ENVIRONMENTAL RESEARCH
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2020
·
IF 5.715
Li Liu,Yunong Li,Wei Li,Ruixue Zhong,Yeqing Lan,Jing Guo
Co 3 O 4 –SnO 2 /rice straw biochar (RSBC) was prepared for the first time via calcining oxalate precipitation precursor dispersed on the surface of RSBC and used as a catalyst for activating PMS to degrade sulfisoxazole (SIZ). The results demonstrated that Co 3 O 4 –SnO 2 /RSBC possessed much better catalytic performance than Co 3 O 4 , Co 3 O 4 –SnO 2 , Co 3 O 4 /RSBC, and SnO 2 /RSBC, which is ascribed to the synergy of Co 3 O 4 , SnO 2 and RSBC. Approximately 98% of SIZ (50 mg/L) was decomposed by PMS (1 mmol/L) activated with Co 3 O 4 –SnO 2 /RSBC (0.1 g/L) within 5 min. The optimal degradation efficiency of SIZ was realized at the initial pH 9. Co 3 O 4 –SnO 2 /RSBC also displayed remarkable stability and reusability, and the degradation rate of SIZ maintained over 90% even after the fifth recycle run. The electron paramagnetic resonance (EPR) technique and quenching experiments proved singlet oxygen ( 1 O 2 ) to be the main reactive oxygen species (ROS) responsible for the SIZ decomposition in the Co 3 O 4 –SnO 2 /RSBC/PMS system. On the basis of the characterization analysis, the identification of the ROS and the SIZ degradation products , the possible mechanism and pathways of the SIZ degradation by a combination of PMS and Co 3 O 4 –SnO 2 /RSBC were further proposed. This study provides not only a new insight into non-radical mechanism for the heterogeneous activating PMS over Co 3 O 4 –SnO 2 /RSBC to degrade organic pollutants but also an eco-friendly synthetic route for exploring novel and efficient catalysts.
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PubMed
高影响因子
Redox Biology
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2020
·
IF 9.986
Lei Zeng,Meng-Di Wang,Sheng-Li Ming,Guo-Li Li,Peng-Wei Yu,Yan-Li Qi,Da-Wei Jiang,Guo-Yu Yang,Jiang Wang,Bei-Bei Chu
Emerging viral pathogens cause substantial morbidity and pose a severe threat to health worldwide. However, a universal antiviral strategy for producing safe and immunogenic inactivated vaccines is lacking. Here, we report an antiviral strategy using the novel singlet oxygen ( 1 O 2 )-generating agent LJ002 to inactivate enveloped viruses and provide effective protection against viral infection. Our results demonstrated that LJ002 efficiently generated 1 O 2 in solution and living cells. Nevertheless, LJ002 exhibited no signs of acute toxicity in vitro or in vivo . The 1 O 2 produced by LJ002 oxidized lipids in the viral envelope and consequently destroyed the viral membrane structure, thus inhibiting the viral and cell membrane fusion necessary for infection. Moreover, the 1 O 2 -based inactivated pseudorabies virus (PRV) vaccine had no effect on the content of the viral surface proteins. Immunization of mice with LJ002-inactiviated PRV vaccine harboring comparable antigen induced more neutralizing antibody responses and efficient protection against PRV infection than conventional formalin-inactivated vaccine. Additionally, LJ002 inactivated a broad spectrum of enveloped viruses. Together, our results may provide a new paradigm of using broad-spectrum, highly effective inactivants functioning through 1 O 2 -mediated lipid oxidation for developing antivirals that target the viral membrane fusion process.
