Optical Materials Express
·
2017
·Vol. 7
·期 3
·913-923
·
IF 2.591
Qian Yang,Chuang Zhao,Jun Zhao,Yong Ye
Interaction between upconversion nanoparticles (UCNPs) and natural photosensitizers (Ps) has not been investigated so far. In order to make new near infrared photosensitizers, the conjugates (Ps-UCNPs) were synthesized by NaYF4 as a substrate and hydrothermal reaction of lanthanide ions Yb3+ with Er3+ or Tm3+, and then interaction with pheophorbide A (Pha) and resveratrol (Res) respectively. Based on the intensity of the fluorescence emission by Ps-UCNPs, the optimal reaction conditions are 16 mM Yb3+/0.4 mM Er3+ at 120°C for 20 h for Pha-UCNPs, and 80 mM Yb3+/0.1 mM Tm3+ at 180°C for 20 h for Res-UCNPs. The nanoparticles have a hexagonal phase or cubic phase with an average diameter size of 220 nm, and selectively emit the stronger red (670 nm) or violet (380 nm) fluorescence. Pha-UCNPs show the strong effects, and the maximum yield of singlet oxygen was seven times more than UCNPs and pheophorbide A alone under 980 nm illumination. It is attributed to the efficient resonance energy transfer from UCNPs to pheophorbide A. Pha-UCNPs is an effective NIR photosensitizer with potential for deep tissue disease photodynamic therapy.
研究领域:
生物医学工程
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纳米医学
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DOI
高影响因子
Journal of Materials Chemistry B
·
2017
·Vol. 5
·期 46
·9175-9182
·
IF 4.543
Jie Gao,Caihong Wang,Hongliang Tan
This work demonstrated the potential of zeolitic imidazolate framework-8 (ZIF-8) as a host for the co-encapsulation of multiple fluorescent cargos to fabricate fluorescent composites for ratiometric sensing. The one-pot self-assembly of 2-methylimidazole, zinc nitrate, 9-anthracenecarboxylic acid (AnC), and polystyrene sphere doped with europium chelate (EuPS) in methanol solution can lead to the formation of dual-emissive EuPS@AnC/ZIF-8 with excellent fluorescent activity. Based on the distinct fluorescent responses of Eu3+ and AnC to singlet oxygen (1O2), EuPS@AnC/ZIF-8 can be developed as a ratiometric sensor for 1O2 detection. In this ratiometric sensor, Eu3+ fluorescence was employed as a reference signal for providing built-in correction to avoid environmental effects, while AnC fluorescence served as a response signal to detect 1O2 because of its turn-off behavior upon reacting with 1O2. Benefiting from the confinement effect of the ZIF-8 host, the presented sensor showed high sensitivity toward 1O2 with a detection limit of 43 nM and excellent selectivity over other reactive oxygen species. More attractively, the target responsive fluorescent color change of EuPS@AnC/ZIF-8 allowed 1O2 to be easily identified by the naked eye under a UV lamp. We hope that this study will provide a new insight into the design and application of multifunctional composites based on metal–organic frameworks.
研究领域:
材料科学
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生物医学工程
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化学
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DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2024
·
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.
研究领域:
环境科学
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材料科学
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生物学
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DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2024
·
IF 12.2
Ziyang Chu,Zhengyan Han,Haibo Liu,Tianhu Chen,Xuehua Zou,Hanlin Wang,Fuwei Sun,Hao Wang,Dong Chen
The simultaneous removal of heavy metal complexes (HMCs) and heavy metal ions presents a significant challenge in treating wastewater. To address this, we propose a Calcite/Peroxymonosulfate (Calcite/PMS) system aimed at simultaneously decomplexing Cu-EDTA and removing Cu ions . Calcite/PMS system could achieve 99.5 % Cu-EDTA decomplexation and 61.9 % Cu ions removal within 60 min under initial conditions of Cu-EDTA (10 mg/L), Calcite (3 g/L), and PMS (2 mM). Singlet oxygen ( 1 O 2 ) emerged as the predominant reactive species responsible for Cu-EDTA decomplexation, which selectively targeted the N-C bonds in the Cu-EDTA structure to produce intermediates with lower biotoxicity than EDTA. Interestingly, solid phase Cu(III) (≡Cu(III)) promoted the generation of superoxide radicals (O 2 •− ) with a contribution of up to 72.8 %. Subsequently, nascent ≡Cu(III) and O 2 •− accelerated the degradation of intermediates. Besides, coexisting organic substances inhibited Cu-EDTA decomplexation, whereas inorganic ions had a weak impact. After five cycles of use, the Calcite/PMS system retained 99.3 % efficiency in decomplexing Cu-EDTA. This investigation provides valuable insights into using calcite to remove HMCs and enhances our comprehension of the decomplexation intermediates accelerating HMCs degradation.
