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APPLIED CATALYSIS B-ENVIRONMENTAL · 2022 · IF 24.319

β particles induced directional inward migration of oxygen vacancies: Surface oxygen vacancies and interface oxygen vacancies synergistically activate PMS

Xinyu Hu,Juntao Wang,Jing Wang,Yao Deng,Huidi Zhang,Tao Xu,Wenlei Wang

In this work, a high-energy β electron beam was applied to promote the generation and directional inward migration of surface oxygen defects. The valence band potential changed to a high potential due to the transfer of surface oxygen vacancies on BiVO 4 /Bi 2 O 3−x . Interface oxygen vacancies have significant advantages in inducing the formation of oxygen vacancy levels and reducing the band gap energy. Surface oxygen vacancy and vacancy levels can prevent the recombination of photogenerated carriers. The electrons enriched in the surface oxygen vacancies can remarkably activate PMS with O−O bonds to degrade ciprofloxacin (CIP). The degradation kinetic constant and CIP mineralization rate of BiVO 4 /Bi 2 O 3−x -450/PMS were 2.09 and 1.51 times higher than those of BiVO 4 /Bi 2 O 3−x /PMS, respectively. BiVO 4 /Bi 2 O 3−x -450 with a lower relative content of surface oxygen vacancies (24.70%) exhibited a stronger activation ability. Obviously, the change of band structure caused by interface oxygen vacancies is the reason for increasing photoactivation efficiency of PMS.

研究领域: 环境科学 · 材料科学
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2023 · IF 22.1

High-efficiency V-Mediated Bi2MoO6 photocatalyst for PMS activation: Modulation of energy band structure and enhancement of surface reaction

Jun Yang,Taiping Xie,Yuhan Mei,Junyu Chen,Hao Sun,Shan Feng,Yu Zhang,Ying Zhao,Jiankang Wang,Xiaoqing Li,Jiahong He,Houyang Chen

High photocorrosion and poor reaction efficiency of Bi 2 MoO 6 greatly hampered its wide application in wastewater treatment . Herein, V doped Bi 2 MoO 6 was prepared by hydrothermal-subsequent annealing strategy for the refractory sulfapyridine abatement through visible-light-driven photocatalytic activation of peroxymonosulfate (PMS). The degradation results revealed V-doped Bi 2 MoO 6 could achieved 100% sulfapyridine removal after 20 min over Bi 2 MoO 6 /PMS/Vis system, much higher than Bi 2 MoO 6 /PMS/Vis system. Experimental and theoretical calculations indicated that the V doping not only changed the energy band structure of Bi 2 MoO 6 and promoted the separation of photogenerated charges as well as improved the adsorption energy of peroxymonosulfate (PMS), H 2 O and dissolved oxygen on the catalyst surface, but also provided additional PMS activation pathway through V 5+ /V 4+ redox cycles, finally contributed to enhanced sulfapyridine degradation performance in Bi 2 MoO 6 /PMS/Vis system. Our work provides insight into designing highly efficient photocatalyst as a promising PMS activator for environmental application.

研究领域: 环境科学 · 材料科学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2023 · IF 8.6

Multi-phase CdS loaded on biochar for photocatalytic activation of peroxymonosulfate for thiamethoxam degradation: π-conjugation improves PMS adsorption

Honghui Jiang,Zhenxin Hu,Yuanhao Ouyang,Xiaodong Ji,Xi Hu,Tingting Li,Ke Ouyang,Ping Wang,Hui Wang,Xinjiang Hu

Mounting evidence highlights the negative impacts of thiamethoxam (THM) on non-target organisms and ecosystem. Herein, multi-phase cadmium sulfide loaded on biochar (CdS@BC) was used to photocatalytic activate peroxymonosulfate (PMS) to remove THM. The obtained CdS@BC significantly improved the photocatalytic performance of PMS on THM degradation with a superior rate constant of 0.165 min −1 , 60 times more than that of BC. In addition, the catalyst displayed excellent stability and reusability. The mechanism of free radical formation by adsorption activation of PMS adsorbed on CdS@BC was characterized using active species detection and Density functional theory (DFT) calculations. According to the DFT study, the phase junction and π-conjugated structure contribute to the stable migration of π-electrons, thus effectively activating the PMS to produce active substances for the degradation of THM. The findings provide a theoretical basis for the design and synthesis of effective catalysts for AOPs to remove emerging organic contaminants from wastewater.