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PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2019
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IF 8.456
Bao-Cheng Huang,Gui-Xiang Huang,Jun Jiang,Wu-Jun Liu,Han-Qing Yu
Carbon-based materials are recognized as promising candidates for pollutant degradation because of their environmental benignity. Massive and cost-effective production and efficient recovery of carbon-based catalysts are crucial to apply this technology. However, various nanostructured carbons with different dimensions are usually utilized as precursors while not considering their complex preparation procedures and the high costs of ingredients. Moreover, catalyst separation and recovery are not given sufficient attention. In this work, a calcium salt-assisted pyrolysis strategy is proposed to tune the catalytic site formation of carbon-based catalysts. Results show that blending equal amounts of Ca2+ (calcium chloride) and organic precursors could greatly improve the catalytic activity of the carbonated product to activate peroxymonosulfate for pollutant degradation. In addition, the proposed synthetic strategy is universal to most of the readily accessed and cost-effective organic precursors. Singlet oxygen is identified as the main reactive oxidant for pollutant removal in the catalytic reaction. By cross-linking calcium ions and alginate as a hydrogel to immobilize the catalyst, the carbon material could be readily recovered. Furthermore, a long-term continuous-flow reactor test is conducted to validate the effectiveness of applying the immobilized catalyst to treat a synthetic wastewater with 0.5 mM bisphenol A. As a result, a green synthesis and immobilization strategy for persulfate catalysts is successfully established, and the prepared catalyst might be applied for wastewater treatment through using calcium salt in two purposes.
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高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2019
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IF 7.65
Qihui Zhang,Dan He,Xinran Li,Wei Feng,Cong Lyu,Yifeng Zhang
Peroxymonosulfate (PMS) has gained attention as oxidant for SR-AOPs. It is essential to develop a stable heterogeneous catalyst with strong hydrophilicity and high electron transfer capability for PMS activating. In this study, cobalt oxyhydroxide (CoOOH) was synthesized and activated PMS for degradation of 2,4-dichlorophenol (2,4-DCP) aiming to assess the feasibility of CoOOH/PMS system. 50 mg/L of 2,4-DCP could be 100% degraded within 120 min with 0.20 g/L CoOOH and 6 mM PMS. CoOOH/PMS system possessed a high degradation efficiency (0.0462 min −1 ), which was about 10 and 4 times higher than Co 3 O 4 /PMS and CoFe 2 O 4 /PMS system, respectively. Furthermore, it was found that CoOOH/PMS system displayed effective catalytic performance over broad pH range (e.g. 3–9). Importantly, the quenching tests revealed that 1 O 2 was identified as dominant reactive oxygen species (ROS). Co (Ⅲ) was rapidly reduced to Co (Ⅱ) owing to the efficient electron transfer rate performance of CoOOH in the catalytic reaction. Then, the regeneration of Co (Ⅱ) facilitated CoOH + owing to the surface of CoOOH with sufficient hydroxyl group, which is crucial for PMS activation and reactive oxygen species-ROS generation. This study proposed an alternative technology based on peroxymonosulfate catalyzed by cobalt-based hydroxide for waste water treatment.
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高影响因子
Journal of Materials Chemistry B
·
2020
·Vol. 8
·期 7
·1371-1382
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IF 5.344
Yunjian Yu,Lin Mei,Yanmei Shi,Xinge Zhang,Kesong Cheng,Fengyi Cao,Liuxue Zhang,Jia Xu,Xiumin Li,Zhenlong Xu
The increasing prevalence of antibiotic resistance highlights the need for new antibacterial drugs and, in particular, the development of alternative approaches such as photodynamic therapy (PDT) and photothermal therapy (PTT) to manage this growing issue. In the present study, a broad-spectrum antibacterial system was produced in which Ag nanoparticle-conjugated graphene quantum dots (GQD–AgNP) were utilised as a blue light-enhanced nanotherapeutic for efficient ternary-mode antimicrobial therapy. The successful conjugation of AgNPs onto the surface of GQDs can significantly improve the production of reactive oxygen species in light-activatable GQDs and the transformation of light energy to hyperthermia with high efficiency. There was a remarkable increase in the sample temperature of nearly 40 °C via photoexcitation after only 10 min of 450 nm laser exposure (14.2 mW cm−2). The hybrids exhibited much more efficient bactericidal capability against both Gram-negative and Gram-positive bacteria compared with GQDs alone, using 450 nm light irradiation. This is likely a consequence of their enhanced PDT, concomitant PTT, and the synergistic function of AgNPs. The antibacterial mechanism of the new-style nanocomposites was found to irreversibly destroy the bacterial membrane structure, leading to the leaking out of the cytoplasmic contents and the death of the bacteria. At low doses, the biocompatible GQD–AgNP hybrids promoted healing in bacteria-infected rat wounds, with negligible adverse impact to the normal tissue, indicating a promising future for combined photodynamic and photothermal antibacterial applications in clinical medicine.
