MATERIALS LETTERS
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2021
·
IF 3.423
Wenbo Liu,Jiabin Zhou,Dan Liu,Su Liu,Xianjie Liu
Accelerating electron transfer can improve the catalytic performance. MIL-88/Go composites were synthesized by hydrothermal method using the oxygen-containing functional group of graphene oxide (GO) as the MIL-88 unit cell nucleus. Fe 2 O 3 /rGO composites with small particle size were prepared by roasting of MIL-88/GO. It has high degradation efficiency (99%) and good recycling performance for tetracycline hydrochloride (TC-HCl) in photo-Fenton system. The combination of oxygen vacancies produced by roasting MIL-88 and the conductivity of reduced graphene oxide (rGO) improves the rate of electron transfer. The efficient electron transfer promotes the formation of OH and O 2 − and thus improve the catalytic activity.
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
APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
·
IF 24.319
Xinliang Liu,Jilong Mo,Wanhai Wu,Hainong Song,Shuangxi Nie
The generation of free radicals was enhanced by triboelectric pulsed direct-current during the organic pollutant degradation. The self-powered electrochemical system was constructed for enhancing 4-CP removal powered by a water-driven triboelectric nanogenerator (WD-TENG). The output of current, voltage, and power of WD-TENG were studied. The removal of 4-CP and its degradation mechanism were also discussed. The results shows that the formation of hydroxyl radicals (·OH) was improved by improving PMA(Mo 5+ ) conversion efficiency by the WD-TENG in the phosphomolybdic acid/H 2 O 2 (PMA/H 2 O 2 ) system, resulting the mineralizing the 4-CP via dichlorination and oxidation . The removal of 4-CP improved by 10% in 120 min in the WD-TENG powered electro-PMA/H 2 O 2 system. This study provides a promising methodology for improving the performance of self-powered electrochemical processes for the treatment of environmental pollution.
研究领域:
环境科学
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电化学工程
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DOI
高影响因子
ENVIRONMENTAL RESEARCH
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2025
·
IF 7.7
Ye Li,Bai-Hang Zhao,Bao-Yu Zhang,Jia-Hang Liu,Xu-Ming Liu
Peroxymonosulfate (PMS)-based advanced oxidation processes have gained significant attention due to their strong oxidative capacity and rapid reaction kinetics. However, the development of efficient, stable, and eco-friendly catalysts remains a major challenge in realizing practical applications. To address this issue, a novel catalyst, Co 1 Ce 2 O x @PAL, was synthesized via the sol-gel method to enhance PMS activation efficiency by leveraging rare-earth doping and the carrier properties of palygorskite (PAL). Comprehensive characterization (SEM, XRD, FTIR, etc.) confirmed successful synthesis and favorable structural properties. Norfloxacin (NOR) was selected as the target contaminant to evaluate the catalytic performance of Co 1 Ce 2 O x @PAL. Under an optimal condition (30% metal loading, 0.3 g/L catalyst, 0.5 mM PMS, pH 6.2), NOR removal efficiency reached 95%, with an apparent rate constant of 0.15 min -1 . Quenching tests and electron paramagnetic resonance (EPR) analyses revealed that played a dominant role in NOR degradation. and were generated through the redox reactions between Co 2+ /Co 3+ and Ce 3+ /Ce 4+ . Furthermore, oxygen vacancies facilitated electron transfer, thereby promoting radical production and NOR degradation efficiency. DFT calculation, including electrostatic potential and frontier orbital analyses (HOMO/LUMO), identified the quinolone and piperazine rings as the most susceptible sites for radical attack. Four potential degradation pathways were proposed accordingly. The catalyst demonstrated a high stability and reusability, maintaining over 80% NOR removal after five cycles. ECOSAR predicted reduced toxicity for most transformation products. This study highlights the potential of Co 1 Ce 2 O x @PAL as an effective catalyst for sustainable water treatment by enabling efficient degradation of trace emerging contaminants and promoting water resource recycling.
