CHEMICAL ENGINEERING JOURNAL
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2026
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IF 12.5
Quanhui Yue,Qianhui Liu,Lagui Yi,Ting Mei,Jinxia Yang,Zihan Zhou,Yilong Jin,Sicong Ma,Shaohui Wang,Xiaomei Liao
Targeted control of tetracycline resistance in aquatic environments is an urgent public health issue. Singlet oxygen ( 1 O 2 ) can selectively attack guanine bases in DNA sequence, offering a potential strategy for eliminating guanine-rich tetracycline resistance genes. However, conventional zero-valent iron (ZVI) activated peroxydisulfate (PDS) processes predominantly rely on non-selective free radicals (e.g. , SO 4 •- and •OH) generated via stepwise single-electron transfer. In this study, we developed a riboflavin-modified ball-milled ZVI (RF-ZVI bm ) that redirected the PDS activation pathway. The optimized RF-ZVI bm /PDS system achieved complete (6-log) inactivation of tetracycline resistant E. coli and effective degradation of the plasmid-encoded tet gene within 15 min, effectively eliminating its transformability. Mechanistic studies revealed that the surface-bound RF functioned as a bifunctional proton-coupled electron transfer (PCET) mediator, it facilitated a concerted transfer of two-electron/proton (2e − /2H + ) owing to the availability of protons in RF-ZVI bm /PDS system. This PCET pathway directly drove PDS activation toward the highly selective generation of 1 O 2 , achieving a remarkable production rate of 136.04 μM•L −1 •min −1 while substantially suppressing radical byproducts. RF-ZVI bm demonstrated excellent reusability over multiple cycles with minimal and environmentally benign modifier leaching, supporting its potential for practical application. This work elucidates a tailored PCET mechanism for dominant 1 O 2 production and provides a potent strategy for controlling the dissemination of tetracycline resistance in water environments.
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高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2026
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IF 9.6
Saeed Rehman,Tao Chen,Hongjuan Sun,Muddasir Hanif,Tongjiang Peng,Osama Tariq Satti,Aref Alshameri
Phthalate esters (PAEs), widely used as plasticizers, persist as recalcitrant organic pollutants with severe ecological implications. In this study, a dual-step pyrolysis strategy was employed to engineer a Fe-N-RHC@p-MMt composite photocatalyst enriched with high-valent Fe sites, nitrogen dopants, and oxygen vacancies. The tailored hybrid achieved a remarkable 92 ± 1.4% degradation of dimethyl phthalate (DMP) with a pseudo-first-order rate constant of 0.64 min −1 in a peroxydisulfate (PDS)-mediated oxidation system under near-visible light irradiation. Structural and spectroscopic analyses revealed graphitized carbon frameworks with superior conductivity, efficient charge migration, and abundant Fe(IV) = O species formation. Mechanistic analysis reveals that Fe₄N centers regulate interfacial electron transfer, stabilize high-valent Fe(IV) = O species, and drive selective non-radical PDS activation dominated by singlet oxygen ( 1 O₂). Moreover, the generated intermediates exhibited significantly reduced toxicity, mutagenicity, and bioaccumulation risks (although intermediates P1, P3, and P6 showed elevated toxicity), validating the process's environmental compatibility. These results highlight Fe-N-RHC@p-MMt as a safe and efficient catalyst for sustainable remediation of PAE-contaminated water.
