CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Shizong Wang,Lejin Xu,Jianlong Wang
Metal-free carbonaceous persulfate activator has received increasing attention recently. Graphitic carbon nitride (g-C 3 N 4 ) is one of the promising carbon materials due to excellent stability and low cost, but its activity for peroxymonosulfate (PMS) activation is low. In this study, g-C 3 N 4 was modified with oxygen atoms in the first step (O-g-C 3 N 4 ), then exfoliated via sequential thermal and ultrasound treatment to produce O-g-C 3 N 4 nanoflakes to increase its catalytic activity to activate PMS. In the presence of O-g-C 3 N 4 nanoflakes, SMX degradation rate achieved 0.079 min −1 , which was much faster than that in the presence of pristine g-C 3 N 4 (0.0083 min −1 ) and untreated O-g-C 3 N 4 (0.012 min −1 ). The surface-bound radicals and direct electron transfer between SMX and PMS contributed to the SMX degradation. Density functional theory (DFT) simulation revealed that oxygen-doping changed the charge distribution. Furthermore, O-g-C 3 N 4 nanoflakes had higher adsorption energy for PMS and SMX (0.518 kcal/mol) than pristine g-C 3 N 4 (0.304 kcal/mol), which contributed to the enhanced PMS activation and SMX degradation. Cycling experiments and comparison of characterization results before and after experiments proved that O-g-C 3 N 4 nanoflakes had superior catalytic and structural stability. This study could provide a high efficient metal-free carbonaceous activator of PMS for the degradation of antibiotics in the wastewater.
研究领域:
环境科学
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材料科学
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化学工程
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高影响因子
CHEMICAL ENGINEERING SCIENCE
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2026
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IF 5.1
Lin Li,Kaiyun Yang,Zhan Ding,Chang Liu
Spodumene is often associated with quartz in ore deposits. Due to their similar physicochemical properties, achieving selective flotation separation using sodium oleate (NaOL) alone is challenging. This study proposes an innovative reagent scheme for selectively separating spodumene from quartz via flotation. The approach employs a Cu(II)/peroxymonosulfate (PMS) advanced oxidation process to activate the spodumene surface, which subsequently promotes the adsorption of NaOL as the collector. Single-mineral flotation tests demonstrated that under the conditions of pH 8, NaOL concentration of 8 × 10 −4 mol/L, Cu(II):PMS molar ratio of 3:1, and total Cu(II)/PMS concentration of 3 × 10 −4 mol/L, the recovery of spodumene reached 93.48%, while that of quartz was only 0.91%. Artificial mixed mineral flotation tests yielded a spodumene concentrate with a Li 2 O grade of 6.52% and a recovery of 83.46%. The activation mechanism was investigated using zeta potential, contact angle, Fourier transform infrared spectroscopy (FTIR), electron paramagnetic resonance (EPR), scanning electron microscopy with energy dispersive spectroscopy (SEM), and X-ray photoelectron spectroscopy (XPS) analyses. The results indicate that OH generated by the Cu(II)/PMS system is associated with cleaning of the spodumene surface and modification of its chemical environment, which in turn correlates with enhanced NaOL adsorption and increased surface hydrophobicity. These observations are consistent with the improved flotation separation of spodumene from quartz under the tested conditions. This study presents a promising activation strategy for the efficient flotation of spodumene.
