Inorganics
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2025
·Vol. 13
·期 9
·279
·
IF 3
Pengcheng Zhu,Zilong Guo,Yulin Sha,Yonghang Li,Xiaoyu Zhang,Yandong Han,Wensheng Yang,Xiaonan Ma
Aqueous singlet oxygen (1O2) sensitization is of high interest due to its wide application in bio-imaging and photodynamic therapy. For organic photosensitizers like porphyrin derivatives, surfactant-assisted micelles have been intensively explored for dispersing hydrophobic sensitizers in aqueous phase; however, they can suffer from poor long-term stability. In this work, palladium octaethylporphyrin (PdOEP)-embedded silica particles were prepared with assistance from Tween micelles, and their corresponding application in aqueous1O2sensitization was explored. With assistance from Tween 80 at a >3 mg/mL concentration, superior (>95%) solubilization of PdOEP was observed in aqueous solution, leading to a high1O2quantum yield (ΦΔ≈ 93%). By optimizing the synthesis conditions, >95% of micellar PdOEP was embedded into silica particles, exhibiting comparable ΦΔ(up to 70%) to micellar systems by effectively suppressing PdOEP aggregation in particles. The PdOEP-embedded silica particles exhibited dramatically enhanced long-term stability (more than one year) compared to corresponding micelles with a half-life of ~38 days. In addition, aqueous1O2sensitization by PdOEP-embedded silica particles was demonstrated upon two-photon excitation in a near-infrared regime (λex= 1030 nm), highlighting the great potential of this method for future biological applications.
研究领域:
光动力治疗
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纳米材料
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生物成像
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活性氧
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药物递送
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DOI
高影响因子
PROCESS SAFETY AND ENVIRONMENTAL PROTECTION
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2025
·
IF 7.8
Tianjian Dang,Guanghua Lu,Min Wang,Yuhao Ji,Yufang Chen,Runren Jiang
The lifetime of free radicals limits the effectiveness of catalytic degradation reactions and the efficient utilization of transient free radicals remains a significant challenge in current research. In this paper, we have developed MIL-125 MOF derivatives, which can influence the morphology and structure of the materials by controlling the calcination time. The CT3 system significantly enhanced the activation performance of persulfate (PDS) and enabled the complete degradation of acetaminophen (ACT) within 20 min. The electron acceptor effect of the C C double bond accelerates the generation of singlet oxygen in the CT3 system, and rapidly acts on ACT, thereby improving the degradation performance of the CT3 system. Product analysis and soybean seed germination experiments confirmed that the toxicity of the degradation products was significantly reduced, and the degraded solution did not affect soybean growth. This study offers novel approaches and insights for utilizing MOF derivatives to activate PDS for the degradation of organic contaminants.
研究领域:
环境科学
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催化化学
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材料科学
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DOI
高影响因子
LANGMUIR
·
2026
·
IF 4.4
Haiyan Zhu,Bing Liu
Porphyrin is an excellent photosensitizer for generating singlet oxygen (SO) in photodynamic therapy, but the aggregation issue has long been reported to weaken its therapeutic efficacy in practical applications. To address this challenge, we here report the design and synthesis of a series of amphiphilic porphyrin-terminated poly(N-isopropylacrylamide), which can self-assemble into sub-50 nm porphyrin nanoparticles via the nanoprecipitation route. We demonstrated that the NP size could be easily tuned by adjusting the self-assembly conditions. Furthermore, compared with pure hydrophobic porphyrin NPs prepared using a similar method, the resulting NPs exhibited an enhanced SO generation rate. Notably, the SO generation rate showed an intriguing temperature dependence, highlighting the potential of these NPs to serve as photosensitizers in photodynamic therapy applications.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2026
·
IF 19.7
Dezhi Kong,Menghui Chu,Jianfei Yao,Juan Wang,Junshuo Nie,Haoru Song,Feifei Wang,Guo Wang,Chen-Ho Tung,Guanyun Zhang,Jikun Li,Yifeng Wang