研究领域:
环境科学
·
化学
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DOI
PubMed
高影响因子
Cell Reports Physical Science
·
2023
·
IF 8.9
Shipeng Ning,Xing Zhang,Meng Suo,Meng Lyu,You Pan,Yi Jiang,Huawei Yang,Jacky Wing Yip Lam,Tianfu Zhang,Linghui Pan,Ben Zhong Tang
The development of strategies to maintain the long-term presence of reactive oxygen species in tumor sites remains an urgent issue to be addressed. Here, we design platelet exosome hybrid liposome nanovesicles (named platelet-derived exosome hybrid liposomes co-loaded with DPDPy and chloroperoxidase [DCHL]) co-loading aggregation-induced emission (AIE) photosensitizers and chloroperoxidases to facilitate uninterrupted singlet oxygen ( 1 O 2 ) generation for enhancing breast cancer immunotherapy. When DCHL enters tumor cells, it lyses under external laser irradiation, thus releasing AIE photosensitizers (DPDPy) and chloroperoxidase. Subsequently, chloroperoxidase utilizes hydrogen peroxide (H 2 O 2 ) and chloride to synthesize HClO, and, as a second step, HClO reacts with H 2 O 2 to form 1 O 2 . Therefore, uninterrupted 1 O 2 generation is achieved. The experimental results show that DCHL plus light can lead to systemic immune response, increase the proportion of central memory T cells and tumor-infiltrating T cells, and thereby delay tumor recurrence and rechallenge. Overall, the DCHL system provides a good idea for the design of tumor treatment system.
研究领域:
肿瘤学
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生物医学工程
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免疫学
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DOI
高影响因子
CHINESE JOURNAL OF CHEMICAL PHYSICS
·
2021
·Vol. 34
·期 4
·406-412
·
IF 1.114
Wang Chen,Xiong Ming-chen,Zhao Xuan,Liu Kun-hui
The pharmaceutically active compound atenolol, a kind of β -blockers, may result in adverse effects both for human health and ecosystems if it is excreted to the surface water resources. To effectively remove atenolol in the environment, both direct and indirect photodegradation, driven by sunlight play an important role. Among indirect photodegradation, singlet oxygen ( 1 O 2 ), as a pivotal reactive species, is likely to determine the fates of atenolol. Nevertheless, the kinetic information on the reaction of atenolol with singlet oxygen has not been well investigated and the reaction rate constant is still ambiguous. Herein, the reaction rate constant of atenolol with singlet oxygen is investigated directly through observing the decay of the 1 O 2 phosphorescence at 1270 nm. It is determined that the reaction rate constant between atenolol and 1 O 2 is 7.0×10 5 (mol/L) −1 · s −1 in D 2 O, 8.0×10 6 (mol/L) −1 · s −1 in acetonitrile, and 8.4×10 5 (mol/L) −1 · s −1 in EtOH, respectively. Furthermore, the solvent effects on the title reaction were also investigated. It is revealed that the solvents with strong polarity and weak hydrogen donating ability are suitable to achieve high rate constant values. These kinetics information on the reaction of atenolol with singlet oxygen may provide fundamental knowledge to the indirect photodegradation of β -blockers.