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高影响因子
APPLIED SURFACE SCIENCE
·
2026
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IF 6.6
Jiaxi Wu,Yuxin Huang,Jingyi Li,Qiang Cheng,Kai Wang
A low-valence cobalt nanoparticles supported on biochar (HS-15Co) was synthesized. • Low-valence Co promotes electron transfer to PAA, sustaining the non-radical activation process. • Singlet oxygen ( 1 O 2 ) is the dominant reactive oxygen species in the HS-15Co/PAA system. • The TC degradation pathway and intermediate toxicity were analyzed. • This work offers insights for designing carbon-supported metal catalysts and enhancing PAA-based water purification. Peracetic acid (PAA)-based advanced oxidation processes (AOPs) are promising for antibiotic wastewater remediation, while the role of cobalt valence states in PAA activation remains unclear. Herein, a series of low-valence Co-loaded biochar catalysts (HS-xCo) were synthesized, realizing uniform dispersion of Co nanoparticles and formation of low-valence Co species. The target HS-15Co catalyst exhibited superior catalytic performance, achieving 94.6% tetracycline (TC) degradation, which was 3.0 times that of pristine biochar. Structural characterizations confirmed that low-valence Co(0)/Co(II) nanoparticles were stably anchored on biochar surface without obvious agglomeration. Quenching experiments and electron spin resonance (EPR) verified singlet oxygen ( 1 O 2 ) as the predominant reactive oxygen species (ROS) responsible for TC degradation. Electrochemical measurements and Density functional theory (DFT) calculations corroborated that Co incorporation significantly enhanced PAA adsorption and promoted interfacial electron transfer, thus boosting PAA activation efficiency. Furthermore, three possible TC degradation pathways were proposed based on liquid chromatography-mass spectrometry (LC-MS) analysis, and toxicity prediction demonstrated that most degradation intermediates showed lower toxicity than parent TC. This work provides a low-valence Co/biochar catalyst for efficient PAA activation through 1 O 2 -dominated pathway, offering a feasible strategy for emerging organic pollutant removal in aquatic environment. Download: Download high-res image (164KB) Download: Download full-size image
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Journal of Environmental Chemical Engineering
·
2026
·Vol. 14
·期 5
·124130
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IF 7.5
Xiang Li,Yu Tian,Yalong Xu,Bo Liu,Shi Zhou,Wei Jiang,Chunbo Liu,Guangbo Che
Precisely designing catalyst structures through chemical strategies to achieve non-radical-mediated Fenton-like catalysis for the efficient removal of organic contaminants is of great significance. Herein, a heptazine-porphyrin organic polymer (HPOP) was synthesized via a nucleophilic substitution reaction. Subsequently, a heptazine-porphyrin organic polymer catalyst featuring Co-N 4 sites (HPOP-Co 20 ) was fabricated through a solvothermal method for efficient peroxymonosulfate (PMS) activation. The porphyrin core effectively anchored the Co-N 4 active sites, inducing the generation of singlet oxygen from PMS. The high conjugation of porphyrin and heptazine effectively enhances the charge transport capability of the catalyst. Upon coordination with Co single atoms, the charge distribution of the polymer was reconstructed, facilitating rapid electron transfer to PMS. Compared with the original HPOP, the reaction rate constant of HPOP-Co 20 activating PMS for degrading sulfamethoxazole (SMX) could reach 1.7018 min −1 , which is 92.99 times that of the HPOP/PMS system (0.0183 min −1 ). The non-radical-mediated characteristic enabled HPOP-Co 20 /PMS to achieve efficient degradation across various water bodies, pollutants, anions, and initial pH conditions. The results of phytotoxicity and continuous wastewater treatment experiments indicated that SMX toxicity decreased after degradation, highlighting the practical application potential of this system. This study introduces a controllable substrate structure and a Co-N 4 site catalyst that promote non-radical pathways and enhance its stability and environmental adaptability.
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高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2026
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IF 6.7
Bing Wang,Yao Liu,XiangBo Feng,MeiMei Xu,EnZhou Liu,YuZhen Zhao,ZongCheng Miao,Zhuo Li
Ag 3 PO 4 exemplifies the persistent activity-stability trade-off in photocatalysis, where its high photo-oxidation capability is inevitably undermined by severe photocorrosion. This work breaks this coupling by constructing Ce 3 + /Ce 4+ redox-mediating centers within Ag 3 PO 4 . The optimal catalyst achieves near-complete degradation of tetracycline antibiotics within 30 min, with a rate constant increased by approximately 3.2 times, and maintains over 85% of its initial activity after five cycles, whereas pristine Ag 3 PO 4 undergoes complete deactivation. Singlet oxygen ( 1 O 2 ) is identified as the dominant species, and a dual-pathway generation mechanism that bypasses the material's inherent constraints is unveiled: alongside the • OOH‑mediated hole oxidation pathway, the Ce 3+ /Ce 4+ couple catalyzes a sequential two‑electron O 2 reduction to H 2 O 2 and its subsequent Fenton‑like conversion to 1 O 2 . Combined spectroscopic and theoretical analyses confirm that these centers act as exclusive electron traps, diverting photoexcited electrons away from Ag + sites—thus inhibiting Ag + → Ag 0 corrosion—and directing both electron and hole densities toward themselves in the excited state. This work demonstrates that engineering atomically dispersed redox mediators can decouple charge separation from detrimental surface reactions, providing a general strategy to simultaneously confer high activity and robust stability upon otherwise fragile photocatalysts.