CAS / MDL: 153719-23-4
研究领域: 环境科学 · 化学工程
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS · 2023 · IF 5.2

Recovery of graphite from anode in spent lithium-ion battery as an efficient peroxymonosulfate (PMS) activator: Performance and mechanism

Jiali Yan,Xi Wang,Jinli Zhai,Chao Gong,Wenjie Zhu,Daoli Yang,Yongming Luo,Xiaoya Gao

The recovery of anode graphite as catalysts is rarely reported in the published works. In this study, a simple method was used to recover anode graphite from spent lithium-ion battery (LIB) as catalyst to activate peroxymonosulfate (PMS) for the degradation of carbamazepine (CBZ). Graphite catalyst exhibited excellent catalytic performance with the mineralization efficiency of CBZ of 81% in the graphite/PMS system. This system was highly effective in a wide pH range of 3.0–11.0. Inorganic ions (Cl - , HCO 3 - , K + , etc) and natural organic matter (HA) exhibited some influences on the degradation of CBZ. The electron-donating groups of C O and C-OH were identified in the recovered graphite, which transferred electrons to activate PMS generating sulfate radical (SO 4 - •), hydroxyl radical (HO•), and singlet oxygen ( 1 O 2 ). Under the attack of multiple reactive species, five intermediates were detected in the degradation of CBZ and disappeared quickly after 1 min. Particularly, the graphite/PMS system was effective for CBZ degradation in real water matrix, showing a higher degradation efficiency of 93% in tap water (TW). This study provides a green and efficient approach for recovering graphite catalyst from spent LIB as PMS catalyst to degrade organic pollutants in wastewater.

研究领域: 环境科学 · 催化材料
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APPLIED SURFACE SCIENCE · 2023 · IF 6.7

Cobalt leaching inhibition: Transforming coordination polymers into spherical Co3O4@NC catalysts for accelerated tetracycline degradation via enhanced PMS activation

Rongyao Ma,Guolang Zhou,Mingrui Gu,Xin Tang,Wenhao Ding,Yu Guan,Yexin Jiang,Jingzhou Yin,Lili Zhang,Edison Huixiang Ang

In this study, we synthesized Co-based coordination polymer-derived nitrogen-doped carbon-coated Co 3 O 4 spheres (Co 3 O 4 @NC) and yolk-shell Co 3 O 4 spheres (Co 3 O 4 -YS) under various atmospheric conditions to explore their efficacy in activating peroxymonosulfate (PMS) for tetracycline (TC) degradation. The Co 3 O 4 @NC, featuring a significantly higher specific surface area (268.4 m 2 /g), exhibited remarkable performance by achieving 90% TC removal in 5 minutes using 0.2 g/L PMS and 0.1 g/L of Co 3 O 4 @NC. This reaction rate was 9.2 times higher than that observed with Co 3 O 4 -YS. Furthermore, the Co 3 O 4 @NC/PMS system demonstrated exceptional stability across a wide pH range, in complex water compositions, and the presence of common coexisting ions. The unique coated structures effectively minimized the leaching of Co ions (below 0.447 mg/L). Additionally, the strong magnetism of Co 3 O 4 @NC allows for easy separation under a magnetic field. Mechanistic investigations identified 1 O 2 , ∙OH, O 2 ∙ - , and SO 4 ∙ - as the principal reactive species. The study also explored potential degradation pathways and toxicity.

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CHEMICAL ENGINEERING JOURNAL · 2024 · IF 13.3

Enhanced electron transfer using NiCo2O4@C hollow nanocages with an electron-shuttle effect for efficient tetracycline degradation

Yuwen Chen,Ke Zhu,Wenlei Qin,Zhiwei Jiang,Zhuofeng Hu,Mika Sillanpää,Kai Yan

Spinel oxides are recognized as promising Fenton-like catalysts for the degradation of antibiotics. However, the catalytic performance is restrained by the poor electron transfer rate (ETR). Herein, hollow NiCo 2 O 4 @C nanocages are rationally designed and prepared to accelerate ETR in peroxymonosulfate (PMS) activation for tetracycline (TC) degradation. Enhanced ETR of the NiCo 2 O 4 @C/PMS system is due to three aspects: (1) The hollow nanocage facilitates the diffusion and adsorption of TC, improving the ion transfer at a macroscopic level; (2) Electron reconfiguration in octahedral sites of NiCo 2 O 4 increases the ratio of Co 2+ , resulting in highly efficient PMS activation; (3) In-situ generated carbon acts as “electron shuttles”, improving the electrical conductivity of catalysts at a microscopic level. As a result, the NiCo 2 O 4 @C demonstrates rapid ETR, leading to a high-efficiency activation of PMS. The NiCo 2 O 4 @C/PMS system exhibits exceptional TC degradation efficiency and reusability. Non-radical pathway, including 1 O 2 and direct electron transfer, dominates the system. This work offers a feasible strategy for enhancing electron transfer in the Fenton-like system.