研究领域:
纳米技术
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抗菌治疗
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光疗
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材料科学
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生物医学工程
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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2026
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IF 19.7
Yunlong Wang,Xin Guo,Kechen Gu,Chengming Xiao,Wenbo Yang,Chuyan Deng,Junwen Qi,Yujun Zhou,Zhigao Zhu,Yue Yang,Jiansheng Li
Spatial confinement switches non-radical pathways from ETP to a ¹O₂-dominant mechanism. • A 2D CoO@MX/GO membrane creates confined nanochannels for this transition. • Pathway shift confirmed by EPR, fluorescence, and DFT calculations. • Membrane achieves 10,000 × faster degradation kinetics than powder catalysts. • Size exclusion/confined oxidation resist NOM/ions for stable single-pass removal. Spatial confinement within a lamellar catalytic membrane is demonstrated to switch non-radical peroxymonosulfate activation from an electron-transfer process (ETP) to a singlet-oxygen ( 1 O 2 )-dominated pathway. This was achieved by intercalating cobalt oxide-decorated MXene nanosheets (CoO@MX) into graphene oxide (GO) laminates to construct a two-dimensional confined catalytic membrane. The membrane enabled four-orders-of-magnitude faster degradation of phenolic compounds than powder catalysts, with apparent rate constants of 0.093–0.127 ms –1 , achieved complete sulfamethoxazole removal within an ultrashort hydraulic residence time of 68 ms, retained approximately 95% removal under humic-acid interference, and maintained 100% removal efficiency over 50 h of continuous operation. The pathway transition toward singlet-oxygen-dominated oxidation, confirmed by electron paramagnetic resonance, in situ fluorescence, and density functional theory calculations, mitigates catalyst fouling and facilitates pollutant mineralization. This work provides a nanoconfinement strategy for steering non-radical oxidation pathways and offers a design principle for efficient, selective, and durable advanced oxidation systems for complex water treatment. Download: Download high-res image (181KB) Download: Download full-size image
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CHEMICAL ENGINEERING SCIENCE
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2026
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IF 5.1
Shangyi Zhao,Jing Li,Yanchanjuan Yang,Shuaiqi Zhao,Aihua Xu,Xiuying Liu,Xiaoxia Li
Sulfite (SO 3 2− ) has emerged as an economical and eco-friendly precursor for reactive species generation in advanced oxidation processes (AOPs). However, conventional activation strategies typically require high sulfite inputs and generate non-selective radicals, limiting their efficiency and practicality. Here, we demonstrate that a trace amount of water‑soluble manganese porphyrin complex (Mn(III)‑TCPP, as low as 4 μM), can efficiently activate Na 2 SO 3 at ultralow concentrations (10–100 μM) to degrade sulfadiazine. The Mn(III)-TCPP/Na 2 SO 3 system exhibited an initial rate 41 times faster than the Mn 2+ /Na 2 SO 3 system and 4.2 times greater than the reported -Mn(III)-NTA/Na 2 SO 3 system. A linear correlation between the degradation rate constant and the Hammett constant (σ + ) of porphyrin substituents confirms that ligand electronic structure modulates Mn redox cycling during SO 3 2− oxidation by dissolved O 2 . Mechanistic studies, including time‑resolved spectroscopy, electrochemical analysis, and reactive species trapping, reveal that the reaction proceeds primarily via superoxide radical and singlet oxygen, representing a distinct departure from conventional sulfate radical or high-valent Mn(V) that has been reported in other metal–ligand AOP systems. This work establishes a new, highly efficient sulfite activation driven by an ultralow-dose metalloporphyrin catalyst and provides fundamental insight into non‑radical oxidation routes for sulfite-based AOPs.