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高影响因子
RSC Advances
·
2026
·Vol. 16
·期 23
·20933-20945
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IF 6.1
Hangdao Qin,Pei Liu,Junnan Hao,Lei Xiao,Yong Wang,Jiming Huang,Jun Chang,Yuru Shen,Bo Xing,Guo Yang
The distillers' grains biochar was prepared by a simple ball-milled process, followed by pyrolysis at different temperatures. The as-prepared biochars were then utilized to degrade ciprofloxacin (CIP) via peroxymonosulfate (PMS) activation. At the optimal pyrolysis temperature of 900 °C, a biochar with a high density of surface defects and a large surface area was generated. Therefore, 100% CIP degradation was attained within 40 min using the DBC900/PMS system. This system also showed good stability across five reuse cycles as well as good performance over a wide range of pH values. The water matrix showed a negligible effect on CIP degradation in this system. Electron paramagnetic resonance (EPR), quenching experiments and electrochemical analysis demonstrated that CIP degradation involved non-radical and electron transfer pathways. The production of 1O2 and electron transfer mediated by the metastable complex DBC900-PMS* were crucially involved in this degradation reaction. Moreover, a possible degradation pathway of CIP was proposed based on the analysis of the intermediate products. Overall, this study provided an enhanced understanding of the biochar-activated PMS mechanism and offered a compelling strategy for the resourceful utilization of waste distillers' grains.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2026
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IF 9.1
Zhibang Gao,Qiumin Wang,Chi Wang,Shuangyou Bao,Fei Wang,Kai Li,Yi Mei
The performance of peroxymonosulfate (PMS)-based advanced oxidation processes is often limited by inefficient reactive oxygen species (ROS) utilization and instability of active metal sites. Herein, a dual-confinement strategy is proposed by integrating spatial pore confinement and coordination confinement into Ti-based metal–organic frameworks (MOFs) to regulate PMS activation. Compared with Ti-BPDC, the pyridine-functionalized Ti-BPYDC framework provides Co N coordination sites, enabling stronger stabilization and electronic modulation of Co active centers. As a result, the Co-Ti-BPYDC/PMS system achieves enhanced tetracycline degradation (98.83% within 30 min), higher reaction kinetics (0.54 min −1 ), and improved mineralization (44.73%). Mechanistic studies reveal that the dual-confinement structure promotes interfacial electron transfer, stabilizes the Co 3+ /Co 2+ redox cycle, and favors a singlet oxygen ( 1 O 2 )-dominated non-radical pathway, while suppressing Co leaching. Consequently, the catalyst exhibits excellent stability and resistance to environmental interference. This work provides a general strategy for designing efficient and stable MOF-based catalysts for advanced oxidation processes.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2026
·
IF 9.1
Yuhang Fan,Rongrong Zhu,Jiaze Liu,Jiaqian Yang,Jiangbo Zhong,Danna Ding,Yuwen Ma,Yuxiang Liang,Ruya Chen,Yijing Xia,Huajun Feng,Yangcheng Ding
Antibiotic resistance proliferation has underscored the urgent need for advanced strategies to treat antibiotic-containing wastewater. This study developed a novel CoFe 2 O 4 -encapsulated carbon nanotube composite (CoFe 2 O 4 @CNT) via a modified impregnation–sintering method for the efficient activation of peroxymonosulfate (PMS) to antibiotic degradation. The CoFe 2 O 4 @CNT/PMS system achieved 95.3% degradation of florfenicol (FLO) within 30 min under optimal operational conditions (pH 7, 5% metal loading, 0.5 mM PMS, 87.5 mg/L catalyst). Quenching experiments and electron paramagnetic resonance spectroscopy identified hydroxyl radicals (•OH), sulfate radicals (SO 4 •− ), superoxide anions (O 2 •− ), and singlet oxygen ( 1 O 2 ) as the primary reactive species responsible for FLO degradation. To enable continuous-flow operation, the catalyst was further immobilized onto a ceramic membrane (designated as CF@CNTCM) via vacuum filtration. The CF@CNTCM/PMS system demonstrated maintained high FLO removal efficiency with negligible cobalt leaching, significantly surpassing conventional cobalt-based catalysts. Furthermore, the system exhibited robust performance in real water matrices, including river water and aquaculture wastewater, effectively reducing chemical oxygen demand and dissolved organic matter. This work presents a sustainable and highly efficient strategy for antibiotic degradation through catalytic ceramic membrane technology, with substantial potential for practical applications in water treatment.
