MINERALS ENGINEERING
·
2025
·
IF 5
Xiaoyu Jiang,Sikai Zhao,Jie Wang,Haiyi Lv,Weizhen Bai,Wenbao Liu,Qiang Zhao,Yanbai Shen
Tetracycline (TC) persistence in aquatic systems poses significant ecological and human health risks, due to its toxicity and resistance to conventional biodegradation. In this study, sulfur and nitrogen modification strategies were employed to enhance the catalytic performance of spinel ferrite MnFe 2 O 4 for TC degradation via H 2 O 2 and peroxymonosulfate (PMS) activation. The catalysts were characterized using SEM, XRD, VSM, CV, and ICP-OES to elucidate the effects of heteroatom modification on morphology, crystal structure, magnetic separability, and metal leaching behavior. S modification markedly enhanced both H 2 O 2 and PMS activation capabilities. The optimized S/MnFe 2 O 4 -5/H 2 O 2 system removed 82 % TC (50 mg/L) within 20 min, an eightfold increase in the reaction rate compared to the unmodified MnFe 2 O 4 /H 2 O 2 . This system maintained high efficiency across a broad pH range (3–11). In contrast, nitrogen modification selectively improved PMS activation, with the optimal N/MnFe 2 O 4 -3/PMS system degrading 74 % TC in 30 min, twice the degradation rate of MnFe 2 O 4 /PMS, and exhibiting minimal metal leaching with excellent recyclability. Scavenger studies confirmed that ·OH constitutes the dominant reactive oxygen species (ROS) in S/MnFe 2 O 4 -5/H 2 O 2 systems, while both ·OH and ·SO 4 - contribute significantly in N/MnFe 2 O 4 -3/PMS systems. Sulfur species act as electron mediators, facilitating the Fe/Mn redox cycle and enhancing ROS generation, whereas zero valence iron (Fe 0 ) formed during nitrogen modification serves as an efficient electron donor to activate PMS. Degradation pathway analysis and toxicity predictions confirmed a substantial reduction of TC environmental hazards. This work provides fundamental insights into the structure–activity relationships of heteroatom-modified MnFe 2 O 4 catalysts, and establishes practical design principles for robust advanced oxidation process catalysts in antibiotic remediation.
✓ 已验证
产品关联
DOI
高影响因子
Journal of Materials Chemistry A
·
2026
·
IF 9.5
Jiani Qin,Minna Duan,Jianping Zhang,Wen Chen,Tingjiang Yan,Chuanyi Wang,Bao Pan
The persistent presence of tetracycline (TC) in aquatic environments demands advanced oxidation processes capable of efficiently degrading this micropollutant. Although peroxymonosulfate (PMS)-based catalysis shows promise in this regard, its practical efficiency is limited by sluggish activation kinetics and rapid charge recombination, necessitating the development of high-performance catalysts. Herein, we present a strategically engineered cobalt-doped tubular carbon nitride (Co-TCN) that integrates morphological control with atomic-level doping to achieve enhanced photocatalytic PMS activation. The unique tubular architecture of TCN improves light harvesting and facilitates mass transfer, while atomically dispersed cobalt species, confirmed by XAS and XPS, act as efficient electron traps and active sites for PMS activation. This synergistic design yields a catalyst with an increased specific surface area, significantly suppressed charge recombination, and accelerated electron transfer. Under visible light, the optimized 1.1%Co-TCN/PMS system achieved a TC degradation rate constant of 15.87 × 10−2 (mg L−1)−1·min−1, which was 15.6-fold higher than that of PMS alone and demonstrates remarkable performance across various antibiotics. Mechanistic investigations reveal a catalytic cycle involving Co2+/Co3+ redox pairs, generating both radical species (SO4˙−, ˙OH, ˙O2−) and non-radical species (1O2). Furthermore, toxicity assessment confirmed the effective detoxification of TC during the degradation process. This work establishes a novel strategy for designing cost-effective, non-precious-metal–based photocatalysts through concurrent structural and electronic modulation, offering a promising approach for sustainable water treatment.
