CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Ruonan Guo,Zenghui Bi,Beidou Xi,Changsheng Guo,Heng Zhang,Ningqing Lv,Guangzhi Hu,Jian Xu
The function of heterogeneous catalyst in singlet oxygen ( 1 O 2 ) generation under acidic and neutral conditions and the effect of sulfate radical on the generation of 1 O 2 is still unclear. This study provided a novel generation pathway of 1 O 2 in the heterogeneous Mn single − atom catalyst (Mn SAC)/peroxymonosulfate (PMS) system. The MnN4 site with the ideal binding strength promoted the activation of PMS to generate sulfate radical (SO 4 •– ), which would be adsorbed on the carbon/nitrogen sites forming SO 4 •– (s) , reacting spontaneously to produce 1 O 2 . The presence of MnN4 and carbon/nitrogen structure sites could shift the oxidation process from a bulk–phase oxidation to a surface oxidation. This shift has important implications in terms of reaction rate and product distribution, as the dual reaction sites decrease the required migration distance for the active species to form 1 O 2 , avoiding the pointless consumption of active substances.
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CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Zhiang Hou,Jinzhu Yue,Hao Chen,Jinnan Wang,Aimin Li,Philippe François-Xavier Corvini
Endocrine disrupting chemicals (EDCs) interfere with the normal secretion, transport and metabolism of human hormones, thus affecting neurological, reproductive and immune functions. Photocatalysis is regarded as a facile organic degradation technique. The construction of heterojunctions can modulate the reactive oxygen species and enhance the photocatalytic performance of semiconductors. However, poor contact interfaces still severely limit carrier separation and transfer. Herein, we have doped Co to modulate the band structure of Bi 2 O 2 CO 3 while facilitating the in situ growth of BiOI on its surface via shared Bi atoms. This approach led to the development of a 2D/2D Co-Bi 2 O 2 CO 3 /BiOI (Co-BOC/BiOI) S-scheme heterojunction characterized by atomically close contact interfaces. Furthermore, the photo-electrochemical characterization results indicate that the light adsorption capacity, carrier separation and transport efficiency of the optimized Co-BOC/BiOI-3 are greatly improved. This system demonstrates almost 100% removal rate for three typical EDCs within 60 min. The degradation kinetic constants show an improvement by an order of magnitude compared to single BiOI and Bi 2 O 2 CO 3 . More importantly, O 2 •﹣ , which is produced from O 2 reduction on high negative conduction band, can be subsequently oxidized into 1 O 2 by photogenerated hole. Electron paramagnetic resonance and quenching experiments indicate that the organics degradation process is dominated by 1 O 2 . This work offers new insights into the construction of high-quality S-scheme heterojunction interfaces for modulation of reactive oxygen species.
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Advanced Fiber Materials
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2025
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IF 21.3
Zhang Luyao,Wang Li,Chen Junliang,Li Jinzhou,Huang Peng,Nie Xinming,Yang Jianping
Due to the shortage of rational waste management, plastic waste has become increasingly serious, posing a serious threat to the environment and humans. The catalytic oxidation of polyethylene terephthalate (PET) waste has been reported to reduce environmental stress and produce valuable products. However, obtaining valuable chemicals from waste plastics under mild conditions driven by specific reactive oxygen species is a great challenge. Herein, N, P-doped Mo 2 C@porous carbon was designed and employed in the peroxymonosulfate-based advanced oxidation reforming of PET hydrolysate. The ethylene glycol (EG) derived from PET fiber was catalytically oxidized to formate via singlet oxygen activation during the peroxymonosulfate-based advanced oxidation process. Compared with Mo 2 C, the N, P-doped Mo 2 C@porous carbon catalyst with a large specific surface area provides more active sites, which has the characteristic of high catalytic activity. It presents the tetracycline degradation efficiency of ~ 80% under a wide pH range (6.8–10.6) and, further, the formate generation rate of ~ 56.5 mmol g cat −1 in the advanced oxidation reforming process of EG in 8 h. The detection and quenching experiments on the oxygen active species comprehensively confirmed that singlet oxygen