APPLIED CATALYSIS B-ENVIRONMENTAL
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2024
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IF 20.2
Ruonan Guo,Changsheng Guo,Zenghui Bi,Heng Zhang,Ningqing Lv,Beidou Xi,Guangzhi Hu,Jian Xu
A novel iron-based single-atom catalyst (Fe SAC) integrated into a catalytic membrane was developed for peroxymonosulfate (PMS) activation and organic pollutant degradation. The Fe SAC membrane was synthesized using a co-precipitation method and acid leaching treatment, and its catalytic activity was evaluated in a continuous flow-through system using nitenpyram (NPR) as a model pollutant. The Fe SAC membrane/PMS system achieved over 90% NPR removal efficiency with low iron leaching (2.85–8.05 μg/L) during 10 hours of continuous operation, and maintained over 80% NPR removal in tap water, Yellow River water, and Yangtze River water. Experimental and theoretical analyses revealed that the strong chemisorption and electron transfer between PMS and FeN4 led to the dominant production of singlet oxygen for NPR degradation. This study demonstrates the potential of SAC-based catalytic membranes for efficient and stable attenuation of refractory organic pollutants in water treatment applications.
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2020
·
IF 10.652
Min-Ping Zhu,Jia-Cheng E. Yang,Xiaoguang Duan,Dan-Dan Zhang,Shaobin Wang,Baoling Yuan,Ming-Lai Fu
Metal organic frameworks (MOFs)-based catalysts are rising stars in advanced oxidation processes (AOPs) to generate reactive oxygen species (ROS). Nevertheless, constructing an affordable and recyclable MOFs-derived catalyst with high reactivity and stability is highly desirable but still challenging. Herein, we unprecedentedly designed a novel CoAl 2 O 4 @γ-Al 2 O 3 pellet (CoAl 2 O 4 @AP) as a heterogeneous catalyst to activate peroxymonosulfate (PMS) toward ROS generation for metronidazole (MNZ) removal. A CoAl 2 O 4 shell was formed on the pellet surface by direct calcination of the surface-nucleated ZIF-67 on γ-Al 2 O 3 pellets. The strong and unique interactions between the Co species of ZIF-67 and γ-Al 2 O 3 resulted in the formation of interfacial CoAl 2 O 4 . The CoAl 2 O 4 @AP exhibited a remarkably higher efficacy for PMS activation than ZIF-67-derived Co 3 O 4 and commercial Co 3 O 4 . The effects of several reaction parameters (i.e., PMS dosage, reaction temperature, initial pH, and background inorganic ions) on MNZ removal were comprehensively investigated and the degradation pathways of MNZ were elucidated. The Co 2+ /Co 3+ and oxygen vacancies of CoAl 2 O 4 @AP were the intrinsic active centers for PMS activation to simultaneously generate a diversity of ROS, among which SO 4 − and 1 O 2 played the decisive roles in MNZ decomposition. After the reaction, CoAl 2 O 4 @AP can be easily separated from the bulk solution and regenerated via a PMS-assisted cleaning process, making the composites highly appealing for practical applications. This pioneering work on constructing microscopic CoAl 2 O 4 -based composites expands the application of MOFs-based catalysts in novel AOPs systems for the treatment of persistent emerging pollutants.
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
ANALYTICA CHIMICA ACTA
·
2024
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IF 5.7
Meng Kou,Feng Qin,Yongda Wang,Lixin Peng,Zheng Hu,Hua Zhao,Zhiguo Zhang
Background Photodynamic therapy (PDT) is emerging as a promising cancer treatment. The PDT efficacy is primarily attributed to the generation of singlet oxygen ( 1 O 2 ), stemming from the integrated effects of the photosensitizer, oxygen, and light. The singlet oxygen quantum yield ( Φ Δ ) serves as a bridge that links these parameters to the overall efficacy of PDT. The near-infrared luminescence of 1 O 2 provides a direct way for determining Φ Δ , but suffers from a poor signal-to-noise ratio. While the chemical trap probe method is detection-friendly, but it has a strict requirement for the excitation wavelength. Therefore, the existing methods for Φ Δ measurement are insufficient. Results In this work, we developed an approach to determine Φ Δ of a broader range of photosensitizers using only the commonly used solvent dimethyl sulfoxide (DMSO), which can be oxidized by 1 O 2 to dimethyl sulfone. This method establishes the relationship between 1 O 2 production and changes in DMSO absorption spectra, eliminating the need for additional chemical probes. This method was validated by measuring the Φ Δ of rose bengal (RB) through systematic changes in absorption spectrum of DMSO under various RB concentrations and different excitation light power densities. Moreover, the Φ Δ of hematoporphyrin monomethyl ether (HMME), as determined by this method, is consistent with measurements obtained using the 1,3-diphenylisobenzofuran (DPBF) trapping probe. This consistency further validates the reliability of this method. Significance and novelty This work presents a direct, probe-free method to determine Φ Δ , reducing potential interference and expanding the range of useable excitation wavelengths. Its ability to measure Φ Δ using only DMSO enhances the accuracy of photosensitizer measurement, and broadens the applicability of the method to a wide range of samples, thereby advancing research on the properties of photosensitizers and further promoting the development of PDT.