✓ 已验证
产品关联
DOI
高影响因子
Journal of Water Process Engineering
·
2026
·
IF 6.6
Guangxu Zhang,Jin Wang,Mengmeng Dou,Wubin Wang,Chao Han,Yadong Hu,Xinyu Li,Kaibo Wang,Yaxuan Liu,Yuting Ma,Xin Zhang
MnTiO 3 catalytic ceramic membrane (MTPCM) is prepared by impregnation- drawing- sintering method. • 1 O 2 has the highest contribution to BPA removal in MTPCM activation PMS system. • The formation pathway of 1 O 2 is explored by density functional theory. • Reveal the combination of active site density and spatial limitation to catalysis. While ceramic ultrafiltration membranes are highly valued in wastewater treatment for their exceptional durability and robust resistance to harsh conditions, their application is often hindered by an inability to efficiently degrade emerging pollutants. To address this, we fabricated a novel MnTiO 3 -modified catalytic ceramic membrane (MTPCM) via a facile solid-phase impregnation-drawing-sintering process. The optimized MTPCM 3 , tightened 30 nm pore size, demonstrates a remarkable capacity to generate high concentrations of reactive oxygen species (ROS) while intensifying pollutant-ROS collisions. Evaluated using bisphenol A (BPA) as a model pollutant and peroxymonosulfate (PMS) as the oxidant, the integrated system achieved an outstanding 95.2% degradation efficiency within 30 min, maintaining robust stability across eight operational cycles. Furthermore, intermediate and toxicity assessments delineated the degradation pathways and confirmed detoxification. Mechanistically, radical quenching experiments coupled with density functional theory (DFT) calculations identified 1 O 2 as the dominant ROS, systematically elucidating its generation pathway. Crucially, finite element simulations confirmed that this superior catalytic performance stems from the synergistic interplay between high-density MnTiO 3 active sites and a pronounced nanoscale confinement effect. Overall, MTPCM offers a simple, scalable, and highly reusable paradigm for advanced wastewater treatment, innovatively structuralizing pores to maximize ROS yield and accelerate interfacial reactions for highly efficient pollutant decontamination. Download: Download high-res image (264KB) Download: Download full-size image
✓ 已验证
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Shizong Wang,Jianlong Wang,Bo Lai
This study investigated the role of support-driven coordination environments in regulating peroxymonosulfate (PMS) activation by single-atom cobalt catalysts. Atomically dispersed cobalt was anchored on graphene oxide (Co/GO) and silica (Co/SiO 2 ) to compare their catalytic pathways and stability. Both catalysts enabled efficient degradation of sulfamethoxazole (SMX), achieving mineralization efficiencies of 36.4 % for Co/GO and 42.7 % for Co/SiO 2 after 60 min. Co/SiO 2 also showed superior structural stability and reduced cobalt leaching during reaction. Mechanistic studies revealed that Co/GO favored the direct formation of Co(IV)=O species, whereas Co/SiO 2 promoted surface-bound radicals, which is attributed to its higher cobalt coordination number and stronger metal-support interactions. Furthermore, both catalysts were incorporated into polyvinylidene fluoride membranes, which maintained high SMX removal efficiency during 7 days of continuous operation with real municipal wastewater. These findings underscore the crucial role of support effects in tailoring PMS activation and offer insights for designing stable single-atom catalysts for water treatment.