研究领域:
环境化学
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催化科学
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水处理技术
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材料科学
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计算化学
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污染物降解
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高级氧化过程
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PubMed
高影响因子
CATALYSIS LETTERS
·
2023
·
IF 2.8
Su Zheng,Sun Yu,Zhang Qi,Wang Jia,Zhou Wenqi,Zhou Suyin,Zhang Jinlong,Liu Yongdi,Zhou Liang,Lei Juying
Photocatalytic cofactor regeneration often encounters the problem of insufficient stability of reduced nicotinamide adenine dinucleotide hydrogen (NADH) regeneration due to the influence of reactive oxygen species. Here, we obtained Pt-loaded CdS nanorods (CdS NRs) with a one-dimensional (1D) rod-like structure by simple hydrothermal and photo-deposition methods. The yield of NADH improved by 52.54% within 40 min. Superoxide radical (·O 2 − ) had been proven to be the main reactive species that leaded to unwanted oxidation after NADH regeneration. After loading Pt, the formation of Schottky junctions between Pt and CdS NRs promoted the separation and migration of photogenerated carriers, resulting in a tendency of ·O 2 − to shift toward hydroxyl radical (·OH). ·OH produces additional intermediates in the oxidation of NADH compared to ·O 2 − , which inhibits the unwanted oxidation of NADH. Meanwhile, the conduction band position of Pt/CdS shifted positively and the ability to reduce O 2 was weakened, thus the ·O 2 − in the system was reduced, which weakened the oxidation of NADH and significantly improved the stability of NADH regeneration. These studies provide a new reference for applying loaded metal catalysts to the stable regeneration of NADH. Graphical Abstract
研究领域:
催化
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材料科学
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光化学
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生物化学
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DOI
高影响因子
iScience
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2022
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IF 6.107
Zheng Qian,Lingzhen Wang,Mawuli Dzakpasu,Yujia Tian,Dahu Ding,Rongzhi Chen,Gen Wang,Shengjiong Yang
The mechanism of spontaneous Fe III /Fe II redox cycling in iron-centered single-atom catalysts (I-SACs) is often overlooked. Consequently, pathways for continuous SO 4 ·- /HO⋅ generation during peroxymonosulfate (PMS) activation by I-SACs remain unclear. Herein, the evolution of the iron center and ligand in I-SACs was comprehensively investigated. I-SACs could be considered as a coordination complex created by iron and a heteroatom N-doped carbonaceous ligand. The ligand-field theory could well explain the electronic behavior of the complex, whereby electrons delocalized by the conjugation effect of the ligand were confirmed to be responsible for the Fe III /Fe II redox cycle. The possible pyridinic ligand in I-SACs was demonstrably weaker than the pyrrolic ligand in Fe III reduction due to its shielding effect on delocalized π orbitals by local lone-pair electrons. The results of this study significantly advance our understanding of the mechanism of spontaneous Fe III /Fe II redox cycling and radical generation pathways in the I-SACs/PMS process.
研究领域:
催化
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环境化学
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材料科学
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DOI
PubMed
高影响因子
CHEMICAL PHYSICS LETTERS
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2025
·
IF 3.1
Ying He,Lidan Ding,Jiabin Zhou,Dan Liu,Ying Zhang
In this study, Fe 2 O 3 /Bi 2 O 3 p-n heterojunction photocatalysts were fabricated to remove tetracycline (TC). The Fe 2 O 3 /Bi 2 O 3 /Vis/PMS system achieved the complete degradation of TC within 80 min, with a reaction rate constant of 0.0553 min −1 , which was 34.5 and 5.8 times higher than individual photocatalytic process and PMS-AOPs, respectively. This superior catalytic performance of Fe 2 O 3 /Bi 2 O 3 is primarily attributed to two key aspects. Firstly, forming a heterojunction promotes efficient segregation of photogenerated electron–hole pairs, wherein holes (h + ) directly activate PMS. Secondly, PMS simultaneously functioned as an electron acceptor to generate SO₄• − , accelerating the Fe 3+ /Fe 2+ redox cycle while inhibiting electron-hole recombination. This study confirmed the dual advantages of enhanced radical generation through PMS-assisted photocatalysis synergistic effects and improved charge separation via heterojunction engineering.