研究领域:
生物医学
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化学
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产品关联
DOI
PubMed
高影响因子
Chemistry-An Asian Journal
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2024
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IF 3.5
Yu Si,Lei Wang,Hao Wu,Shoucai Yan,Yang Wang,Xiao Qian,Ziang Liu,Engin U. Akkaya
Controlled release of singlet oxygen from chemical sources is becoming an interesting path for eliciting apoptotic death of cancer cells. In this work, we present the synthesis and characterization of hitherto unknown class of aromatic endoperoxides, namely quinoline endoperoxides. Quinolines, especially after quaternization, show significant targeting of mitochondria. This leads to more effective cytotoxicity in cancer cell cultures suggesting a potential utility in cancer therapy.
研究领域:
癌症治疗
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药物化学
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细胞生物学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF DRUG DELIVERY SCIENCE AND TECHNOLOGY
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2020
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IF 2.734
Jingjing Dong,Yan Zhang,Pengyue Guo,Huanghuang Xu,Yuan Wang,Dongzhi Yang
Photodynamic therapy (PDT) has received extensive attention in tumor treatment due to its advantages in overcoming drug resistance for chemotherapy. In this work, we prepared a nanoplatform generated from graphene quantum dots capped in hollow mesoporous silica nanoparticles (GQDs/hMSN). The singlet oxygen ( 1 O 2 ) generation efficiency and photodynamic therapy effect of GQDs/hMSN were studied in vitro and in vivo . GQDs/hMSN had good 1 O 2 generation yield in water. Based on the findings from cellular experiments, we concluded that doxorubicin (DOX) loaded GQDs/hMSN (GQDs/hMSN(DOX)) had synergistic chemo-photodynamic therapeutic effect. From in vivo therapy on HeLa tumor-bearing mice, GQDs/hMSN exhibited significant accumulation in the tumor site, where DOX was also released from the nanoplatform due to the unique tumor microenvironment . This work further confirmed the usefulness of GQDs/hMSN nanoplatform as a potentially useful vector for combinational therapy of cancer.
研究领域:
生物医学工程
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肿瘤学
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纳米医学
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产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2021
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IF 7.312
Peizhen Yang,Songrong Li,Liang Xiaofu,An Xiaojing,Dongfang Liu,Wenli Huang
The degradation of organic contaminants via traditional radical-dominated advanced oxidation processes (AOPs) under high salinity conditions was limited due to side reactions between coexisting inorganic anions and radicals. Herein, a nonradical oxidation process via peroxymonosulfate (PMS) activation by CuO/MXene for treating high-salinity organic wastewater was developed. Rapid removal efficiency of target pollutant carbamazepine (CBZ) was significantly enhanced to 95.88% within 20 min by CuO/MXene under high salinity conditions (NaCl, 200 mM), compared to the efficiency of 4.30% exhibited by PMS alone. Besides, CBZ maintained a higher removal efficiency of > 81.04% in complex highly saline wastewater composed of eight common inorganic anions. Radical quenching experiments and electron paramagnetic resonance (EPR) analysis confirmed that radical and nonradical oxidation processes were involved in the catalytic process. However, singlet oxygen ( 1 O 2 ) was identified as the primary reactive species, and its contribution rate to CBZ degradation was > 73.58% in a wide pH range (3.0-9.0). The oxygenated functional groups and the interaction between CuO/MXene and PMS facilitated the production of 1 O 2 . The degradation pathway was proposed based on the detection of intermediates. This work provided a new inspiration for the decontamination of organic contaminants under high salinity conditions via a nonradical oxidation process.