is the key reactive oxygen species during the advanced catalytic oxidation reactions. This work provided a constructive demonstration for designing advanced oxidation catalysts to catalyze the reforming of waste PET fiber plastics into valuable chemicals. Graphical The catalytic reforming of polyethylene terephthalate (PET) waste and proper treatment of fiber-based microplastics have emerged as critical areas of research and innovation to alleviate environmental stress and generate valuable products. This work sheds light on the efficient Mo 2 C@porous C catalyst design via singlet oxygen activation for persulfate-based advanced oxidation reforming of EG from PET fiber waste, providing a potential countermeasure to address plastic waste pollution and achieve carbon neutrality
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SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Peng Jin,Niao Fu,Ruining Bai,Qingzhi Liu,Yujiao Liu,Mei Chen,Jieli He
Eutrophication-driven cyanobacterial blooms release microcystin-LR (MC-LR), a potent hepatotoxin, posing severe environmental and public health risks. Effective, safe MC-LR degradation is critical for water remediation. Herein, we propose a rationally designed unique donor–acceptor–acceptor (D-A1-A2) structural strategy to synthesize a covalent organic framework (COF-TFP-TAPT-Me) for visible-light-driven, controllable 1 O₂-mediated MC-LR photocatalysis. Structural/optoelectronic characterization confirmed triazine-based A2 (Melem) incorporation narrowed the parent D-A1 COF's band gap to 1.15 eV (vs. 1.38 eV) and enhanced charge separation via forming continuous π-conjugation, ordered π-π stacking, and a multi-level energy structure that promotes directional electron transfer (1.6-fold higher photocurrent than the parent COF). COF-TFP-TAPT-Me nearly completely degraded MC-LR in 25 min, with a pseudo-first-order rate constant 1.66-fold higher than the parent COF and outperforming benchmarks like P25 and PCN. Mechanistically, its D-A1-A2 configuration effectively enables highly selective and dominant 1 O₂ generation in metal-free COFs (in contrast to mixed ROS in the parent COF) via photosensitized energy transfer, selectively attacking MC-LR's Adda chain (UPLC–MS verified). The catalyst retains >95 % activity after 5 cycles, is stable in natural water, and shows >80 % cell viability in cytotoxicity assays. This work highlights a novel D-A1-A2 framework for regulating 1 O₂-dominated degradation, offering a trinity of high efficiency, stability, and low toxicity strategy for water purification.
研究领域:
环境科学
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材料化学
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光催化
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水处理
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有机框架
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ORGANIC & BIOMOLECULAR CHEMISTRY
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2019
·Vol. 17
·期 34
·8001-8007
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IF 3.49
Chengjun Wang,Ying Qian
A novel photosensitizer BDPI-lyso has been developed for photodynamic therapy (PDT). The photosensitizer BDPI-lyso showed a high singlet oxygen quantum yield (ΦΔ = 0.95) and low fluorescence quantum yield (ΦF = 0.05) in EtOH. Different singlet oxygen quantum yields were found in acidic solution (pH = 5, ΦΔ = 0.51) and in neutral solution (pH = 7, ΦΔ = 0.38). DFT and TD-DFT calculations of BDPI-lyso and its protonated product BDPI-lysoH+ indicated that the S1/T3 transition was responsible for the intersystem crossing (ISC) enhancement which would promote the production of singlet oxygen. The negligible dark cytotoxicity toward the hepatoma cell line Bel-7402 was confirmed by MTT assay, AO/EB dual staining, and cell images. Upon exposure to a low dose of light illumination, the disruption of the cell plasma membrane and the calculated half-maximal inhibitory concentration (IC50) of 0.4 μM showed a high phototoxicity of the photosensitizer BDPI-lyso. The light-induced intracellular ROS generation was verified as the PDT mechanism of BDPI-lyso. Colocalization experiments of LysoTracker Green and BDPI-lyso in the dark indicated the good lysosome-targeting ability of BDPI-lyso. The images of cells costained with LysoTracker Green and BDPI-lyso, and the appearance of intracellular and extracellular blebs with green fluorescence after light illumination revealed the light-induced dysfunction of lysosomes and cell apoptosis.