CAS / MDL: 10026-22-9 98-00-0
研究领域: 环境科学 · 材料科学 · 催化 · 水处理
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SEPARATION AND PURIFICATION TECHNOLOGY · 2024 · IF 8.1

Fe0-modified sulfur-rich vacancy CoS2 enhanced persulfate photoactivation: Achieving high surface adsorption and rapid degradation of antibiotics

Xiao Feng,Hao Chen,Siyuan Guo,Xiaoyu Wang,Tengfeng Xie,Dejun Wang,Yanhong Lin

Efficient photocatalysts are key to achieving efficient photoactivation of AOPs based on PMS. In this work, a sulfur-rich vacancy magnetically separable Fe 0 /CoS 2 -S v photocatalyst with high surface adsorption capacity and rapid PMS activation capacity was designed for the efficient degradation of typical antibiotics. A tetracycline removal rate of 92.2 % and a high TOC mineralization rate were achieved within 4 min in the PMS/Vis system. The excellent catalytic performance was attributed to the synergistic effect of Fe, Co, and S on PMS activation and the generation of sulfur-oxygen vacancies by the composites. These vacancies greatly enhanced the catalytic performance of the PMS system, where the generated singlet oxygen ( 1 O 2 ) was identified as the main active substance in the degradation process. In addition, the SO 4 2- based photocatalytic-assisted advanced oxidation processes (SR-AOPs) for the degradation of organic pollutants were thoroughly investigated. XPS comparisons before and after the catalyst reaction revealed that the reducing nano-Fe 0 and metastable S 2 2- promoted the cycling between Co 3+ and Co 2+ , thus accelerating the rapid activation of PMS. This work provides a new perspective for the further development of efficient and rapid PMS photo-activators for environmental remediation in water bodies.

CAS / MDL: 106-51-4 299-11-6
研究领域: 环境科学 · 化学工程 · 材料科学 · 水处理
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CHEMOSPHERE · 2022 · IF 8.943

Polyaniline@g-C3N4 derived N-rich porous carbon for selective degradation of phenolic pollutants via peroxymonosulfate activation: An electron transfer mechanism

Lidong Kou,Qingfeng Fan,Yuhong Yang,Xianying Duan,Kai Jiang,Jing Wang

N -doped carbons have attracted extensive attention as catalysts for peroxymonosulfate (PMS) activation towards environmental remediation. However, synthesis of N -rich carbocatalysts is challenging and PMS activation mechanism is still unclear. Herein, novel N -rich porous carbocatalysts ( C -P x CN-T) were synthesized by carbonization of polyaniline nanorods coated g-C 3 N 4 . C –P 50 CN-900 (polyaniline content 50%) calcined at 900 °C had high surface area (358 m 2 /g), product yield (27.1%) and N content (12.27 at%). It showed superior performance in activating PMS to degrade and mineralize various phenolic pollutants in a wide pH range (2–11) and with the co-existence of water constituents. A positive correlation was observed between phenol oxidation rates and contents of C O, C –C/C C and graphitic N, which served as active sites to facilitate adsorption of pollutants and PMS on C –P 50 CN-900 and subsequent electron-transfer from pollutants to PMS. Overall, this study provides new insights into rational design of N -doped carbocatalysts and elucidation of electron transfer pathway in PMS activation.

研究领域: 环境科学 · 材料科学 · 化学工程 · 催化
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CHEMICAL PHYSICS LETTERS · 2022 · IF 2.719

Construction of 3D-sized Mn (II)-doped MoS2@activated alumina beads as PMS activator for tetracycline degradation under light irradiation

Huan Zhang,Chang Liu,Yu Wang,Feifei Jia,Shaoxian Song

In this work, Mn (II) was doped into MoS 2 structure and then anchored on activated alumina beads to construct 3D-sized composites (Mn-MoS 2 @AABs). This component material was used as PMS activator for tetracycline (TC) degradation under light irradiation. According to experiment results, Mn-MoS 2 @AABs exhibited well degradation performance to TC, which ascribed to excellent photo-response property of Mn-MoS 2 and activation of Mn. Importantly, the 3D-sized structure made it facilely be recycled from solution, which catered to the demand for the practical application. Therefore, the novel strategy of designing Mn-MoS 2 @AABs had great significance for environmental restoration.