研究领域:
环境科学
·
催化
·
材料科学
·
化学工程
·
水处理技术
✓ 已验证
产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Ziyang Chu,Haibo Liu,Tianhu Chen,Hanlin Wang,Fuwei Sun,Xuehua Zou,Dong Chen,Dionysios D. Dionysiou
This work investigated the performance and mechanisms of calcite activating peroxymonosulfate (PMS) for the simultaneous elimination of lead (Pb(II)), cadmium (Cd(II)), and norfloxacin (NOR). At an initial pH = 7, 1.0 g/L calcite, and 0.5 mM PMS, the removal of Pb(II), Cd(II), and NOR was 97.5%, 96.0%, and 98.1%, respectively. The results of EPR, quenching, and chemical probe quantification experiments revealed that singlet oxygen ( 1 O 2 ) derived from calcite activating PMS dominated NOR degradation. Meanwhile, surface complexation and carbonate precipitation were identified as the main mechanisms in the removal of Pb(II) and Cd(II) by ATR-FTIR and different ionic strength experiments, respectively. Kinetic analysis and XPS results indicated that the solid phase Pb(IV) generated through surface complexed Pb(II) oxidized by PMS facilitated the NOR degradation. The NOR degradation pathway along with biological toxicity assessment was also presented through HPLC-MS and ECOSAR software. This study provides the prospects of using natural carbonate minerals to activate PMS for treating the combined contamination of antibiotics and heavy metal ions, and also provides a new understanding of the removal of organic substances in the presence of heavy metal ions.
研究领域:
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
CATALYSIS LETTERS
·
2024
·
IF 2.3
Feng Guo,Wang Xu,Wang Yajie,Sun Hongxin,Li Guohua
In PMS catalytic oxidation studies, we design and prepare a Mn 3 O 4 /CuO (CMO-2) composite catalyst using metal–organic frameworks (MOFs) as precursors. Compared with Mn 3 O 4 , its activated per-oxy-monosulfate activation catalyzed the degradation of pollutants with nearly six times higher activity efficiency. The experimental findings demonstrate that CMO-2 derived from metal–organic frameworks offer the advantages of wide adaptability to solution pH, along with improved versatility, stability, and recyclability. Further experiments involving radical scavenging, electrochemistry, and electron spin resonance (EPR) techniques confirm that the CMO-2 derived from MOF structures exhibit more significant interfacial engineering effects. This leads to an expansion of active interfaces, enhancing the accessibility and dispersion of active sites. Consequently, it significantly improves the efficiency of electron-transfer reactions and promotes a wide range of reactive oxygen species (ROSs), including SO 4 •− •OH and 1 O 2 . Graphical Abstract Based on the synergistic effect of copper-manganese bimetallic, the copper-manganese composite catalyst (CMO-2) prepared by doping 0.5 g of Cu-MOF showed the best catalytic activity in activating PMS, and the resulting ROS S could efficiently degrade organic pollutants.
研究领域:
环境科学
·
材料科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
RSC Advances
·
2016
·Vol. 6
·期 74
·70271-70276
·
IF 3.289
Ying Huang,Zhaohui Wang,Changling Fang,Wenqian Liu,Xiaoyi Lou,Jianshe Liu
Addition order of reagents in the Acid Orange 7 (AO7) degradation process was investigated by varying the concentration of Fe(II), the Fe(II)/peroxymonosulfate (PMS) molar ratio and stepwise addition of Fe(II) and PMS. The importance of addition order of reagents was confirmed and an order of Fe(II)–PMS to improve the oxidation efficiency was recommended.
研究领域:
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2022
·
IF 7.968
Xingyan Chen,Lifen Liu
In advanced oxidation processes (AOPs), organic pollutants are oxidized, but getting the most energy out of pollutant in reducing cost of AOPs is still a challenge. In this study, MoS 2 / Co 0.75 Mo 3 S 3.75 composite nano-catalyst with high density catalytic active sites was synthesized by homogeneous and dispersed doping of single Co atoms in MoS 2 by one-step hydrothermal method. The prepared catalyst was coated on stainless steel with silica sol for electrode application under visible light and activation of PMS (peroxymonosulfate) in Photocatalytic fuel cell (PFC) system. The synergy system at pH 6.5, visible light irradiation and 0.06 mM [PMS], was able to rapidly degrade RhB (50 mg·L −1 ) within 10 min and reach 98% degradation within 21 min (kinetic rate constant 0.261 min −1 ). The role of visible light contributes to RhB degradation more than oxidation by just PMS in PFC (Photocatalytic Fuel Cell). The dispersed Co sites have a significant effect of activating PMS, improving catalytic activity and enhancing reaction under closed circuit. The system has good stability, is also applicable to significant removal of tetracycline(TC, 76.35%) and bisphenol A (BPA, 53.76%). In MoS 2 / Co 0.75 Mo 3 S 3.75 -vis/PMS/PFC, species such as •OH, SO 4 •− , O 2 •− , h + and 1 O 2 jointly promote the degradation of RhB. This work provides a perspective for further study of two-dimensional metallic sulfide doped with transition metal ions and application of such vis/PMS/PFC system in removing other toxic pollutants .