Visible light regulates electronic states to promote Fenton-like catalysis. • Dual single-atom CoMo-CN catalyst enhences micropollutant degradation and mineralization. • CoMo-CN/PMS/vis-light system achieves highly selective singlet oxygen generation. Singlet oxygen ( 1 O 2 ) plays a critical role in oxidative transformations, yet achieving selective and rapid generation via peroxymonosulfate (PMS), a recently developed strategy, remains a nontrivial challenge. Here we demonstrate that visible light can function as an unconventional electronic-state regulator to control PMS activation toward 1 O 2 production. Using a dual single-atom CoMo catalyst anchored on graphitic carbon nitride, irradiation induces a reversible and opposite electronic-state modulation of Co and Mo through dynamic charge redistribution. This reconfiguration weakens the overly strong interaction between Co sites and oxygenated intermediates, thereby lowering the desorption barrier of 1 O 2 and increasing reaction flux along a disproportionation-like pathway. The system exhibits markedly enhanced PMS activation, accelerated pollutant degradation, deep mineralization, broad substrate applicability, and robust performance under complex water matrices and device-relevant conditions. Notably, charge-carrier recombination in transition-metal-modified semiconductors, typically detrimental to conventional photocatalysis, is instead advantageous for PMS activation. Our findings establish light as a mild and reversible regulator of metal electronic states, providing a general framework for catalytic behavior tuning beyond conventional photocatalysis. Synopsis Visible light acts to modulate electronic-state in a Co-Mo dual single-atom catalyst (Co reduced, Mo oxidized) to enhance selective 1 O 2 generation from peroxymonosulfate, enabling efficient removal of organic micropollutants from water. Download: Download high-res image (201KB) Download: Download full-size image
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ChemNanoMat
·
2019
·Vol. 6
·期 1
·124-131
·
IF 3.431
Jia-Ru Feng,Si-Yong Qin,Lei Rong,Yin-Jia Cheng,Yi-Han Ma,Ai-Qing Zhang
Graphical Oligopeptide amphiphiles (OPAs) with different degrees of unsaturation self-assemble into shape-specific nanostructures. The linoleic acid-bearing OPA could generate singlet oxygen ( 1 O 2 ) in the presence of lipoxidase and catalytic iron (II) ion, which offers new insight into designing self-deliverable nanoplatform for 1 O 2 -mediated cancer treatment. We report here on three oligopeptide amphiphiles (OPA1-3) with different unsaturated double bonds, which self-assemble into shape-specific nanostructures. It was found that OPA1 with saturated hydrophobic tail self-assembled into conventional cylindrical nanofibers, while the unsaturated OPA2-3 molecules self-organized into helical nanoarchitectures. Due to the different double bond numbers in hydrophobic tails of OPA2-3, the helical pitch and width of their self-assemblies varied. Specially, linoleic acid-bearing OPA3 could be oxidized by lipoxidase to create hydroperoxide-containing OPA4, which further generated singlet oxygen ( 1 O 2 ) in the presence of catalytic iron (II) ion. The established system may provide a self-deliverable nanoplatform for 1 O 2 -mediated cancer treatment.
研究领域:
生物化学
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纳米医学
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肿瘤学
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DOI
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2024
·
IF 10.8
Hongchao Li,Xinyue Zhang,Shuai Yang,Yibing Sun,Jieshu Qian
Significant efforts have recently been exerted toward construction of singlet oxygen (1O2)-dominated catalytic oxidation systems for selective removal of organic contaminants from wastewater, with peroxides serving as the chemical source. However, the relevance of 1O2 in the removal of pollutants remains ambiguous and requires elucidation. In this study, we scrupulously exclude the significant role of 1O2 in contaminant degradation in various peroxymonosulfate (PMS) activation systems. Multiple experimental results indicate that the activation of PMS catalyzed by CuO, MnO2, Fe-doped g-C3N4 (Fe–CN), or N-doped graphite does not predominantly follow the 1O2 pathway. More importantly, the reactivity of 1O2 is remarkably overestimated in the literature, given its inferior capacity in degradation of a range of heterocyclic contaminants and aromatic compounds possessing electron-withdrawing groups. In addition, the strong physical quenching effect of water, coupled with the low oxidizing ability of 1O2, would notably reduce the utilization efficiency of peroxide, which is particularly apparent in the degradation of micropollutants. We reckon that this study is expected to end the long-running dispute associated with the relevance of 1O2 in pollutant removal.