研究领域:
环境科学
·
药理学
·
化学动力学
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DOI
高影响因子
WATER RESEARCH
·
2017
·
IF 6.942
Yang Zhou,Jin Jiang,Yuan Gao,Su-Yan Pang,Yi Yang,Jun Ma,Jia Gu,Juan Li,Zhen Wang,Li-Hong Wang,Li-Peng Yuan,Yue Yang
In this study, the kinetics of reactions of peroxymonosulfate (PMS) with ten model phenols (including phenol, methylphenols, methoxyphenols, and dihydroxybenzenes) were examined. The oxidation kinetics of these phenols by PMS except for catechol and resorcinol showed autocatalysis in alkaline conditions (pH 8.5 and 10), due to the contribution of singlet oxygen ( 1 O 2 ) produced from PMS activation by quinone intermediates formed from their phenolic parents. The oxidation rates of ortho- and meta-substituted methylphenols and methoxyphenols by PMS were much higher than their para-substituted counterparts under similar conditions. This was attributed to the relatively low yields of quinone intermediates from para-substituted phenols. SMX could be efficiently degraded by PMS in the presence of phenols which showed great autocatalysis when they individually reacted with PMS, and the addition of methanol in excess had negligible influence suggesting that 1 O 2 rather than hydroxyl radical and sulfate radical played an important role. Transformation of SMX by 1 O 2 underwent three pathways including hydroxylation of aniline ring, oxidation of aromatic amine group to generate nitro-SMX, and oxidative coupling to generate azo-SMX and hydroxylated azo-SMX. These results obtained in this work improve the understanding of in situ chemical oxidation using PMS for remediation of subsurface, where phenolic and quinonoid moieties are ubiquitous.
研究领域:
环境科学
·
化学
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DOI
PubMed
高影响因子
Journal of Materials Chemistry B
·
2020
·Vol. 8
·期 13
·2598-2606
·
IF 5.344
Zhenzhen Li,Dong Wang,Mingsheng Xu,Jingmin Wang,Xiaolong Hu,Sadat Anwar,Antonio Claudio Tedesco,Paulo Cesar Morais,Hong Bi
Recently, graphene quantum dots (GQDs) have been extensively studied in biomedical areas such as bio-imaging, bio-sensing and photothermal therapy due to their superior optical and physiochemical properties compared to traditional organic biomarkers. Application of GQDs in photodynamic therapy (PDT) has been explored since 2014, but currently the main challenges are inadequate singlet oxygen (1O2) quantum yield (QY), poor solubility and biocompatibility. Herein, we report on the synthesis of a new class of fluorine-containing GQDs (F-GQDs) by an oxidative cutting method using fluorinated graphite as the raw material. The as-synthesized F-GQD sample demonstrates an average particle size of 2.1 nm with a fluorine doping content of 1.43%. The F-GQDs have a better water solubility and biocompatibility than the GQDs, and emit strong green fluorescence at 365 nm excitation with a relative fluorescence QY of 13.72%. Moreover, the fluorescence imaging effect as well as photodynamic activity was successfully tested in both an in vitro HepG2 cell line model and a 3D multicellular spheroid model, the latter of which mimics the tumour microenvironment. Further studies using UV-visible spectroscopy to monitor the degradation of water-soluble 9,10-anthracenediyl-bis(methylene)dimalonic acid (ABDA) demonstrate that the F-GQD sample generates 1O2 efficiently (QY = 0.49) under visible light irradiation. Compared to non-fluorinated GQDs, the as-reported F-GQDs appear to be a more promising photosensitizer for image-guided PDT.