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高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2026
·
IF 5.4
Shenfei Li,Huihui Peng,Xiaoqiang An,Huachun Lan,Xuelian Yu
Nonradical oxidation via peroxymonosulfate (PMS) activation has attracted considerable attention for organic pollutant degradation, while the control and regulation of singlet oxygen ( 1 O 2 ) generation in catalytic oxidation are still challenging and the underlying mechanism remains ambiguous. In this paper, we synthesized a nitrogen-doped carbon-supported manganese-based catalyst by using ZIF-8 as a metal-organic framework (MOF) template for the in-situ loading of active components. When used for peroxymonosulfate activation, the MnO-Mn 6 N 2.58 /N-C catalyst exhibits a high Bisphenol A (BPA) degradation rate of 0.133 min -1 , exceeding PMS oxidation alone by 67 times. Mechanistic investigations reveal that the degradation process relies on the direct electron transfer from heterogeneous catalysts to PMS, contributing to efficient 1 O 2 generation for BPA degradation via a nonradical pathway. We demonstrate that Mn(II)/Mn(III) redox cycling on the catalyst surface activates PMS into superoxide (O 2 • - ), which in turn converts into 1 O 2 , thereby elucidating the underlying mechanism for high-efficiency degradation. This work provides a novel strategy to design heterogeneous Mn-based catalysts for recalcitrant organic wastewater remediation via a nonradical oxidation pathway.
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高影响因子
Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Jinli Qiu,Yao Feng,Zhiqin Luo,Xinying Chu,Xiaoxue Pan,Fuqiang Liu
Heterogeneous Electro-Fenton (HEF) technology, which requires only oxygen and electric energy, holds significant potential for organic wastewater treatment due to its high efficiency. In this study, an iron-carbon composite cathode catalyst (Fe 3 C/BC) featuring highly dispersed Fe 3 C active sites on biochar (BC) was designed and synthesized to degrade nitenpyram (NTP), a representative neonicotinoid pesticide. The optimized Fe 3 C/BC-HEF system exhibited remarkable catalytic activity for NTP degradation, along with strong pH tolerance (3.0–9.0) and adaptability to various water matrices. This excellent performance can be attributed not only to its enhanced H 2 O 2 generation capability but also to the obviously faster H 2 O 2 activation efficiency to produce reactive oxygen species (ROS) for NTP degradation. Reactive species quenching experiments and electron paramagnetic resonance (EPR) spectroscopy confirmed that singlet oxygen (¹O 2 ) was the dominant reactive species responsible for NTP degradation. Furthermore, combined with HPLC-MS/MS analysis and Fukui index calculation, the intermediate products and degradation pathway of NTP were verified. The excellent reusability and stability of the cathode could be due to the protective role of BC, which minimized direct contact between Fe₃C active sites and the reaction solution, and thus reducing Fe 3 C corrosion during the HEF process. This study offers important insights into the design of superior metal-carbon hybrid cathode for electrochemical water remediation technologies.