研究领域:
环境科学
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化学工程
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产品关联
DOI
高影响因子
ANALYTICA CHIMICA ACTA
·
2025
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IF 6
Meng Kou,Feng Qin,Zhiguo Zhang,Linjun Li
Background Singlet oxygen ( 1 O 2 ) is a highly reactive oxygen species, playing an important role in a wide range of fields. The singlet oxygen quantum yield ( Ф Δ ) is a fundamental parameter for evaluating the efficiency of 1 O 2 generation by dye molecules. Various methods have been developed for Ф Δ measurement by exploiting the photoluminescence and chemical reactivity of 1 O 2 . We recently proposed a method for determining Ф Δ based on the reaction between Dimethyl Sulfoxide (DMSO) and 1 O 2 . However, due to the limited solubility of the reaction product, we supposed that the DMSO– 1 O 2 reaction would exhibit a termination point, which may affect the applicability of this method. Results In this work, we found that upon 1 O 2 generation, the absorption spectrum of DMSO initially changes and then reaches a plateau, which is attributed to the occurrence of a reaction termination in DMSO– 1 O 2 . Moreover, the occurrence time of the saturation point is inversely proportional to the excitation power density. When using the DMSO absorption change method to determine Ф Δ , the measurement must be conducted before this saturation point. Furthermore, due to the presence of the termination in DMSO– 1 O 2 reaction, the chemical probe method can still be applied for the determination of Ф Δ in DMSO under certain conditions. The relative degradation rate ( k ) of the probe exhibits an inflection point, with the slope k 2 after this point being greater than k 1 before it. This is because, prior to the inflection point, 1 O 2 generated by dye molecules react with both DMSO and chemical probe, and thus the degradation of probe reflects only a fraction of the total 1 O 2 . Hence, for the chemical probe method, measurements should be taken after inflection point. Significance This work provides a robust methodology for accurate determination of Ф Δ in DMSO, highlighting the necessity of selecting appropriate time windows tailored to each measurement method.
研究领域:
光化学
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活性氧物种
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分析方法学
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产品关联
DOI
PubMed
高影响因子
NEW JOURNAL OF CHEMISTRY
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2019
·Vol. 43
·期 41
·16385-16390
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IF 3.069
Qian Xu,Ying Gao,Xiaofu Wu,Hao Hang,Hua Li,Yonghong Chen,Weijie Wang,Hui Tong
Two subphthalocyanine (SubPc)-based conjugated porous polymers, SubPc-P1 and SubPc-P2, have been designed and synthesized by an A3 + B2 and A4 + B2 type Sonogashira cross-coupling reaction, in which axial coupling is absent and present, respectively. These two polymers exhibit Brunauer–Emmett–Teller surface areas of 434 m2 g−1 and 106 m2 g−1, respectively. Combining their porosity with strong light harvesting capability, SubPc-P1 and SubPc-P2 can efficiently absorb long-wavelength photons even in the near-infrared region to generate singlet oxygen rapidly. In addition, compared with SubPc-P2, SubPc-P1 shows red-shifted light absorption and a larger specific surface area, which agrees well with the better singlet oxygen generation ability upon irradiation at 690 nm.
研究领域:
材料科学
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光化学
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生物医学工程
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DOI
高影响因子
CHEMICAL PHYSICS
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2024
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IF 2
Lu Li,Feng Qin,Yongda Wang,Zhiguo Zhang
The proportion of singlet oxygen ( R ) produced from the triplet state of porphyrin in aqueous solutions was investigated by substituting porphyrin molecules with the metalloporphyrin Platinum(II) meso -tetraphenylporphyrin (Pt-TPP). The feasibility of using platinum porphyrin as a substitute for porphyrin to study the photophysical properties in photodynamic therapy (PDT) was confirmed. The model of first-order decay in a water-methanol mixed solution encompasses potential deactivation processes of the excited triplet states and was built, which was confirmed by monitoring the change in the total transition rate of the T 1 state ( A 0 ) value at different water contents under anoxic environments, obtained through measuring the phosphorescence lifetime ( τ p ) of Pt-TPP. Combined with A 0 and the quenching rate constant of T 1 by O 2 ( k q ), the formula for R in relation to changes in oxygen can be deduced in pure water.