研究领域:
生物化学
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医学
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药物化学
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Frontiers of Environmental Science & Engineering
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2020
·Vol. 15
·期 4
·1-11
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IF 4.053
Xi Tianhao,Li Xiaodan,Zhang Qihui,Liu Ning,Niu Shu,Dong Zhaojun,Lyu Cong
Cobalt oxyhydroxide (CoOOH) has been turned out to be a high-efficiency catalyst for peroxymonosulfate (PMS) activation. In this study, CoOOH was loaded on bismuth oxide (Bi 2 O 3 ) using a facile chemical precipitation process to improve its catalytic activity and stability. The result showed that the catalytic performance on the 2,4-dichlorophenol (2,4-DCP) degradation was significantly enhanced with only 11 wt% Bi 2 O 3 loading. The degradation rate in the CoOOH@Bi 2 O 3 /PMS system (0.2011 min −1 ) was nearly 6.0 times higher than that in the CoOOH/PMS system (0.0337 min −1 ). Furthermore, CoOOH@Bi 2 O 3 displayed better stability with less Co ions leaching (16.4% lower than CoOOH) in the PMS system. These phenomena were attributed to the Bi 2 O 3 loading which significantly increased the conductivity and specific surface area of the CoOOH@Bi 2 O 3 composite. Faster electron transfer facilitated the redox reaction of Co (III) / Co (II) and thus was more favorable for reactive oxygen species (ROS) generation. Meanwhile, larger specific surface area furnished more active sites for PMS activation. More importantly, there were both non-radical ( 1 O 2 ) and radicals (SO 4 − •, O 2 − •, and OH•) in the CoOOH@Bi 2 O 3 /PMS system and 1 O 2 was the dominant one. In general, this study provided a simple and practical strategy to enhance the catalytic activity and stability of cobalt oxyhydroxide in the PMS system.
研究领域:
环境科学
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催化化学
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JOURNAL OF NANOBIOTECHNOLOGY
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2026
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IF 12.6
Hao Zhang,Xiaoyu Song,Leilei Zhao,Chenlong Wang,Shen Chen,Yinghui Wang,Li Zhang,Fangyi Xu,Hongjie Zhang,Qilong Wang,Chao Luo
Photodynamic therapy (PDT) holds significant potential for tumor treatment, yet its immunotherapeutic efficacy is severely constrained by the immunosuppressive tumor microenvironment (TME) marked by lactate accumulation, hypoxia, and glutathione (GSH) overexpression. To overcome these limitations, we engineered an injectable hydrogel system (FPH@A/C) that synergistically integrates oxygen-independent PDT, ferroptosis activation, and lactate metabolic reprogramming to remodel immunosuppressive TME and potentiate antitumor immunity. The hydrogel comprises singlet oxygen-preloaded iron-based nanoparticles (FPH), lithium carbonate (LC), and sodium alginate (ALG), rapidly crosslinking into a stable matrix when encountering physiological Ca²⁺ concentration for localized therapeutic delivery. Within TME, GSH-triggered FPH degradation releases Fe²⁺ and pre-stored singlet oxygen, enabling chemodynamic therapy (CDT) and photo-independent PDT to induce tumor ferroptosis. Simultaneously, LC reprograms lactate-a metabolic byproduct-into an energy substrate for CD8⁺ T cells, counteracting lactate-driven immunosuppression. Notably, combining FPH@A/C with immune checkpoint blockade (ICB) therapy demonstrates synergistic effects, robustly enhancing dendritic cell maturation and cytotoxic T lymphocyte infiltration. This multifunctional platform establishes a novel paradigm for colorectal cancer immunotherapy by concurrently addressing metabolic constraints and immune evasion mechanisms.