研究领域:
环境科学
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电化学工程
·
农药污染治理
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2025
·
IF 13.2
Wei Li,Qing Li,Liangliang Zhu,Su Chen
Global plastic production, particularly polyethylene terephthalate (PET), has surged in modern society, yet conventional disposal methods like incineration and landfills pose severe environmental risks. Photothermal catalysis emerges as a sustainable solution, combining photo with thermal catalysis processes to reduce energy consumption while enhancing catalytic efficiency. Herein, we demonstrate a promising approach employing black phosphorus nanosheets (BPNSs) featuring exceptional photothermal conversion and singlet oxygen ( 1 O 2 ) generation to photothermally accelerate PET depolymerization. Integrating with Fe 3 O 4 nanoparticles, the formed covalent P-O bonds shield reactive phosphorus atoms in BPNSs from oxidation to improve their stability, and Fe 3 O 4 enables magnetic recovery and synergy with PET's carbonyl groups. Under solar irradiation, the BPNSs-Fe 3 O 4 composite achieves 98.3 % PET conversion and 95.2 % bis(2-hydroxyethyl) terephthalate (BHET) yield at 185 °C in ethylene glycol, 2.8-fold and 6.5-fold higher than traditional thermal catalysis, respectively. Mechanistic studies reveal that localized photothermal heating and 1 O 2 -driven nucleophilic elimination of ester groups collaboratively enhance the reaction kinetics, reducing the activation energy by 53.7 %. Successful outdoor validation and BHET repolymerization confirm the practicability. This closed-loop photothermal strategy demonstrates excellent efficiency and product quality, offering a viable pathway toward sustainable plastic upcycling with dual environmental and economic potentials.
研究领域:
材料科学
·
环境科学
·
化学工程
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能源科学
·
可持续发展技术
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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Yandong Sun,Weiguang Han,Fangyuan Zhang,Hui Li,Ziqi Zhang,Xue Zhang,Boxiong Shen,Sheng-Qi Guo,Tianyi Ma
The generation of singlet oxygen ( 1 O 2 ) based on photocatalytic activation O 2 is considered to have important application prospects in purifying refractory organic pollutants in water. However, the uncertain dual pathway transformation of activated O 2 severely limits the generation of 1 O 2 . In this work, we show a robust BiOCl with dual defects (adjacent I-substitution defect and Cl vacancy) in halogen layer for the selective activation of O 2 to generate 1 O 2 . Combining experiments and theoretical calculations, we confirm that dual defects are beneficial in optimizing band structures, improving carrier separation efficiency, and promoting O 2 adsorption and activation. More importantly, it is confirmed that dual defects can directionally convert O 2 into 1 O 2 by increasing the thermodynamic conversion energy barrier of non- 1 O 2 conversion pathways and serving as a necessary site for 1 O 2 generation with dual functions of oxidation and reduction. Applying dual defect modified BiOCl to the removal of refractory aromatic pollutants in water, it is found that it has efficient and stable photocatalytic degradation efficiency and broad environmental adaptability. This work not only provides in-depth insights into the mechanism of photocatalytic activation of O 2 to selective produce 1 O 2 , but also lays the foundation for further development of highly active photocatalysts for environmental remediation and energy conversion.
研究领域:
环境科学
·
材料科学
·
化学
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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Chuanshun Feng,Shuo Chen,Linjie Guan,Guoen Zhang,Feng Lin,Qicheng Zhang,Xiaobin Fan,Wenchao Peng,Yang Li
A metal-free carbon catalyst co-doped with boron and silicon (2B-BCSi) is designed and synthesized in this work. Its custom-engineered internal electric field achieves the barrier-free and selective generation of singlet oxygen ( 1 O 2 ). Guided by theoretical analysis and density functional theory (DFT) calculations, low‑electronegativity heteroatoms were incorporated into the carbon scaffold to an adjacent electric‑field configuration (B δ+ -C-Si δ+ ). By generating an internal electric field-induced molecular tension and leveraging boron-moderated charge transfer, the system circumvents the adsorption constraints of terminal oxygen that limits traditional approaches. Thereby, it facilitates 1 O 2 production from PMS via a novel barrier-free pathway, resulting in unprecedented selectivity for 1 O 2 (>93.6 %). This system demonstrates significant advantages in electron-rich pollutant degradation (0.437 min −1 ) and organic synthesis (242.8 mg h −1 L −1 ), establishing an electric-field engineering paradigm for precise ROS control while providing dual-path solutions for environmental remediation and value-added chemical production.
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