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高影响因子
Journal of Water Process Engineering
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2026
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IF 6.6
Guangxu Zhang,Jin Wang,Wubin Wang,Yadong Hu,Mengmeng Dou,Chao Han,Xinyu Li,Kaibo Wang,Yaxuan Liu,Yuting Ma
MnTiO 3 catalytic ceramic membrane (MTPCM) is prepared via solid particle impregnation- drawing- sintering method. • MTPCM 3 exhibits high BSA rejection primarily through dynamic cake layer formation and pore constriction. • Intermittent PMS backwash reduces chemical consumption while mitigating irreversible fouling. • MTPCM exhibits stable filtration performance over multi-cycle operation with PMS backwash. Ultrafiltration membrane's irreversible fouling-induced pore blockage and gel layer frequently reduce membrane lifespan. Peroxymonosulfate (PMS) can generate free radicals under appropriate catalysts, offering a promising strategy for membrane fouling control. This study developed a MnTiO 3 -modified catalytic ceramic ultrafiltration membrane (MTPCM) via an impregnation-drawing-sintering process. MTPCM achieved a BSA rejection >92%, attributed to dynamic cake layer formation and fouling-induced pore constriction. Higher membrane pressure, greater pollutant concentration, and longer filtration duration enhanced BSA removal by accelerating filter cake layer formation. Under optimized PMS backwash conditions (1 bar, 30 min, pH 7), the cleaning efficiency reached ∼60% after five cycles, approximately 2.3 times higher than that of water backwash (∼26%). Furthermore, an intermittent backwash strategy (four water backwashes followed by one PMS backwash) was evaluated: the MTPCM maintained ∼50% of its initial flux after 15 h of operation (three cycles), demonstrating stable multi-cycle performance with reduced PMS consumption. Hermia membrane fouling model analysis suggests that PMS backwash plays an important role in reducing irreversible fouling and may contribute to maintaining membrane performance during cyclic operation.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2026
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IF 12.5
Sijie Ge,Ge Chen,Zhaochang Wu,Mengchen Zong,Ruolan Chen,Jie Zhang
A bimetallic spinel Mn 0.8 Co 2.2 O 4 catalyst was successfully synthesized for PMS activation • Mn 0.8 Co 2.2 O 4 /PMS gains 100% OFX removal (25 min), 76.96% PMS use, 96.9% TOC removal • Coexisting radical and nonradical pathways via Co/Mn redox and oxygen vacancies • DFT confirmed Mn doping improved PMS adsorption, O O bond elongation, and d-band upshift • The catalyst exhibited excellent stability, reusability, and broad-spectrum applicability Ofloxacin (OFX), a recalcitrant fluoroquinolone antibiotic, poses significant risks to ecosystems and human health, necessitating the development of efficient remediation technologies. In this study, a bimetallic spinel Mn 0.8 Co 2.2 O 4 catalyst was successfully synthesized via pyrolysis of a CoMn-BTC metal-organic framework precursor and employed for peroxymonosulfate (PMS) activation toward OFX degradation. The incorporation of Mn into the Co 3 O 4 lattice induced lattice distortion, enlarging specific surface area (45.3 m 2 /g), and enriching Co 2+ content (58.34%), oxygen vacancies, and hydroxyl groups, thereby enhancing electron transfer capability and redox activity. The Mn 0.8 Co 2.2 O 4 /PMS system achieved complete OFX removal within 25 min (k = 0.14219 min −1 ), 1.78 times higher than pristine Co 3 O 4 , with high PMS utilization (75.96%) and near-complete mineralization (96.9% TOC removal). The catalyst exhibited excellent stability over five cycles with minimal metal leaching (Co: 0.365 mg/L, Mn: 0.079 mg/L) and maintained high efficiency (≥88.81%) across pH 3–11. Both radical (•O 2 − , SO 4 •- , •OH) and non-radical ( 1 O 2 , Co(IV) = O) pathways contributed, with 1 O 2 and •O 2 − predominant, with Co/Mn redox cycles and oxygen vacancies serving as key active sites. Electrochemical analysis and density functional theory calculations further confirmed that Mn doping enhanced PMS adsorption energy, elongated the O O bond, facilitated interfacial electron transfer, and shifted the d-band center closer to the Fermi level, thereby boosting catalytic activity. Three plausible degradation pathways were proposed based on reactive site analysis and intermediate identification. This work provides fundamental insights into Mn-doped cobalt spinel for Fenton-like PMS activation and demonstrates their potential as efficient, stable catalysts for antibiotic-contaminated wastewater remediation. Download: Download high-res image (296KB) Download: Download full-size image
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2026
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IF 12.5
Huajing Zhou,Yuanxin Huang,Wenbo Zhao,Lingxiang Zhao,Sai Tian,Tiancheng Li,Liang He
Lattice oxygen defects promote efficient oxidant activation • Iron and manganese sites drive singlet oxygen dominated oxidation • Rapid antibiotic degradation achieved in real water matrices • Catalyst shows low metal leaching and good cycling stability • Treated effluents show low ecological risk in seed germination tests Enhancing the activation efficiency of peroxymonosulfate (PMS) to generate reactive oxygen species (ROS) is crucial for boosting Fenton-like reactions. However, simultaneously promoting PMS adsorption, accelerating interfacial electron transfer, and shifting the activation pathway to optimize its activation kinetics still poses a substantial challenge. Herein, we developed a bimetallic catalyst enriched with lattice oxygen defects, denoted as Fe 14 Mn 1 -LOx, for PMS activation toward the remediation of emerging organic contaminants in aquatic environments. Combined