研究领域:
环境科学
·
材料科学
·
化学工程
·
电化学
·
催化
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2023
·
IF 13.6
Cong Pan,Yan Sun,Yiqie Dong,Haobo Hou,Ming-Feng Kai,Jirong Lan
It is a green and sustainable path to establish cheap solid waste-based catalyst to establish peroxymonosulfate (PMS) catalytic system for the degradation of carbamazepine (CBZ) in water. In this study, durable copper tailing waste residue-based catalyst (CSWR) was prepared, and efficient CSWR/PMS system was constructed for catalytic degradation of CBZ for first time. The morphology and structure of CSWR changed from clumps to porous and loose amorphous by alkali leaching and medium temperature calcination . The reconstructed surface of the CSWR exposes more active sites promotes the catalytic reaction and increases the degradation rate of CBZ by more than 39.8 times. And the CSWR/PMS achieved a CBZ removal of nearly 99.99 % in 20 min. In particular, perovskite-type iron-calcium compounds were formed, which stimulated the production of more HO • and SO 4 •− in the system. DFT calculation shows that CSWR has stronger adsorption energy and electron transfer ability to PMS molecules, which improved the degradation efficiency of the system. In general, this study proposed a means of high-value waste utilization, which provided a new idea for the preparation of solid waste based environmental functional materials and is expected to be widely used in practical wastewater treatment .
研究领域:
环境科学
·
废水处理
·
催化材料
✓ 已验证
产品关联
DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Yiqun Chen,Xiaori Huang,Dedong Sun,Hongchao Ma,Guowen Wang,Chun Ma,Jun Hao
In this study, the Fe 3 O 4 /Co 3 [Co(CN) 6 ] 2 composite catalyst was synthesized by co-precipitation method. The morphology and the structure of Fe 3 O 4 /Co 3 [Co(CN) 6 ] 2 composites were characterized by XRD, FTIR, SEM, TEM, EDS, XPS, VSM. The results showed that the removal rate of RhB (10 mg/L) reached 99.5% in 40 min in the 0.4-Fe 3 O 4 /Co 3 [Co(CN) 6 ] 2 (200 mg/L) + PMS (50 mg/L) system with a pseudo first-order degradation rate constant (k) of 0.121 min −1 , which is nearly 2.16 times of that (0.0561 min −1 ) in the Co 3 [Co(CN) 6 ] 2 + PMS system and 18.9 times of that (0.0064 min −1 ) in the Fe 3 O 4 + PMS system. The observed synergistic catalysis between Fe 3 O 4 and Co 3 [Co(CN) 6 ] 2 in Fe 3 O 4 /Co 3 [Co(CN) 6 ] 2 enhanced the degradation of RhB. The electron paramagnetic resonance (EPR) analysis and quenching experiment indicated that SO 4 − and OH played important roles in the degradation process of RhB. A synergistic catalytic mechanism of PMS activation by Fe 3 O 4 /Co 3 [Co(CN) 6 ] 2 , which mainly involves the enhanced Co 2+ /Co 3+ cycle by Fe 2+ donated electrons, was proposed. In summary, owing to its easy preparation, excellent catalytic activity, and reusability, the Fe 3 O 4 /Co 3 [Co(CN) 6 ] 2 composite catalyst is a good candidate for remediation of contaminated water.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Jincheng Mu,Jinming Feng,Xinyang Wang,Baojun Liu
