SCIENCE OF THE TOTAL ENVIRONMENT
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2021
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IF 7.963
Fuwei Sun,Tianhu Chen,Haibo Liu,Xuehua Zou,Peixun Zhai,Ziyang Chu,Daobing Shu,Hanlin Wang,Dong Chen
Occurring naturally siderite (FeCO 3 ) was used as the heterogeneous catalyst to activate peroxodisulfate (PDS) for the degradation of sulfadiazine under different initial pH values. The findings of this system exhibited various ROS (e.g. 1 O 2 , SO 4 − and OH) present during a wide range of pH values. Among them, 1 O 2 could significantly facilitate the initial degradation rate, and the increased pH enhanced the role of 1 O 2 . The factors including initial pH values, siderite dosage, PDS concentration, initial contaminants concentration, and water matrix were discussed. The role of each ROS was investigated through quenching test and electron paramagnetic resonance (EPR). Furthermore, the comprehensive degradation process was proposed based on the LC-MS results. And the cycle test demonstrates the reusability of siderite at a pH of 3. Accordingly, this study is of great significance for understanding the degradation of such sulfonamide pollutants in the siderite/PDS system.
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高影响因子
ANALYTICAL CHEMISTRY
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2019
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IF 6.35
Xiaoya Fan,Yanying Wang,Li Deng,Lin Li,Xinfeng Zhang,Peng Wu
Singlet oxygen, generated from type-II photosensitization, has become increasingly popular in bioassay development in recent years. However, the transient nature of singlet oxygen in water (lifetime shorter than 4 μs) as well as its high activity make it easily inactivated by solvent molecules and other coexisting species, thus deteriorating use in the analytical sensitivity. Here, we proposed the use of a simple redox mediator for storing the energy of the transient singlet oxygen. To demonstrate such an idea, singlet oxygen generated from photosensitization of the double strand DNA–SYBR Green I (dsDNA-SG) complex was explored as a redox donor that can be modulated through formation and deformation of the dsDNA structure. After screening of a series of redox mediators with luminol chemiluminescence (CL) as the probe, ferrocyanide (K4Fe(CN)6) was found to be the most efficient, resulting in ∼30-fold intensified luminol CL. By storing the oxidative capacity of singlet oxygen in ferrocyanide, the dsDNA-SG complex was evolved into a photosensitization-mediated chemiluminescence (PMCL) biosensing platform for DNA detection. Such a PMCL sensing platform allows label- and amplification-free detection of picomolar-scale DNA with a limit of detection (LOD) of 1.5 pM (0.45 fmol in absolute). The excellent sensitivity of PMCL sensing confirmed that such a facile storage approach to oxidative capacity would be appealing for singlet-oxygen-involved biosensing.
研究领域:
分析化学
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生物医学工程
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光化学
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Dawei Song,Yukun Pan,Huan Chen,Yaqin Shi,Yanan Huang,Bo Niu,Donghui Long,Yayun Zhang
Singlet oxygen ( 1 O 2 ) plays a crucial role in environmental catalysis owing to its long lifetime, strong electrophilicity, and high selectivity, whereas selective generation of 1 O 2 with conventional catalysts remains challenges. Herein, we for the first time construct a FeS 2 -FeMoO 4 heterostructure supported on graphene oxide (FeMoS-GO), and subsequently evaluate its efficacy in peroxymonosulfate (PMS) activation for degrading organic pollutants. Compared with non-heterostructures, our catalyst alters the electron density and coordination environment of Fe and Mo, enhancing electron transfer and facilitating the cyclic conversion of Fe 2+ /Fe 3+ during PMS adsorption and activation. Experiments indicate that FeMoS-GO generates nearly 100 % 1 O 2 , with concentrations two to three orders of magnitude higher than those of •OH and SO 4 •- . Density functional theory (DFT) calculations and electrochemical tests also support the high efficiency of electron transfer and PMS adsorption by heterostructure. The degradation for phenol of FeMoS-GO is 100 times faster than that of the non-heterogeneous structure, and its degradation rate for various organic pollutants exceeds 90 %, while also demonstrating satisfactory performance in interference and stability tests. Our findings offer new insights and approaches for the efficient and controlled generation of 1 O 2 in water treatment and environmental remediation.
