI/PDS pretreatment on propagation of antibiotic resistance genes in bioreactors: Driven by antibiotic residues and sulfate assimilation

Sulfate radical-based advanced oxidation processes (AOPs) combined biological system was a promising technology for treating antibiotic wastewater. However, how pretreatment influence antibiotic resistance genes (ARGs) propagation remains largely elusive, especially the produced by-products (antibiotic residues and sulfate) are often ignored. Herein, we investigated the effects of zero valent iron/persulfate pretreatment on ARGs in bioreactors treating sulfadiazine wastewater. Results showed absolute and relative abundance of ARGs reduced by 59.8%− 81.9% and 9.1%− 52.9% after pretreatments. The effect of 90-min pretreatment was better than that of the 30-min. The ARGs reduction was due to decreased antibiotic residues and stimulated sulfate assimilation. Reduced antibiotic residues was a major factor in ARGs attenuation, which could suppress oxidative stress, inhibit mobile genetic elements emergence and resistant strains proliferation. The presence of sulfate in influent supplemented microbial sulfur sources and facilitated the in-situ synthesis of antioxidant cysteine through sulfate assimilation, which drove ARGs attenuation by alleviating oxidative stress. This is the first detailed analysis about the regulatory mechanism of how sulfate radical-based AOPs mediate in ARGs attenuation, which is expected to provide theoretical basis for solving concerns about by-products and developing practical methods to hinder ARGs propagation.

MnFe2O4 nanoparticles coated on one-dimensional carbon nanowires derived from Nitrilotriacetic acid as efficient catalysts to activate peroxymonosulfate for moxifloxacin degradation

Sulfate radical-based advanced oxidation processes (AOPs) are highly reliable for the elimination of recalcitrant contaminants by increasing degradability and reducing toxicity. Here, MnFe2O4 nanowires (MnFe2O4 NWs), composed of abundant MnFe2O4 nanoparticles immobilized on one-dimensional carbon nanowires derived from annealed MnFe-Nitrilotriacetic acid (MnFe-NTA) precursor was successfully synthesized. The MnFe2O4 NWs, which could provide more active sites, were then utilized to activate peroxymonosulfate (PMS) for oxidizing the target pollutant Moxifloxacin (MOX) in an aqueous solution. The MnFe2O4 NWs/PMS system acquired 91.9% removal of MOX and achieved 55.1% chemical oxygen demand (COD) degradation efficiency in 30 min. The results exhibited that the increased catalyst doses and PMS concentration lead to ascending MOX removal rate, which decreased with the participation of co-existing ions. Besides, there is a close relationship between original pH and MOX degradation efficiency. It was found that SO4⋅–, ⋅OH, 1O2, and O2⋅– were involved in the MOX degradation by quenching experiments and electron paramagnetic resonance (EPR) detection. More importantly, the stable magnetism of MnFe2O4 NWs contributed to its convenient recycling. Finally, a reliable mechanism for activating PMS was proposed based on the aforementioned results and previous researches, which could exhibit a novel horizon in effluent treatment.

Performance and mechanism of sulfite mediated oxidation of organic contaminants using iron(III) titanium oxide as catalyst

As sulfite has been employed currently in the catalytic degradation of various pollutants, the construction of more suitable and cheaper catalytic systems is required. Herein, a heterogeneous system for S(IV) activation by iron(III) titanium oxide (Fe2TiO5) was proposed to proceed the removal of acid orange 7 (AO7) and seven typical pharmaceutical and personal care products (PPCPs). Typically, the AO7 (10 mg L−1) can be degraded up to 67% within 60 min ([Fe2TiO5] = 0.8 g L−1, [S(IV)] = 2.0 mM, pH = 6.0). The effects of initial AO7 concentration, pH, Fe2TiO5 dosage, S(IV) concentration, and co-existing anions (HCO3− and H2PO4−) were examined to explore the application conditions and resistance of Fe2TiO5 −S(IV) system. Moreover, the stability of Fe2TiO5 −S(IV) system was tested by sequential runs, while XRD was also performed for the robustness evaluation of catalyst. The scavenging experiment showed that the active species in the system mainly include SO5•−, HO•, and SO4•−, while SO4•− being the dominant one. Through the competitive experiments of EDTA, the density functional theory (DFT) computation and the XPS analysis, a sensible mechanism was proposed that the electron transfer within Fe(III)−SO32− complex and the Fe(III)−Fe(II)−Fe(III) redox process were crucial for the sulfite activation. Meanwhile, a quantitative structural-activity relationship (QSAR) model for pseudo-first-order rate constants (kobs) was established with a high significance (R2 = 0.991, p = 0.006) by using four descriptors. This work provides an innovative strategy of sulfate radical-based advanced oxidation processes (SR−AOPs) for organic contaminants degradation using metal oxide catalysts.