研究领域:
环境科学
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化学工程
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PubMed
高影响因子
IEEE PHOTONICS TECHNOLOGY LETTERS
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2022
·Vol. 34
·期 12
·661-664
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IF 2.414
Tianfeng Wang,Jianfei Dong
Anti-fungal blue light (ABL) therapies are based on the photochemical reaction of endogenous photosensitizer (PS) in fungal cells. Knowing the spectral sensitivity of these cells for the ability to generate singlet oxygen is thus important to determine the most effective wavelength of such light therapies, and thereby to design ABL therapeutic devices, e.g., by light emitting diodes. We propose a modeling method of such spectral sensitivity in this work, based on the absorption spectra of cells and other inherent characteristic parameters, i.e., singlet oxygen quantum yield and the extinction coefficient of the endogenous PS. Specifically, the absorption spectra are determined by the PSs inside the fungus Candida albicans and human epithelial cells. Then, the concentration of PS in those two types of cells was measured by high-performance liquid chromatography (HPLC) assays. The HPLC assays show that the coproporphyrin (CP) is the main PS in C. albicans, accounting for 60% of the total PS. The simulation results demonstrate that the 390~420nm light can stimulate the PS in the cells to generate more singlet oxygen in C. albicans than in epithelial cells; and this range is the same as the CP Soret band. In contrast, the light with wavelengths >450nm is less effective in exciting the PS in C. albicans, and leads to more singlet oxygen generation in V.E. cells than shorter wavelength. We thus conclude that 390~420nm light is the most effective range for inhibiting C. albicans with the least damage to human host cells.
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TALANTA
·
2020
·
IF 5.339
Chang Ping Yang,Li He,Cheng Zhi Huang,Yuan Fang Li,Shu Jun Zhen
Due to the ultra-weak and instantaneous chemiluminescence (CL) of luminol–H 2 O 2 system, developing new catalysts to dramatically enhance and produce persistent CL emission is crucial. In this study, the Cu-metal-organic frameworks (Cu–MOFs) with flower morphology converted from Cu-based metal-organic gels (Cu–MOGs) could catalyze luminol–H 2 O 2 system, exhibiting persistent CL. The possible mechanism of this persistent emission of luminol was attributed to the gradual generation of OH˙, O 2 ˙ − and 1 O 2 in Cu–MOFs–catalyzed luminol–H 2 O 2 system. In addition, OH˙ and O 2 ˙− were continuously recombined into singlet oxygen on the surface of Cu–MOFs which further prolonged the duration time of the CL leading to the persistent emission, due to the longer lifetime of 1 O 2 compared to OH˙ and O 2 ˙ − . Furthermore, based on the high-intensity emission of Cu–MOFs–catalyzed luminol–H 2 O 2 system, the strategy for sensitive response to quercetin was established with good linearity within the range of 0.05–1.2 μM and a detection limit of 49.7 nM. This study provides a new idea for developing persistent CL catalysts.
研究领域:
化学
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材料科学
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分析化学
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PubMed
高影响因子
APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Dong Li,Kaixuan Wang,Jiahong Tang,Yizhou Zhao,Hanan Elhaes,Muhammad Tahir,Medhat A. Ibrahim,Yujing Li
Two-dimensional (2D) organic-inorganic hybrid halide perovskites have gained extensive attention in photovoltaics , photodetectors and light-emitting diodes owing to their unique optoelectronic properties and superior stability compared with their three-dimensional (3D) counterparts. However, 2D perovskites have rarely been applied for photochemical conversion applications. Herein, a series of 2D BA 2 MA n-1 Pb n Br 3n+1 perovskite nanosheets have been synthesized through a facile, ligand-free precipitation (LFP) method at room temperature . Using the specific chemical trapping techniques, we show for the first time that the 2D perovskite nanosheets can effectively generate photosensitized singlet oxygen ( 1 O 2 ) via energy transfer from triplet excitons to molecular oxygen in non-polar solvent. Based on this discovery, the as-prepared BA 2 PbBr 4 and BA 2 MAPb 2 Br 7 nanosheets successfully catalyze the ENE reaction and 1,2-addition reaction between olefin and singlet oxygen under visible light . Our study is anticipated to develop and demonstrate new mechanisms for 2D halide perovskite materials in photodynamic therapy and photocatalytic applications.