研究领域:
生物化学
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医学
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2020
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IF 10.652
Tongcai Liu,Danyu Zhang,Kai Yin,Chunping Yang,Shenglian Luo,John C. Crittenden
Unactivated peroxymonosulfate (PMS) degrading organic contaminants has been reported. Previous studies have focused on direct PMS oxidation, while the role of singlet oxygen ( 1 O 2 ) is often overlooked. Here, we studied the oxidation of thiacloprid (THIA) of the neonicotinoid insecticides by PMS without explicit activation. According to electron spin resonance spectroscopy and quenching experiments, the nonradical mechanism (i.e., direct PMS oxidation and 1 O 2 oxidation) was responsible for the THIA degradation. There are two pathways to generate 1 O 2 . The pyridine nitrogen of THIA structure can combine with PMS to produce epoxide , which is beneficial to generation of 1 O 2 . However, the contribution of 1 O 2 from PMS self-decomposition can be ignored. According to kinetic solvent isotropic effect analysis, the overall THIA degradation was attributed to 36.5% 1 O 2 oxidation and 63.5% direct PMS oxidation. A structure-activity assessment and density functional theory suggested that thioether sulfur, amidine nitrogen and the cyanoimino groups were the main reaction sites. Product analysis further confirmed the involvement of 1 O 2 and PMS. Moreover, three major THIA degradation pathways were proposed, including (i) heterolytic cleavage of peroxo bonds and transfer of oxygen atoms, (ii) electron transfer and (iii) oxidation of cyanoimino groups to generate nitroso/nitro-THIA. In addition, identification byproducts (Except for TP141) had lower ecotoxicity toxicity (using ECOSAR) in fish, daphnid and green algae. Effects of pH and natural water matrices on THIA oxidation via PMS were further evaluated. This study investigated the overlooked 1 O 2 oxidation reaction to elucidate the mechanism. The new mechanistic knowledge has important implications for other contaminants for their interactions with PMS.
研究领域:
环境科学
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化学
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DOI
高影响因子
ANALYTICAL CHEMISTRY
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2022
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IF 8.008
Xuwen Gao,Huimin Zhao,Dongyang Wang,Yuqi Xu,Bin Zhang,Guizheng Zou
Singlet oxygen (1O2) is an important reactive oxygen species (ROS) that is intensively involved in natural photochemical and photobiological processes. Herein, selectively lighting up 1O2 is achieved in the aggregation-induced emission (AIE) of electrochemiluminescence (ECL) from the Zn2+-mediated AIE assembly of Au nanoclusters (Zn2+-AIE-AuNCs). Zn2+-AIE-AuNCs can exhibit efficient AIE ECL and photoluminescence (PL) along with 1O2 generation in energy and charge transfer routes, respectively. The AIE ECL of the Zn2+-AIE-AuNCs/tripropylamine (TEA) system in carbonate buffer is located around 703 nm with the dimeric aggregate of 1O2 as an emitter because electrochemically oxidizing coexisted Zn2+-AIE-AuNCs and TEA in carbonate buffer would promote the oxygen vacancy (Ov) of Zn2+-AIE-AuNCs, which could selectively enable the generation of emissive singlet oxygen in the energy transfer route by effectively transferring the energy from excited singlet Zn2+-AIE-AuNCs to the triplet ground state of dissolved oxygen (3O2). No emissive 1O2 is detected via electrochemically oxidizing the Zn2+-AIE-AuNCs in the case without either carbonate buffer or TEA, and the Zn2+-AIE-AuNCs/TEA system can only exhibit AIE ECL around 485 nm with Zn2+-AIE-AuNCs as the emitter in carbonate-free buffers. Photoexciting Zn2+-AIE-AuNCs merely brings out band-gap-engineered AIE PL around ∼485 nm with Zn2+-AIE-AuNCs as the emitter, which manifests that the 1O2 generated in the charge transfer route via photoexciting Zn2+-AIE-AuNCs is un-emissive. This work not only proposes an effective strategy for AIE with 1O2 as an emitter but also opens a promising way to selectively light up 1O2.
研究领域:
化学
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材料科学
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光化学
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电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF BIOMEDICAL OPTICS
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2011
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IF 3.188
Bolin Hu,Nan Zeng,Zhiyi Liu,Yanhong Ji,Weidong Xie,Qing Peng,Yong Zhou,Yonghong He,Hui Ma
Photodynamic therapy is a promising cancer treatment that involves activation of photosensitizer by visible light to create singlet oxygen. This highly reactive oxygen species is believed to induce cell death and tissue destruction in PDT. Our approach used a near-infrared area CCD with high quantum efficiency to detect singlet oxygen by its 1270-nm luminescence. Two-dimensional singlet oxygen images with its near-infrared luminescence during photosensitization could be obtained with a CCD integration time of 1 s, without scanning. Thus this system can produce singlet oxygen luminescence images faster and achieve more accurate measurements in comparison to raster-scanning methods. The experimental data show a linear relationship between the singlet oxygen luminescence intensity and sample concentration. This method provides a detection sensitivity of 0.0181 μg/ml (benzoporphyrin derivative monoacid ring A dissolved in ethanol) and a spatial resolution better than 50 μm. A pilot study was conducted on a total of six female Kunming mice. The results from this study demonstrate the system's potential for in vivo measurements. Further experiments were carried out on two tumor-bearing nude mice. Singlet oxygen luminescence images were acquired from the tumor-bearing nude mouse with intravenous injection of BPD-MA, and the experimental results showed real-time singlet oxygen signal depletion as a function of the light exposure.
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DOI
高影响因子
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