experimental and theoretical mechanistic studies reveal that the intrinsic catalytic activity of Fe 14 Mn 1 -LOx originates from the intermetallic lattice oxygen defects (Fe-O latt -Mn). These defects significantly elongate the O O bond of adsorbed PMS and drastically lower its dissociation energy to 5.79 kJ mol −1 . Furthermore, the Fe-O latt -Mn sites increase the electron density near the Fermi level and adopt a bidentate coordination configuration, enabling faster and more efficient electron transfer to the O O bond, thereby promoting the generation of radical and non-radical species, predominantly singlet oxygen ( 1 O 2 ) with a contribution as high as 97.4%. Benefiting from these merits, the Fe 14 Mn 1 -LOx catalyst exhibits an exceptional degradation rate constant of 0.513 min −1 for tetracycline (TC), a representative emerging contaminant. This rate is 3.72 and 24.4 times higher than those of pristine FeOx (0.138 min −1 ) and MnOx (0.021 min −1 ), respectively. Remarkably, complete TC removal (100%) is achieved within just 10 min, outperforming most reported analogous catalysts. This work underscores the critical role of precisely engineering intermetallic lattice oxygen defects to modulate heterogeneous PMS activation, offering an innovative catalyst design strategy for efficient deep purification of emerging contaminants in real water matrices. Download: Download high-res image (263KB) Download: Download full-size image
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高影响因子
Desalination and Water Treatment
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2026
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IF 3.4
Yantao Zhu,Jianping Sun,Ying Xie,Qiyu Liu,Fu Zhu,Yetong Chen,Zeyu Wang,Manni Li,Hassaan Ahmad Butt,Huizhong Chi
Cu 0 - activated peroxymonosulfate (PMS) is a promising advanced oxidation process for the removal of pharmaceuticals and personal care products, yet its performance is often limited by inefficient Cu(II)/Cu(I) redox cycling as well as the low steady-state availability of reactive copper species. Here, we constructed a Cu 0 /HA/NCP/PMS system by integrating hydroxylamine as a reductant and neocuproine as a Cu(I) - complexing ligand to intensify naproxen degradation and investigate the underlying activation pathway. Under typical conditions, the synergistic combination of HA and NCP caused NPX removal to enable 98.57% within 6 min. This is significantly higher than those in Cu 0 /PMS, Cu 0 /NCP/PMS, and Cu 0 /HA/PMS. The system maintained high efficiency across pH 3.0 ~ 7.0. Scavenging tests and nitrobenzene probing indicated that ⋅ O H / S O 4 ⋅ − pathways were not dominant, whereas benzoic acid caused only moderate inhibition, collectively supporting a non-radical pathway. Spectroscopic and LC-MS evidence revealed a ligand-stabilized high-valent copper oxidant, with characteristic absorption at 358 nm and a signal at m/z 479 assigned to [Cu(III) - (NCP) 2 ] 3+ . This work provides a mechanistically grounded “reduction and complexation” strategy to overcome Cu - based persulfate activation bottlenecks and achieve rapid, pH - resilient degradation of NPX.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2026
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IF 12.5
Yu Jiang,Yinghao Tang,Cheng Tang,Cheng Qian,Si Wang,Xiuquan Xiong,Zipeng Zhang,Mengying Jia,Fangxian Wang,Qiong Liu
A metal-free P/O dual-site functional carbon nitride was synthetized. • P O Lewis-acid centers and O-coordinated electron-rich sites were induced to CN-P5. • CN-P5 removed 5 mg/L APAP within 60 min using 1 mM PMS. • APAP was degraded via hydroxylation, C N scission, ring opening, and mineralization. • PPCPs at realistic level were removed from actual domestic sewage continuously. Peroxymonosulfate (PMS) activation-based advanced oxidation processes provide powerful strategies for persistent pharmaceuticals and personal care products (PPCPs) removal in aquatic environments and wastewater. However, intrinsically sluggish PMS decomposition kinetics and inefficient utilization of reactive species impede their practical implementation. Developing robust, metal-free photocatalysts capable of efficiently activating PMS under mild conditions remains challenging. In this study, a metal-free P/O dual-site functional carbon nitride (CN-P5) featuring localized polarization was rationally constructed via phytic acid-assisted thermal polymerization, enabling efficient PMS activation under visible-light for rapid PPCPs degradation. With 1 mM PMS, complete removal of 5 mg/L acetaminophen (APAP) was achieved within 60 min. The degradation proceeded through hydroxylation, C N scission, ring opening, and progressive mineralization, accompanied by decreasing predicted toxicity of intermediates. Characterizations combined with density functional theory calculations revealed that P atoms partially substitute framework C to generate electron-deficient P O Lewis acid centers, preferentially accumulating photogenerated holes and promoting PMS adsorption. Meanwhile, O atoms coordinate at bridging N sites, giving rise to electron-rich P O units. The synergistic integration of these polarized dual P O dipolar sites boosted PMS activation efficiency. To demonstrate application potential, CN-P5 was packed into a fixed-bed continuous-flow reactor, enabling simultaneous and efficient removal of APAP, norfloxacin and sulfamethoxazole from real lake water matrices. Moreover, the reactor maintains stable removal efficiency for APAP, norfloxacin and ofloxacin continuously at realistic concentrations from actual domestic sewage. Collectively, this work establishes a scalable, metal-free PMS activation platform that couples dual-sites electronic engineering with continuous processing for PPCPs abatement in real waters.