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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高影响因子
JOURNAL OF FLUORESCENCE
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2024
·
IF 2.6
Zuo Pengli,Peng Jun,Yao Yuyang,Tan Wei,Cheng Lan,Zhang Jinyu,Lu Xiuhua
Due to the unique chemical and biomedical properties of carbon dots (CDs), they have increasingly obtained the attention in many research fields, for example, bioimaging, fluorescence sensing, and drug delivery, etc. Recently, it was found that, under light excitation, CDs can also be exploited as a novel photosensitizer to prepare reactive oxygen species (ROS), which expand their applications in the field of photodynamic therapy for cancer treatment. Nevertheless, the high cost and complex fabrication approach of CDs significantly limit their applications. To address this issue, bottom-up routes usually utilize sustainable and inexpensive carbon precursor as starting materials, employed N,N-dimethylformamide (DMF) or ethanol as an environmental-friendly solvent. Bottom-up approach was energy efficient, and the purification process was relatively simple by dialysis. Therefore, carbon dots (CDs) were facilely fabricated in a one-pot solvothermal process using 1-aminoanthraquinone as a precursor, and their application as photosensitizers for in vitro antitumor cells, especially photodynamic therapy (PDT) was established. Then the photophysical and nanoscale dimensions properties of the fabricated CDs were characterized via TEM, UV–visible, fluorescence, and FT-IR spectroscopy. The synthesized N-doped CDs can easily dissolve in water, possess very low biotoxicity, yellow-light emission (maximum peak at 587 nm). More importantly, PDT studies demonstrated that the obtained CDs possess a high singlet oxygen yield of 35%, and exhibit significant phototoxicity to cancer cells upon 635 nm laser irradiation. These studies highlight that N-doped CDs can be facilely synthesized from only one precursor, and are a potentially novel theranostic agent for in vivo PDT.
研究领域:
材料科学
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生物医学工程
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肿瘤学
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DOI
PubMed
高影响因子
RSC Advances
·
2015
·Vol. 5
·期 100
·81897-81904
·
IF 3.84
Junliang Lv,Xin Zhang,Nana Li,Baoju Wang,Sailing He
Metal nanoparticles (MNPs) can be used as a kind of new photodynamic therapy (PDT) agent because singlet oxygen (1O2) can be generated through directly sensitizing MNPs. Gold nanorods, gold nanoshells and gold nanoechinus were confirmed to be efficient PDT agents in vivo. However, the major excitation spectra of 1O2 from all of them are not in the optical biological window (650–900 nm). Herein, gold bipyramids (GBPs) with tunable absorption wavelength were prepared and used to explore 1O2 generation capability. 1O2 can be generated when GBPs were excited by continuous-wave light within a wide range of wavelengths (660–975 nm). The highest 1O2 generation capabilities were obtained when they were excited at the wavelength of the absorption peak, which was quite different from those of other gold nanomaterials. It was also found that 1O2 can be generated efficiently by a laser of very low power density (200 mW cm−2). The capability of GBPs for PDT has been demonstrated through the destruction of cancer cells. The synergistic effect of PDT and photothermal therapy for the destruction of cancer cells was also demonstrated.
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高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2020
·
IF 9.038
Jingjing Yang,Wen Zhu,Qian Yao,Guining Lu,Chen Yang,Zhi Dang
This study explored the photochemical activity of nitrogen-doped biochars (NCMs) by investigating their role in the degradation of sulfamethazine under simulated sunlight irradiation. NCMs with different doping amounts were prepared from corn straw and urea. Results showed that nitrogen doping can notably enhance the photodegradation of SMT rather than raw char. NCMs are of photochemical activity under visible light, which was confirmed by monochromatic light experiments. Quenching experiments, ESR, pH effect, and the influence of O 2 were carried out to explore the involved oxidation mechanism in this system. Results showed that 1 O 2 was the main reactive oxygen species . 1 O 2 was produced from O 2 by both energy transfer and electron transfer . DFT calculations showed that pyridinic N doping can decrease the energy of intersystem crossing and thus benefit the generation of 1 O 2 by triplet-triplet energy transfer. Results underscore the explicit importance of nitrogen element in photochemical reactivity of chars under simulated light irradiation even when the nitrogen content is low. It is a meaningful reminder for us to pay more attention to the assessment of the fate and transport of contaminants in the soil where it is rich in NCMs as well as the potential use of NCMs for pollutants remediation, since visible light is very abundant near the earth’s surface.
研究领域:
环境科学
·
化学
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DOI
PubMed
高影响因子
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