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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2026
·
IF 19.7
Xuefei Li,Cheng Cheng,Lixia Yang,Zhenglin Chen,Shuqu Zhang,Jianping Zou
Bi 3+ doping enhances the singlet oxygen ( 1 O 2 ) lifetime. • Oxygen vacancy-rich Bi-Co 3 O 4 catalyst. • Under irradiation, Bi-Co 3 O 4 can efficiently degrade toluene and sterilize bacteria. • Bi-Co 3 O 4 exhibits efficient antibacterial activity, providing new insights for practical indoor air purification Developing efficient materials with excellent adsorption properties and photoactivity is pivotal for photocatalytic abatement of VOCs and bacteria in the air. Herein, Bi 3+ -doped Co 3 O 4 (Bi-Co 3 O 4 ) photocatalysts were successfully synthesized via a one-step hydrothermal-calcination method. Incorporation of Bi 3+ ions induces lattice distortion in Co 3 O 4 , generating oxygen vacancies (OVs), which subsequently modulates the electronic structure of Co 3 O 4 and produces singlet oxygen species ( 1 O 2 ) with a lifetime of 30 min. The Bi-Co 3 O 4 , with a geometric area of 24 cm 2 , achieves complete degradation (100%) of 50 ppm toluene within 30 min and a high mineralization rate of 93.4%. It retains outstanding photocatalytic activity even after multiple usage cycles. Notably, high-reactivity oxygen species at the Bi-Co 3 O 4 interface can effectively eliminate Escherichia coli ( E. coli ) and Staphylococcus aureus ( S. aureus ). This work offers theoretical insights for the design of stable and efficient photocatalysts aimed at improving indoor air quality. Download: Download high-res image (212KB) Download: Download full-size image
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高影响因子
CHEMOSPHERE
·
2023
·
IF 8.8
Jie Li,Hua Yin,Haoyu Luo,Yingchao Li,Xufa Rong,Zhi Dang
Polychlorinated biphenyls (PCBs) degradation by peroxymonosulfate (PMS) activation through •OH and SO 4 •– radical oxidation process was the effective technology in the last decades; however, there were few research focusing on removing PCBs by O 2 •– and 1 O 2 induced by PMS activation. In this work, 90.86% of 2,4,4-trichlorodiphenyl (PCB 28) was degraded by 0.3 g/L Fe 3 C@Fe-800 activated 0.5 mM PMS system under the synergistic action of O 2 •– and 1 O 2 . The structures of Fe 3 C@Fe-800 were identified by Scanning electron microscope (SEM), High resolution-transmission electron microscopy (HR-TEM), X-ray photoelectron spectroscopy (XPS), Brunauer-Emmett-Teller (BET), Raman spectra and Fourier transform infrared (FT-IR) spectra. Electron paramagnetic resonance (EPR) measurements and quenching tests verified that O 2 •– and 1 O 2 were the primary reactive species in Fe 3 C@Fe-800/PMS/PCB 28 ternary reaction system. Density functional theory (DFT), Linear sweep voltammetry (LSV), and chronoamperometry test revealed that electron-deficient Fe atoms on Fe 3 C were the main active sites in Fe 3 C@Fe-800 for PMS activation to generate 1 O 2 . Unlike the reported •OH and SO 4 •– mediated degradation induced by the iron-based catalyst, both O 2 •– and 1 O 2 contributed to PCB 28 degradation： nucleophilic dichlorination reaction by O 2 •- and then ring-open oxidation process by 1 O 2 . Fe 3 C@Fe-800/PMS system had excellent catalytic performance under different reaction conditions and possessed desirable inorganic salt and natural organic matter resistance. This work elucidated the important role of Fe 3 C in PMS activation to generate O 2 •- and 1 O 2 for PCB 28 decontamination by nonradical way and provided a clue to design rationally catalysts in polychlorinated biphenyl pollution remediation.