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PROCESS SAFETY AND ENVIRONMENTAL PROTECTION
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2026
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IF 7.8
Huanxuan Li,Chen Liu,Tao Rao,Zhong Zhou,Zhitong Yao,Wei Han,Jingang Huang,Shaodan Xu,Xiuyan Liu
Developing stable and efficient catalysts for peroxymonosulfate (PMS) activation is of critical significance for the remediation of antibiotic-contaminated wastewater, as conventional catalytic systems often suffer from insufficient activity, poor stability, or a narrow pH adaptation range. Herein, sulfur-doped metal-organic framework (MOF)-derived catalysts (Co-BDC@S) were successfully synthesized via a one-step pyrolysis of cobalt(II) 1,4-benzenedicarboxylate (Co-BDC) and sulfur powder. Systematic optimization of the synthesis parameters revealed that the Co-BDC@S-700–4 catalyst (where the subscripts "700" and "4" denote the calcination temperature and sulfur doping amount, respectively) exhibits superior PMS activation performance. Specifically, it achieves 97 % removal of ciprofloxacin (CIP, 20 mg/L) within 30 min, accompanied by an ultrahigh initial apparent rate constant of 0.268 min⁻¹ . The system has excellent pH tolerance (3–10) and maintains > 73 % efficiency after 5 cycles (Co leaching <1.0 mg/L), meeting wastewater discharge standards. Mechanistic studies confirm singlet oxygen (¹O₂) as the dominant reactive species, whose high steady-state concentration (5.24 ×10⁻¹² M) is attributed to the synergistic effect of Co₄S₃ and sulfur vacancies facilitating electron transfer and non-radical pathways. Furthermore, ultra-performance Liquid Chromatography Triple Time-of-Flight Mass Spectrometry (UPLC-Triple-TOF/MS) identified 22 transformation intermediates during CIP degradation, and ecological toxicity assessment via the ECOSAR model confirms their significantly reduced environmental risks. This work provides a stable, eco-friendly catalyst and valuable mechanistic insights for designing advanced oxidation systems.
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Journal of Environmental Sciences
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2026
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IF 6.3
Lihui Zhao,Can Jin,He Liu,Zhaozhe Yang,Yupeng Liu
Bisphenol A (BPA), a widespread endocrine-disrupting compound, necessitates efficient activation of peroxymonosulfate (PMS) for its degradation. Conventional carbon-based catalysts frequently exhibit limited efficiency, poor stability, and potential environmental risks. Bamboo-derived porous carbon material (BCM) and bamboo-derived porous carbon material loaded with Fe (BCM-Fe) serve as effective catalysts for activating PMS to degrade BPA. The BCM/PMS system achieved a BPA removal efficiency of 94.44 % within 150 minutes, while the BCM-Fe/PMS system attained 97.8 %. Quenching experiments and electron paramagnetic resonance (EPR) analysis identified non-radical singlet oxygen (¹O₂) as the dominant reactive species. Density functional theory (DFT) calculations demonstrated that atomically dispersed Fe species on BCM-Fe significantly enhanced PMS adsorption energy and activation kinetics compared to BCM. Both catalysts exhibited excellent reusability, confirming their potential as practical and sustainable catalysts. This study provides fundamental insights for designing efficient, environmentally benign carbon-based catalysts for advanced oxidation processes.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2026
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IF 9.6
Yulu Zhang,Huali Yu,Peike Cao,Xuning Li,Shifu Wang,Huangzhao Wei,Haiyan Guo,Lianfeng Wang