研究领域: 环境科学 · 材料科学
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Water · 2024 ·Vol. 17 ·期 1 ·24 · IF 3

Performance and Mechanism of In Situ Prepared NF@CoMnNi-LDH Composites to Activate PMS for Degradation of Enrofloxacin in Water

Yiqiong Yang,Yubin Zhang,Xuyang Gao,Zitong Yang,Haozhou Wang,Xiaodong Zhang

To overcome the disadvantage of difficult recovery of powder catalysts and improve catalyst utilization, the selection of foam metal substrates as supports can reduce the difficulty of material recovery and effectively inhibit the leaching of metal ions. Herein, CoMnNi-layered double hydroxide (LDH) derived from Co-Mn ZIF was immobilized onto nickel foam (NF) through in situ synthesis. The results of XRD and SEM analyses of the samples indicated that the LDH was successfully grown on the nickel foam matrix, and the material could maintain its original morphology to the maximum extent after loading. By comparing the XPS of the material before and after the reaction, it was confirmed that the surface hydroxyl group and C=O of the material were involved in the activation of peroxymonosulfate (PMS). The results of the quenching reaction showed that SO4•−and1O2are the main active substances in the oxidation of enrofloxacin (ENR). When the dosage of NF@CoMnNi-LDH was 0.4 g/L, the pH of the solution was 6.82, and when the dosage of PMS was 2.0 mM, the degradation rate of ENR reached 82.6% within 30 min. This research offers novel insights into the degradation of antibiotics from water using a monolithic catalyst supported by metal foam.

研究领域: 环境科学 · 材料科学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2024 · IF 8.1

Feasibility of phenolic contaminant removal from high-saline wastewater by chloride-mediated activation of peroxymonosulfate (PMS) and peracetic acid (PAA)

Zhao Song,Yu Zhang,Peiru He,Xuesong Liu,Nanqi Ren,Yidi Chen

Phenolic pollutants are highly toxic and can affect the growth and reproduction of aquatic organisms, as well as contaminate drinking water resources, posing a significant threat to both ecological and human health. However, conventional biological treatment processes are constrained in treating high salinity organic wastewaters due to the potentially lethal effects of high concentrations of dissolved salts on microorganisms. While advanced oxidation processes have shown promise in removing phenolic contaminants from high-saline wastewater, their widespread application is always limited by the high costs associated with energy and chemical usage. In this study, we explored the potential application of directly introducing peroxymonosulfate (PMS) and peracetic acid (PAA) to high-salinity water for the removal of nine phenolic contaminants. By establishing a correlation between the degradation rate constants in the PMS/Cl – ( k PMS ) and PAA/Cl – ( k PAA ) systems and various molecule descriptors, two multiple linear regression models were developed to predict the degradation rate constants under investigation. Additionally, we selected bisphenol A (BPA) as the target contaminant and investigated the impact of common ions found in natural water, such as HCO 3 – , NO 3 – , and humic acid, on the removal of BPA using two systems. Finally, we conducted experiments using tap water and sewage water to demonstrate the practical application and performance of the two systems. These experiments aimed to provide valuable insights into the influence of background chloride on PMS and PAA activation, as well as the potential of direct PMS/PAA introduction for eliminating phenolic micropollutants from high-saline wastewaters.

研究领域: 环境科学 · 化学工程
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Journal of Environmental Chemical Engineering · 2026 ·Vol. 14 ·期 5 ·124163 · IF 7.5

Dual non-radical pathways triggered by Mn3O4@g-C3N4 with synergistic interfacial effect toward PMS activation for bisphenol A degradation

Zhiyun Jiang,Mingjing Ge,Xiaoting Jie,Lixiao Ni,Shiyin Li

Efficient and durable activation of peroxymonosulfate (PMS) for the degradation of persistent organic pollutants remains challenging owing to the instability of active catalytic sites. Here, a Mn 3 O 4 @g-C 3 N 4 heterostructured catalyst (MCN-2) is constructed to enable efficient PMS activation and enhance the generation of non-radicals for rapid bisphenol A (BPA) degradation. MCN-2 preferentially adsorbs the peroxy oxygen atom of PMS, facilitating O-O and O-H bond cleavage to form the high-valent Mn-oxo species (Mn(IV)=O), which further reacts with PMS to yield singlet oxygen ( 1 O 2 ). The resulting 1 O 2 (60.5%) and Mn(IV)=O species (39.5%) synergistically drive rapid non-radical oxidation. Here, Mn 3 O 4 provides catalytic active sites, whereas g-C 3 N 4 enhances adsorption, shortens the mass-transfer distance between BPA and reactive oxygen species (ROS), and functions as an electron reservoir to sustain Mn redox cycling. Consequently, the synergistic 1 O 2 and Mn(IV)=O species system delivers a k-value of 0.258 min −1 for BPA degradation, which is 258 times and 6.45 times higher than that of the g-C 3 N 4 /PMS and Mn 3 O 4 /PMS systems, respectively. Moreover, MCN-2-based catalytic membranes enable stable BPA removal under continuous-flow conditions, and toxicity assessments demonstrate significantly reduced acute toxicity and mutagenicity of the transformation products, highlighting the potential for scalable and environmentally benign water treatment.

CAS / MDL: 75-05-8
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