Cobalt-based oxides are promising candidates for heterogeneous activation of peroxymonosulfate-based (PMS) advanced oxidation processes towards contaminants degradation, hence improving their catalytic performance is desirable requirement. Herein, an oxygen vacancy-rich flower-like CoMoO 4 catalyst (CoMoO 4 -V O ) assembled with nanosheets was successfully synthesized and applied for PMS activation to eliminate emerging contaminants. The CoMoO 4 -V O catalyst exhibits superior organic pollutants (e.g. sulfamethoxazole, SMX) removal performance with an apparent reaction rate of 1.29 min −1 , which is much higher than that of the original CoMoO 4 catalyst (0.30 min −1 ). Additionally, the catalyst also shows remarkable contaminants conversion in real river water, and even achieves more than 90 % of SMX degradation efficiency under a continuous flow reaction condition with a hydraulic retention time of approximately 2 min. The characterization and density functional theory (DFT) calculation results indicate that much electron accumulates around the formed oxygen vacancy on the surface of catalyst and transfers towards substrates. Meanwhile, the introduction of more oxygen vacancies could boost the adsorption of PMS as well as SMX, and the electron-donation capacity of catalyst, thus improving the generation of reactive oxygen species and the subsequent contaminate elimination. Radical quenching and capture experiments demonstrate that the enhanced degradation performance of CoMoO 4 -V O catalyst is attributed to the boosted radical pathway, especially for SO 4 − species, while scarcely contributed from the non-radical 1 O 2 species. This work provides an effective catalyst for contaminant elimination through PMS activation and deeply reveals the defect engineering-induced activity enhancement mechanism.
研究领域:
环境科学
·
化学工程
·
材料科学
·
催化
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
·
2022
·
IF 10.319
Caiyan Gao,Xuezhen Feng,Lian Yi,Xiaoyong Wu,Renji Zheng,Gaoke Zhang,Yubiao Li
Formaldehyde (FA), as an important chemical raw material, has been widely used in many fields. However, the discharge of a large amount of FA-containing wastewater poses a serious threat to the environment and human health. Recently, the in-situ hydrogen energy release technology of hydrogen-containing stable liquid has been extensively explored due to its safe storage. Exploring a robust method to achieve FA removal and synchronous in-situ hydrogen release from FA containing wastewater is of great significant for environmental protection and energy crisis alleviation. Here, we have innovatively introduced peroxymonosulfate (PMS) activation technology into FA removal and hydrogen production simultaneously. The composite of nitrogen doped carbon coating Co 9 S 8 nanotubes (Co 9 S 8 @N−C) is employed as a proof of concept for FA decomposition and simultaneously hydrogen production based on PMS activation system. As expected, the Co 9 S 8 @N−C/PMS system presents much superior hydrogen production efficiency and satisfactory FA removal rate towards FA wastewater than those of common catalysis, photocatalysis and Fenton reaction in the basic condition in a wide range of FA concentration. The hydrogen yield reaches a value as high as 471 μmol within 60 min, corresponding to a FA degradation rate of 30% with an initial FA concentration of 0.722 mol L −1 . Characterizations and density functional theory (DFT) calculations suggest that the free radical process dominated by superoxide radical (O 2 ⋅ − ) and nonradical process dominated by singlet oxygen ( 1 O 2 ), which are induced by Co 9 S 8 @N−C/PMS system, are responsible for highly efficient hydrogen production via FA degradation. These generated O 2 ⋅ − and 1 O 2 can extract ⋅ H from FA to form ⋅ OOH intermediate, which can further combine with the ⋅ H from water to produce hydrogen. This study provides an applicable technique for environmental purification and new energy development based on FA containing wastewater.
研究领域:
环境科学
·
化学工程
·
能源技术
·
水处理
✓ 已验证
DOI
高影响因子