研究领域:
环境催化
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材料科学
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高级氧化过程
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水处理技术
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多相催化
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Journal of Water Process Engineering
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2024
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IF 6.3
Xingping Deng,Hua Yang,Dongye Zhao,Jingchun Guan,Zhengxuan Gu,Liang Zhang
Graphitic carbon nitride (g-C 3 N 4 ), a nitrogen-rich polymeric semiconductor, has gained significant attention as a photocatalyst . However, its potential to activate permonosulfate (PMS) has been somewhat limited. Prior research has demonstrated that manganese-doped g-C 3 N 4 can effectively activate PMS to degrade pollutants, with Mn 3+ playing a pivotal role. Consequently, enhancing the Mn 3+ content within the system is of paramount importance. In this study, we developed a novel class of manganese‑copper doped g-C 3 N 4 materials using a hydrothermal-calcination process. The optimized material, denoted as Mn 5 Cu 5 -CN, was synthesized at a Mn/Cu molar ratio of 1:1. When applied to degrade a model contaminant, acetaminophen (ACP), the Mn 5 Cu 5 -CN/PMS system demonstrated remarkable efficiency, degrading nearly 20 mg/L of ACP within 30 min (material dosage = 0.4 g/L, PMS concentration = 2.0 mM). The Mn 5 Cu 5 -CN exhibited favourable performance across a broad pH range. Singlet oxygen ( 1 O 2 ) was identified as a major player in the degradation of ACP. X-ray photoelectron spectroscopy (XPS) analyses revealed that the cyclic redox reactions of Mn 3+ /Mn 4+ and Cu + /Cu 2+ led to the abundant generation of 1 O 2 . Superoxide (O 2 •- ) was identified as an important intermediate product in these processes. Additionally, the g-C 3 N 4 present in the material also facilitated the generation of reactive oxygen species (ROS). This study provides a fresh perspective on the utilization of g-C 3 N 4 for pollutant degradation, highlighting the potential of Mn Cu doped g-C 3 N 4 materials in environmental remediation.
研究领域:
环境科学
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材料科学
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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Danlian Huang,Yulin Ren,Meiqing Ren,Guangfu Wang,Li Du,Ruijin Li,Wenbo Xu,Hai Huang,Sai Li,Lu Shen
Peracetic acid (PAA) has shown good potential in advanced oxidation techniques, but the mechanism regulating the generation of non-radical species in peracetic acid has not been clarified. Herein, Ov-Co 3 O 4 /C-x was prepared by pyrolysis of ZIF-L precursors at different temperatures to achieve the regulation of oxygen vacancy concentration and used for the degradation of sulfamethazine (SMT) by activated PAA. When x = 350 °C, the prepared Ov-Co 3 O 4 /C-350 with the highest oxygen vacancy content had the highest SMT removal efficiency and the highest rate constant( k obs ), which degraded SMT by 99.6 % within 30 min. The role of oxygen vacancies(OVs) on the surface of Ov-Co 3 O 4 /C-350 was investigated using quenching experiments, Electron Paramagnetic Resonance (EPR) and X-ray Photoelectron Spectroscopy (XPS) techniques. The results showed that oxygen vacancy on the metal oxide surface can be converted into more reactive oxygen(O*), and surface OVs of Ov-Co 3 O 4 /C-350 enable efficient capture of PAA, thus generating 1 O 2 and R-O•. The higher the content of oxygen vacancies is, the more 1 O 2 is produced, while concentration of R-O• was not significantly correlated with oxygen vacancy content. Furthermore, the degradation pathway of SMT was predicted through density functional theory (DFT) calculations and identifications of intermediates, indicating that electron-rich sites such as aromatic rings and S-N bonds in the SMT molecule are more easily oxidized by reactive species. Besides, due to the low biotoxicity of the degradation products of the Ov-Co 3 O 4 /C-350/PAA system, the reaction can effectively reduce the biotoxicity and developmental toxicity. This study provides a controllable surface property strategy for a new idea in PAA-based AOP.
研究领域:
环境科学
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化学工程
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Nature Communications
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2026
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IF 18.1
Zhu Shien,Yang Xiaofei,He Di,Zhang Yanyan,Liu Hang,Zhou Xiaoyu,Su Dawei,Wang Guoxiu,Wang Tianyi,Wang Chengyin
Coral reefs, vital marine ecosystems, are increasingly threatened by global warming and chemical pollutants such as benzophenone-3 (BP-3), a widely used UV filter. To address this challenge, we present a carbon-doped graphitic carbon nitride (g-C 3 N 4 ) photocatalyst with efficient singlet oxygen ( 1 O 2 ) generation for BP-3 degradation and coral vitality restoration under simulated seawater conditions. The photocatalyst exhibits improved stability and photocatalytic performance in complex seawater environments, with enhanced charge separation and an approximately eightfold increase in the apparent degradation rate of BP-3 compared with pristine g-C 3 N 4 . Toxicity assessments indicate reduced ecological risks of degradation intermediates and significant recovery of zooxanthellae density and coral–algal symbiosis. Immobilized catalyst architectures further minimize material loss and provide a suitable substrate for coral attachment. In this work, we demonstrate a seawater-stable, 1 O 2 -driven photocatalytic strategy that enables efficient BP-3 removal and promotes coral vitality recovery, thereby offering a scalable approach for marine environmental remediation and coral ecosystem restoration.