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高影响因子
JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
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2026
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IF 7.1
Cong Geng,Xue Yang,Shengnan Chen,Zhiwei Zhao,Yinyan Guan,Weichun Gao,Jiyan Liang,Chen Yuan,Xiaofeng Chen
In recent years, the pervasive presence of antibiotics in surface water and their potential ecological risks have garnered significant attention. The advanced oxidation system of a dual-wavelength UV (VUV/UVC) synergistic peroxymonosulfate (PMS) has been employed as a potential technology for removing organic pollutants from water. The VUV/UVC/PMS process entails the irradiation of PMS with VUV (185 nm) and UVC (254 nm) to concurrently generate hydroxyl radicals (·OH), sulfate radicals (SO 4 ·- ), and singlet oxygen ( 1 O 2 ). This process has markedly enhanced pefloxacin (PEF) and levofloxacin (LEV) degradation efficiency. The experimental findings suggest that the VUV/UVC/PMS system attains optimal degradation of PEF and LEV under conditions of low initial PEF and LEV concentrations, elevated initial PMS concentration, elevated reaction temperature, and an initial pH of 11. In this system, ·OH, SO 4 ·- , and 1 O 2 are the main active species responsible for the degradation of LEV, contributing 84.46%, 5.52%, and 7.98%, respectively. Through EEM spectra and high-resolution mass spectrometry analysis, the degradation pathways of PEF and LEV were inferred, and the synergistic mechanism between VUV and PMS was revealed. A comparison of the individual processes with the VUV/UVC/PMS system showed a significant reduction in energy consumption, with PEF degradation energy consumption decreasing by 7.58%-41.87% and LEV degradation energy consumption decreasing by 2.7%-76.34%. The study indicates that the VUV/UVC/PMS system possesses the advantages of high efficiency, low energy consumption, and simple operation, making it a green and sustainable process for treating antibiotic pollution in surface water.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Yanlong Sun,Lei Yang,Hangyang Feng,Qianwei Liang,Jingyu Huang,Kangtao Zhou,Tianlie Luo,Chengzhi Zhou,Liguo Shen,Junfeng Niu
Diversified pharmaceuticals and personal care products (PPCPs) were developed, and complex wastewater also appeared simultaneously. The development of catalyst for advanced oxidation processes (AOPs) that can adapt to the complex needs of wastewater treatment is urgent. In this study, a high entropy single atom catalyst (HESACs) was synthesized and applied in peroxymonosulfate (PMS)-based AOPs for the removal of acyclovir (ACV). X-ray absorption fine structure, X-ray diffraction, and X-ray photoelectron spectroscopy analysis confirmed the successful synthesis of HESACs. The mechanism of PMS activation was elucidated through quenching studies and electron paramagnetic resonance analysis. During PMS activation in HESACs, ACV undergoes degradation via multiple pathways, including • O 2 − , • OH, SO 4 •− , 1 O 2 , high-valent metal-oxo, and direct electron transfer. These pathways enhance the adaptability of the system to the complex wastewater demands. ACV was completely degraded within 7 min, achieving 28.82 % mineralization within 30 min in the HESACs/PMS system. Furthermore, the system demonstrated higher removal efficiency under alkaline conditions, with degradation efficiency remaining above 90 % after five cycles. The degradation intermediates of ACV were identified, and the degradation mechanism was elucidated. The system is capable of detoxifying ACV. DFT calculations results indicate that regions with negative potential and atoms exhibiting higher f − values in ACV molecules are more prone to attack within the HESACs/PMS system. This study presents the synthesis and application of HESACs in complex water environments for the degradation of PPCPs.