Spin state regulation has emerged as a promising strategy to enhance the catalytic performance of transition-metal catalysts in peroxymonosulfate (PMS) activation. Herein, boron doping and facet engineering were synergistically applied to regulate the spin state of hematite, yielding B-doped hematite nanorods (B-HNRs) and nanocubes (B-HNCs) with highly efficient PMS activation and abundant 1 O 2 production. X-ray absorption near-edge structure (XANES) and 57 Fe Mössbauer spectra analysis revealed that the boron incorporation resulted in the formation of high spin (HS) Fe(II) species with smaller crystal field splitting energy compared to Fe(III). Density functional theory (DFT) calculations revealed that boron doping enhanced the overlap between Fe 3 d orbitals and O 2 p orbitals of PMS molecules, thereby facilitating electron transfer between PMS and Fe centers. Compared with B-HNCs, B-HNRs possessing more HS Fe(II) exhibited stronger PMS adsorption, greater O O bond activation, and consequently achieved higher 1 O 2 selectivity (91.6%) and superior catalytic performance. The generated 1 O 2 displayed strong resistance to common aqueous interferences and enabled selective pollutant oxidation. Furthermore, the successful continuous-flow reactor operation demonstrated its practical application potential. This work not only offers an innovative approach for the rational modification of transition-metal catalysts but also deepens the mechanistic understanding of PMS activation at the atomic level. Download: Download high-res image (151KB) Download: Download full-size image
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JOURNAL OF HAZARDOUS MATERIALS
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2026
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IF 10.6
Lan Li,Hui Chen,Yuheng Chen,Baiyang Chen
Singlet oxygen ( 1 O 2 ) is a key reactive species in environmental, chemical, and biological systems. For decades, furfuryl alcohol (FFA) has been used as a probe for quantifying 1 O 2 based on the assumption that it reacts selectively with 1 O 2 but is inert toward other oxidants. However, we demonstrate that this assumption is fundamentally flawed in the chlorine-hydrogen peroxide (H 2 O 2 ) system-one of the most common contexts for 1 O 2 generation. Results demonstrate that chlorine alone can degrade FFA significantly, implying that previous studies may have systematically overestimated 1 O 2 yields. Specifically, raising pH facilitated the decay of chlorine but hindered FFA degradation, suggesting that 1 O 2 formation is unfavorable under alkaline conditions. Increasing the dosage of chlorine enhanced FFA degradation, but decreased the relative contribution of 1 O 2 to FFA degradation. More strangely, increasing the FFA dosage unexpectedly reduced the kinetics of FFA degradation, implying that the concentration of 1 O 2 was not constant under fixed chlorine-H 2 O 2 condition. Maintaining low dissolved oxygen enhanced FFA decay, suggesting that superoxide is not an intermediate for 1 O 2 formation. Furthermore, pyranone was not formed during FFA degradation processes, invalidating it as a characteristic product. These evidences together challenge the accountability regarding FFA selectivity, pyranone formation, and 1 O 2 formation mechanisms before using FFA for 1 O 2 quantification in chlorine-involved systems.
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Journal of Environmental Chemical Engineering
·
2026
·Vol. 14
·期 3
·122789
·
IF 7.5
Dancheng Zhu,Caiyun Zhang,Jiabin Shen,Chao Shen,Chuanhong Jin,Hao Xu
Sulfamethoxazole (SMX), a widely used sulfonamide antibiotic, is a persistent aquatic pollutant due to its resistance to conventional treatment. Here, a Cu-ZSM-5/Ti 3 C 2 composite catalyst was fabricated by electrostatic self-assembly for peroxymonosulfate (PMS) activation. Characterization by XRD, SEM, TEM, XPS, and zeta potential analysis confirmed the successful integration of the components. The catalyst achieved 97.59% removal of 10 mg/L SMX within 30 min. Quenching and EPR results indicated that 1 O 2 was the major reactive species. The enhanced performance under alkaline conditions was associated with the negatively charged composite surface (-38.8 mV at pH 9), the deprotonated state of SMX, and favorable interfacial interactions that may promote preferential oxidation of the isoxazole moiety. Control experiments using a physically mixed sample showed markedly lower activity, especially at pH 11, highlighting the importance of the intimate heterointerface created by self-assembly. The superior activity was attributed to the synergistic interaction between Cu species in Cu-ZSM-5 and Ti-based sites in Ti 3 C 2 . This work provides insight into designing selective PMS activation catalysts for antibiotic-contaminated water treatment.
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