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JOURNAL OF ENVIRONMENTAL MANAGEMENT
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2026
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IF 9.2
Yan Wang,Xin Yang,Chen-Xuan Li,Wenhui Xu,Hong Mei,Feng Zhang,Zhuoya Gao,Yelei Liu,Kai Zhou,Houyun Yang,Kangping Cui
The coexistence of high-value pigment copper phthalocyanine (CuPc) and synthetic dyes in textile wastewater presents a dual challenge of environmental pollution and resource wastage. Herein, a novel singlet oxygen ( 1 O 2 )-dominated self-derived catalytic system was developed to simultaneously degrade rhodamine B (RhB) and recover valuable CuPc. Instead of requiring of the addition of external catalysts, wastewater-borne CuPc acted as an efficient heterogeneous activator for peroxymonosulfate (PMS). The system achieved 93.1% RhB removal within 30 min with an apparent rate constant of 0.089 min −1 , significantly outperforming the individual systems. Mechanistic studies combined with theoretical calculations revealed that the unique Cu-N 4 active sites facilitated PMS activation to generate 1 O 2 as the primary reactive oxygen species. This 1 O 2 -dominated pathway enabled the selective oxidation of electron-rich RhB while preserving the electron-deficient CuPc macrocycle, resulting in an over 80% recovery yield of CuPc. The system exhibited robust performance across a wide pH range (3.0-11.0) and in the presence of interfering anions. Moreover, the practical applicability of the system was further validated in simulated textile wastewater. This work provides a cost-effective, waste-derived catalytic strategy for complex textile wastewater treatment, promoting both pollution control and circular resource recovery.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2026
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IF 19.7
Zeyu Gong,Huajie Zhong,Linjing Tong,Jiaxing Yu,Yu Hou,Yuan Tao,Guosheng Chen,Junhui Wang,Gangfeng Ouyang
The catalytic activation of peroxymonosulfate (PMS) by covalent organic frameworks (COF) presents a promising advanced oxidation process (AOP) for water remediation. However, the influence of atomic-level linkage engineering on the PMS activation mechanism remains poorly understood. Here, we demonstrate that subtle manipulation of imine linkage orientation in two isomeric COF dictates their catalytic activity towards selectively generating singlet oxygen ( 1 O 2 ), a long-lived reactive oxygen species. We reveal that the spatial arrangement of the polar C N bond governs electronic structure and electron transfer behaviors by modulating intralayer coplanarity and the degree of electron delocalization across the COF skeleton. This structural control directly impacts the PMS adsorption and consequent 1 O 2 catalytic generation pathway, resulting in a 9.6-fold difference in the degradation rate constant for sulfamethoxazole (SMX, a cytotoxic antibiotic pollutant). The optimal COF catalyst achieves complete removal of SMX within 2 min, outperforming most state-of-the-art catalysts. This work elucidates the critical role of linkage orientation in COF-catalyzed PMS activation and providing new insights into the water remediation by 1 O 2 -mediated AOPs.
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FOOD MICROBIOLOGY
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2026
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IF 5.4
Jian Chen,Shiya Guo,Huan Li,Shigenobu Koseki,Jianhao Zhang,Xiaowei Sheng,Yanbo Wang
Dielectric barrier discharge (DBD) cold plasma combined with d -tryptophan ( d -Trp) exhibited a pronounced synergistic inactivation effect against Shewanella baltica , a dominant spoilage bacterium in aquatic products, and the underlying reactive oxygen species (ROS)-mediated mechanism was elucidated. 40 s combined treatment (DBD + d -Trp) achieved a 7.31 log CFU/mL reduction, markedly exceeding the 1.3 log reduction obtained with DBD treatment alone. Physicochemical analysis showed elevated hydrogen peroxide and nitrite levels accompanied by decreased pH in the synergistic system. Electron paramagnetic resonance and radical scavenging assays revealed that d -Trp selectively enhanced singlet oxygen ( 1 O 2 ) generation while suppressing hydroxyl radicals and superoxide anions, thereby reshaping the ROS profile compared to DBD treatment alone. Severe cellular damage was observed by scanning electron microscopy, and increased alkaline phosphatase release, potassium leakage, and membrane depolarization confirmed disruption of the cell envelope integrity. Elevated intracellular ROS accumulation and dysregulation of antioxidant enzyme activity indicated aggravated oxidative stress leading to bacterial death. The synergistic inactivation effect was further validated in fish juice, demonstrating superior efficacy compared to individual treatments. These findings demonstrate that d -Trp potentiates plasma inactivation through selective modulation of ROS composition and provide a mechanistic foundation for developing targeted control strategies against specific spoilage bacteria in aquatic products.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2026