研究领域:
环境科学
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材料化学
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催化
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水处理技术
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DOI
高影响因子
Biomaterials Science
·
2021
·Vol. 9
·期 11
·4054-4065
·
IF 6.843
Desheng Cao,Hua He,Wei Li,Jin Yan,Jianhua Wu,Mengyuan Yin,Yang Zhou,Zhuchao Zhou,Lichen Yin
Anti-tumor treatment based on free radicals is often inefficient in hypoxic tumors, mainly because of the oxygen-dependent generation mechanism of reactive oxygen species (ROS). Herein, we report an NIR laser-controlled nano-system that is capable of generating alkyl radicals in situ in an oxygen-independent approach. Hollow mesoporous Prussian blue nanoparticles (HPB NPs) were developed to co-encapsulate the azo initiator (AIBI) and 1-tetradecanol as the phase change material (PCM, melting point of ∼39 °C), obtaining the AP@HPB NPs. At normal body temperature, the PCM remained in the solid state to prevent the pre-leakage of AIBI. Upon NIR laser irradiation (808 nm) at the tumor site, AP@HPB NPs generated heat upon photothermal conversion, which melted the PCM to release AIBI and decomposed AIBI to produce toxicity free alkyl radicals under both normoxic and hypoxic conditions. The alkyl free radicals efficiently killed tumor cells by causing oxidative stress and damaging DNA. Meanwhile, NIR light-induced hyperthermia cooperated with free radicals to efficiently eradicate tumors. This study therefore provides a promising strategy toward oxygen-independent free radical therapy, especially for the treatment of hypoxic tumors.
研究领域:
纳米技术
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癌症治疗
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生物医学工程
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药学
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DOI
PubMed
高影响因子
INORGANIC CHEMISTRY COMMUNICATIONS
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2025
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IF 5.4
Shikun Song,Xi Tong,Jie Tan,Jingjing Xu,Mindong Chen,Li Sun
In this study, CoWO 4 /CeO 2 composites were synthesized by a hydrothermal method and used as activated peroxymonosulfate (PMS) catalysts for the degradation of antibiotic sulfadiazine (SDZ). The synthesized composites underwent systematic characterization on the synthesized composites to investigate the effects of Co: Ce atomic ratio, initial pH, PMS dosage, inorganic anions and other factors on the degradation performance. The results showed that 5 mg/L of SDZ could be degraded basically completely (99.8 % degradation rate) in 20 min by CWC-2/PMS system. Moreover, the degradation rate of SDZ was still more than 82 % after the composite was reused four times. The free radical quenching experiments and EPR tests confirm the redox potential difference between Co 3+ /Co 2+ and Ce 4+ /Ce 3+ was utilized for bimetallic cycling. And it could activate PMS to mainly produce SO 4 − • and O 2 − • radicals efficiently. Thus SDZ could be degraded effectively in this system.
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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催化
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产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
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IF 9.7
Ying Jiang,Hao Lu,Lingli Lei,Daniel Scherman,Yingshuai Liu
The design of nanomedicines targeting specific tumor microenvironment (TME) characteristics, such as low pH, hypoxia, and elevated glutathione (GSH) concentration, holds significant potential for selectively killing cancer cells. In this study, we have developed a TME-responsive nanoparticle, i.e. , MIL-53(Fe)@MnO 2 stabilized with polyethylene glycol (FMP), which is capable of depleting GSH and sustainably generating hydroxyl radical (•OH) for enhanced chemodynamic therapy of cancer. After endocytosis, the FMP nanoparticles undergo gradual decomposition, resulting in GSH depletion while releasing Fenton-active Fe 2+ and Mn 2+ ions. These ions then subsequently catalyze a Fenton-like reaction to generate highly toxic •OH, ultimately inducing oxidative cell death. As a synergistic effect, the depletion of GSH further enhances therapeutic efficacy by inhibiting intracellular •OH scavenging. In vivo experiments demonstrated that this synergistically chemotherapeutic approach efficiently suppressed tumor growth without inducing significant systemic toxicity. This work presents a promising nanotherapeutic strategy that simultaneously depletes intracellular GSH and sustains cytotoxic •OH generation for enhanced tumor treatment.