研究领域:
环境科学
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催化
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材料化学
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水处理技术
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物理化学
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高影响因子
Journal of Environmental Chemical Engineering
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2024
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IF 7.4
Jie Lin,Yunxiong Zeng,Xingyu Zhan,Jingcai Xu,Xinqing Wang,Bo Hong,Xiaoling Peng,Jing Li,Hongwei Chen,Yingchun Xia
Ciprofloxacin (CIP) possesses significant ecological risks to aquatic environments, prompting the search for effective removal methods. Peroxymonosulfate (PMS) based activation emerges as a promising method for water-based CIP degradation. In this study, alginate was converted into spherical calcium alginate hydrogels (CAH) as an activator of PMS to remove CIP. The optimized CAH/PMS can degrade 86.73 % of CIP within 85 min with a first-order kinetic constant of 0.039 min −1 . In addition, a relationship between spherical size of CAH (2.4, 3.5, 4.0 and 5.0 mm) and activities of CIP degradation is established, demonstrating 4.0 mm diameter CAH (4.0-CAH) possessing the highest CIP removal efficiency, far higher than 2.4-CAH (50.25 %, 0.014 min −1 ), 3.5-CAH (51.54 %, 0.021 min −1 ), and 5.0-CAH (78.71 %, 0.036 min −1 ). Besides, 4.0-CAH/PMS are not susceptible to various interference factors, including water bodies, pH, ion, and organic matter. The capture test shows excellent CIP degradation of 4.0-CAH is mainly dominated by a synergistic effect of superoxide radical, hydroxyl radical and singlet oxygen. This study highlights the practicality of scalable CAH as a metal-free catalyst for PMS activation and CIP removal, emphasizing its advantages in cost-effectiveness, easy regeneration, environmental friendliness.
研究领域:
环境科学
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化学工程
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材料科学
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水处理技术
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高影响因子
Journal of Environmental Chemical Engineering
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2024
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IF 7.4
Wanqi Tang,Yanyang Liu,Qingliang You,Xiaofang Yang,Guiying Liao,Dongsheng Wang,Ying Yan,Qigao Shang
The cobalt monoatomic catalyst with 3D ordered macropores structure (3DOM Co/NC) was prepared using the crystalline porous material ZIF-67 and SiO 2 as the precursor and template, and used to investigate the effect of its activation with peroxymonosulfate (PMS) on sulfamethoxazole (SMX) removal. The mesoporous structure mostly retained after ZIF-67 carbonisation, and the formation of new homogeneous macropores after the removal of the SiO 2 template, which greatly increases the surface area of the catalyst (429 m 2 g −1 ) and promotes long-range mass transfer. Additionally, Co monoatomic sites were formed in the porous skeleton, providing electrons that were utilised for the activation of PMS. This distinctive structure enables it to almost completely degrade of 20 ppm SMX within 3 min and show excellent catalytic degradation efficiency in a wide pH range (3.0–9.0) and high-salinity simulated wastewater (10–100 mM). In addition, the main ROS in the catalytic degradation process were explored as 1 O 2 and O •2- . Combined with the results of DFT calculations and product analyses, the active sites of SMX were predicted and the degradation pathways and mechanisms were inferred, confirming that the degradation process of SMX poses a low risk of toxicity to the environment. This study reveals that the addition of 3DOM Co/NC was more favourable for the activation of PMS for SMX degradation, which contributes to the development and improvement of advanced oxidation processes for environmental remediation.
研究领域:
环境科学
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催化化学
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材料科学
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高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2024
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IF 4.9
Xinrui Han,Geng Li,Weiyan Su,Xusheng Xu,Mengjiao Yu,Guangyu Wu,Weinan Xing
The degradation of recalcitrant antibiotics through the activation of peroxymonosulfate (PMS) is an important branch of advanced oxidation processes (AOPs), with widespread attention given to the application of metal-organic frameworks (MOFs) in this field. The article successfully synthesized Cu x O/N-doped carbon/Cu-MOF (Cu x O/NC/Cu-MOF) nanocomposites by low-temperature thermal treatment of Cu-MOF precursors. Compared with the original MOF, these partially decomposed composite materials exhibit significantly stronger catalytic activity towards PMS, efficiently removing organic pollutants such as tetracycline (TC). After optimization, the sample treated at 400 °C, under visible light with PMS assistance, achieves an impressive degradation rate, almost completely degrading a 50 mL TC solution (10 mg/L) after 80 min. This achievement surpasses the degradation rate observed with the original Cu-MOF by 2.1 times. In the composite system of Cu x O/NC/Cu-MOF+PMS+Vis, the significant enhancement of activity is credited to the effective spatial separation of photogenerated electrons and holes, as well as the utilization of 1 O 2 as the primary active oxygen species. This work provides a simple preparation strategy for the development of Cu-based PMS activators with excellent photocatalytic performance.
研究领域:
环境科学
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材料科学
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DOI
高影响因子
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