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IF 9.1
Mengxin Liu,Pu Zhang,Boran Chen,Zhenyu Yang,Huinan Che,Yanhui Ao
Singlet oxygen ( 1 O 2 ) is promising for volatile organic compounds (VOC) removal in solar-driven interfacial evaporation (SDIE) systems, owing to its selectivity for electron-rich organic compounds and anti-interference capability. The radical precursor ·SO 5 − from peroxymonosulfate (PMS) is often strongly adsorbed and quenched on catalyst surfaces, impeding efficient 1 O 2 generation. To address this, we developed a bifunctional Co 3 O 4 /polyacrylamide hybrid hydrogel (Co 3 O 4 /PAMHH) evaporator, embedding Co 3 O 4 catalyst in a hydrophilic, hydrogen-bonding PAMHH network. This design precisely lowers the adsorption energy of ·SO 5 − on Co 3 O 4 surface to facilitate its desorption and enrichment within PAMHH pores, thereby establishing an optimal microenvironment for 1 O 2 formation. Scavenging experiments and ESR spectroscopy verified the directional production of 1 O 2 . With this design, Co 3 O 4 –0.2/PAMHH achieves stable phenol (PE) degradation across diverse pH and ionic conditions, achieving 90.4% PE removal in bulk water and 99.3% in condensed water with 2 mM PMS. Leveraging Co 3 O 4 's photothermal properties, an impressive evaporation rate of 3.40 kg m −2 h −1 was achieved under one sun irradiation. This work presents a novel microenvironment-regulated strategy that selectively directs PMS activation toward 1 O 2 , enabling simultaneous high-rate solar interfacial evaporation and efficient VOC removal. It establishes a new paradigm for precise control of reaction pathways in bifunctional solar-driven systems and offers a sustainable solution for integrated water purification and pollutant remediation.
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高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2025
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IF 6.3
Xinyu Wang,Tianren Li,Chunrui Zhao,Zian Fang,Mingyu Li
The selective conversion of peroxymonosulfate (PMS) to singlet oxygen ( 1 O 2 ) critically depends on precise electronic structure engineering of the catalysts. The PMS electron-donating pathway enables 1 O 2 generation, but the high energy barriers associated with the initial intermediate *SO 5 •− formation result in an unsatisfactory 1 O 2 yield. Herein, Co-doped ZnO was designed by calcination of zeolitic imidazolate framework. Co doping significantly improved the visible-light response, enhanced the photogenerated carrier separation and migration of ZnO, and increased the ZnO valence band potential. These effects promoted the electron-donating reaction of PMS to produce 1 O 2 . The optimized Co-ZnO-3/vis/PMS system exhibited a 27.2-fold higher methylene blue degradation rate constant (k = 0.9871 min⁻¹) with 43.7 % total organic carbon removal within 5 min. In addition, the developed 1 O 2 -dominated oxidation system removed 83.1 % of chromaticity, 59.9 % of total phenol, and 24.8 % of chemical oxidation demand from the coking wastewater tailwater. This work provides a pathway for tailoring 1 O 2 -dominated reactive species for contaminant removal, providing a theoretical guideline for the deep treatment of coking wastewater tailwater.
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
Surfaces and Interfaces
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2025
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IF 6.3
Dengping Zhang,XiangYu Zhang,Jing Hu,Wen Wang,Yuqing Lv,Xiao li Qian
Recent years, persulfate (PS) activation has mainly relied on metal ion activation, carbon materials, and their doped counterparts. However, traditional methods exhibit numerous limitations. Ionic liquids (ILs), due to their customizable nature, offer new potential for targeted non-radical catalysis. In this study, 1-butyl-3-methyl-1H-imidazol-3-ium bis((trifluoromethyl)sulfonyl) amide ([Bmim][Tf 2 N]) was used to enhance peroxydisulfate (PDS) activation for degrading oxytetracycline (OTC), achieving almost complete degradation in just 20 minutes. The mechanism revealed that the imidazole ring in the [Bmim][Tf 2 N] cation acts as an electron donor, promoting the cleavage of the O-O bond in the PDS and generating 1 O 2 . And, the iminium nitrogen in the anion acts as an electron acceptor, facilitating the breaking of the S-O bond in the PDS twice in succession, further producing 1 O 2 . This represents a successful application of ILs for PDS activation, providing new insights into designing efficient, targeted catalytic methods.
研究领域:
环境化学
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催化科学
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绿色化学
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高级氧化工艺
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离子液体应用
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高影响因子
危险品化学品经营许可证（带存储）