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PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Lei Zhou,Yubo Yan,Hengyang Mao,Shouyong Zhou,Jiayu Hui,Haodong Li,Meisheng Li,Yijiang Zhao,Qi Zhang,Shanshan Xia
Antibiotic contamination of aquatic ecosystems has attracted growing concern over the past few years. As a novel and low-cost catalytic membrane, attapulgite-based ceramic membrane (ATPCM) impregnated with Co 3 O 4 (Co-ATPCM) was successfully prepared for the degradation of sulfamethoxazole (SMX) under peroxymonosulfate (PMS) activation. The physical and chemical properties of ATPCM and Co-ATPCM were characterized by SEM-EDS, XRD, XPS, zeta potential, contact angle and the three-point bending test. Co was stably anchored on ATPCM via X-O-Co (X denotes Al, Si or Mg) bonds during the catalytic process, avoiding Co leaching. Approximately 70 % SMX could be removed by the optimized Co-ATPCM in batch experiments over a wide pH range from 4.0 to 10.0. Furthermore, 58 % SMX degradation was observed during filtration experiments with a high water flux of up to 774 L m −2 h −1 (LMH). According to the quenching experiment and electron paramagnetic resonance (EPR) spectroscopy, SO 4 − , OH and 1 O 2 were involved in the SMX degradation process, while 1 O 2 played a dominant role. Density functional theory (DFT) calculation successfully predicted that the sits on SMX molecules with high Fukui index were more susceptible to attacks by free radicals, confirmed by liquid chromatography-Quadrupole-time of flight mass spectrometer (LC-MS). Consequently, a possible pathway for the catalytic oxidation process was proposed based on the results of DFT and LC-MS. This study provided a promising strategy using natural magnesium aluminum silicate clay minerals to prepare cost-effective, efficient, and eco-friendly catalytic membranes for wastewater treatment.
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高影响因子
APPLIED SURFACE SCIENCE
·
2021
·
IF 6.707
Xin Jiang,Sanmei Liu,Wen Wang,Shunli Shi,Zhenxing Zeng,Chao Chen
Photocatlytic water disinfection for pathengenic miroorgasnisms removal is of great importance to public health safety, however the photocataltyic performance is unsatisfactory due to the low reactive oxygen species (ROS) generation. In this work, an innovative energy-transfer-mediated oxygen activation system on PCN-224-Zn is proposed for selective singlet oxygen generation without the need of electron-hole separation. The as-prepared PCN-224-Zn exhibits remarkable singlet triggered photocatalytic E-coli inactivation and organic pollutant degradation performance. The enhanced photocatalytic activity is attributed to the introduction of Zn into the metal-organic frameworks (MOFs) that facilitates the transformation of electron-hole couple from singlet to triplet state for selective singlet oxygen generation with high efficiency. This work provides a new oxygen activation pathway for efficient and selective ROS generation without the need of electron-hole separation.
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高影响因子
危险品化学品经营许可证（带存储）