研究领域:
纳米医学
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癌症治疗
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生物无机化学
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活性氧治疗
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靶向药物递送
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产品关联
DOI
PubMed
高影响因子
LANGMUIR
·
2025
·
IF 3.9
Tanxia Xiang,Yunlan Xu,Dengjie Zhong,Danli Tang
Organic pollutants present in wastewater pose severe threats to aquatic organisms and human health. In this study, a magnetic MFO/NCS@MoS2 composite catalyst was successfully synthesized via a hydrothermal method and applied for catalytic ozonation of methylene blue (MB). The catalyst was systematically characterized using multiple techniques including XRD, FT-IR, SEM, TEM, and XPS. Results revealed that the incorporation of chitosan (CS) effectively expanded the interlayer spacing of MoS2, which not only enhanced the structural stability but also promoted mass transfer and full exposure of active sites, thus promoting the generation of free radicals and nonfree radicals. As an electron donor, Mo4+ and unsaturated sulfur atoms on the surface of MoS2 not only provided active centers for catalytic ozonation, but also promoted the valence cycling between Mn2+/Mn3+ and Fe2+/Fe3+. In this way, the active centers of Mo4+ and unsaturated sulfur from MoS2 cooperated with the Mn/Fe bimetallic centers from MnFe2O4 to make the catalytic reaction continue. The 1.0MFO/NCS@MoS2/O3 system exhibited excellent catalytic activity and removed 99.13% of MB within 6 min. In addition, it possessed remarkable structural stability, strong anti-interference capability, and environmental compatibility. Radical trapping experiments verified that 1O2, O2•–, and •OH were involved in the degradation process. This study provides a new design strategy for developing efficient and recyclable ozonation catalysts.
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PubMed
高影响因子
RESEARCH ON CHEMICAL INTERMEDIATES
·
2018
·Vol. 44
·期 12
·7391-7410
·
IF 1.674
Wang Qiuyue,Zhang Yunfei,Wang Hongwu,Ma Luming
This study investigated the commercially available zero-valent copper powder and copper foil to activate molecular oxygen (O 2 ) and ozone for the degradation of organic pollutants. Under aerobic atmospheric conditions, copper powder effectively removed 50 mg/L of acetaminophen (ACT) within 2 h, though the degradation rate using the foil was less than 20% of the powder. However, copper foil activated ozone to effectively degrade ACT. The total organic carbon (TOC) removal reached a high of 58.3% at a catalyst concentration of 40 g/L, but only 26.8% with ozone alone. The initial solution pH and dosage of copper foil were key operational parameters affecting the ozone activation process. H 2 O 2 and Cu(I) were important intermediates in the process as hydroxyl radicals ( · OH) were identified via EPR (electron paramagnetic resonance) experiments and free radical scavengers. The generation of · OH was attributed to a Fenton-like reaction between Cu(I) and H 2 O 2 ; this free-radical generation mechanism differs from typical transition metal oxide catalysts. This study outlines a promising approach to significantly increase the generation of · OH and effectively remove refractory organic compounds. Furthermore, these copper products are applied in structural components of practical water treatment. Thus, the study of corrosion resistance to oxygen and ozone in aqueous solution have both a practical and theoretical significance. It was determined that copper products were resistant to oxygen corrosion in aqueous solution, but not resistant to ozone corrosion.
研究领域:
环境科学
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化学工程
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水处理
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DOI
高影响因子
ACS Applied Materials & Interfaces
·
2023
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IF 9.5
Jianghao Xing,Yuqi Yang,Wei Zhang,Jianqin Yan,Haisheng Qian,Jiqing Hao,Liang Cheng,Xianwen Wang
Tumors have become the biggest obstacle to human health, and there are various treatment methods at present. Photothermal therapy (PTT) is usually ineffective and does not inhibit tumor progression due to the inability of the lasers to penetrate deeply. Therefore, most existing studies chose a 1064 nm laser with stronger penetrating power; meanwhile, studies have shown that the inclusion of harmful free radicals can significantly improve the antitumor efficacy. Herein, TiO nanosheets (NSs) were creatively prepared and encapsulated with an alkyl radical generator {2,2′-azobis[2-(2-imidazoline-2-yl)propane] dihydrochloride, [AIPH]} in sodium alginate (ALG) hydrogel for effective tumor killing by PTT and pairing with dangerous free radicals. TiO NSs were obtained by the liquid-phase exfoliation method, together with AIPH, which were in situ coencapsulated multifunctional hydrogels formed by the combination of Ca2+ and ALG. This ALG hydrogel could enrich TiO NSs and AIPH at the tumor site for a long time, and through the excellent photothermal properties of TiO NSs, AIPH could slowly and effectively generate alkyl radicals at the tumor site, which, in turn, gave it a better antitumor effect compared with that of TiO NSs in the deep hypoxic environment of the tumor. The AIPH + TiO + ALG hydrogel has distinctive anticancer capabilities based on the results of both in vivo and in vitro experiments. This material also has good biosafety. By combining PTT and free radical treatment, this work provides a novel therapeutic method to achieve oxygen-independent free radical production and enhance therapeutic efficacy.
研究领域:
纳米技术
·
生物医学工程
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癌症研究
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材料科学
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产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）