研究领域:
材料科学
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生物医学工程
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纳米技术
·
癌症治疗
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DOI
PubMed
高影响因子
RSC Advances
·
2020
·Vol. 10
·期 34
·19997-20008
·
IF 3.119
Jiayan Zhou,Chunyang Sun,Chunshui Yu
Highly-controllable release consisting of preventing unnecessary drug leakage at physiologically normal tissues and triggering sufficient drug release at tumor sites is the main aim of nanoparticle-based tumor therapy. Developing drug-conjugation strategies with covalent bonds in response to a characteristic stimulus, such as reactive oxygen species (ROS) generated by photodynamic therapy (PDT) has attracted much attention. ROS can not only cause cytotoxicity, but also trigger the cleavage of ROS-responsive linkers. Therefore, it is feasible to design a new model of controlled drug release via the breakage of ROS-responsive linkers and degradation of nanoparticles. The self-supply of the stimulus and highly-controllable drug release can be achieved by encapsulation of photosensitizer (PS) and chemotherapeutic drugs simultaneously without any support of tumor endogenous stimuli. Therefore, we used thioketal (TK) linkers as the responsive linkers due to their reaction with singlet oxygen (1O2, SO), a type of ROS. They were conjugated to the side groups of polyphosphoesters (PPE) via click chemistry to acquire the core cross-linked SO-responsive PPE nanoparticles poly(thioketal phosphoesters) (TK-PPE). TK-PPE coated with the photosensitizer chlorin e6 (Ce6) and chemotherapeutic drug doxorubicin (DOX) simultaneously were prepared and named as TK-PPECe6&DOX. TK-PPECe6&DOX kept stable due to the high stability of the TK-linkers in the normal physiological environment. With self-production of SO as the stimulating factor from the encapsulated Ce6, highly-controlled drug release was achieved. After incubation of tumor cells, 660 nm laser irradiation induced SO generation, resulting in the cleavage of TK-linkers and boosted-release of DOX. Highly-controllable drug release of TK-PPECe6&DOX through self-production of stimulus increased antitumor efficacy, offering a promising avenue for clinical on-demand chemotherapy.
研究领域:
纳米技术
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癌症治疗
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药学
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生物医学工程
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DOI
PubMed
高影响因子
Advanced Fiber Materials
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2025
·
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
研究领域:
环境科学
·
材料化学
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DOI
高影响因子
APPLIED ORGANOMETALLIC CHEMISTRY
·
2026
·Vol. 40
·期 7
·e70612
·
IF 4.3
Danhui Zhao,Jishi Chen,Chuantao Hou
Elucidating the structural evolution of secondary building units (SBUs) in lanthanide-porphyrin frameworks (Ln-PMOFs) remains a compelling challenge in targeted crystal engineering. Herein, a novel 3D framework, QPF-13, featuring unique intermediate-nuclearity Tb 3 and Tb 4 clusters, was synthesized from Tb (III) and tetrakis(3-carboxyphenyl)porphyrin. Significantly, QPF-13 bridges the structural gap between previously established low-nuclearity (Ln 2 ) and high-nuclearity (Ln 7 /Ln 9 ) extremes, successfully completing the SBU evolutionary landscape within this systematic series. Furthermore, the rigid spatial confinement of the porphyrin macrocycles effectively suppresses self-quenching, enabling robust visible-light-driven singlet oxygen generation. Consequently, QPF-13 demonstrates excellent photocatalytic performance in the selective oxidation of 1,5-dihydroxynaphthalene. This work provides deep crystallographic insights into Ln-coordination assembly and establishes a rational structural library for designing advanced photooxidation catalysts.
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DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2026
·
IF 10.6
Qi Huang,Jie Huang,Xin Zhang,Mu-Cen Yao,Yan-Yun Hu,Yi Hu,Zheng- Shuang Hua,Guo-Ping Sheng
Ubiquitous non-photosynthetic microorganisms play a crucial role in the environmental attenuation of contaminants. However, this microbial-driven transformation is often ineffective for bio-inert or bio-toxic emerging contaminants (ECs). Herein, we demonstrated that non-photosynthetic microorganisms such as Escherichia coli , Bacillus subtilis , Shewanella oneidensis and microorganisms from actual waters could produce singlet oxygen ( 1 O 2 ) through photoexcited extracellular metabolites, effectively driving the transformation of ECs such as cimetidine, estriol and sulfamethoxazole. The extracellular metabolites of these non-photosynthetic microorganisms exhibited high photochemical 1 O 2 -producing capability. The quantum yields of 1 O 2 produced by the extracellular metabolites of Escherichia coli , Bacillus subtilis , and Shewanella oneidensis were 25.02 ± 0.95%, 32.65 ± 1.53%, and 16.98 ± 0.37%, respectively, which were comparable to those of photosynthetic microorganisms, and notably higher than that of natural organic matter. For non-photosynthetic microorganisms, low-molecular-weight compounds (<1 kDa) in extracellular metabolites were primarily responsible for 1 O 2 photoproduction. Metabolomics revealed that diverse photosensitizers capable of producing 1 O 2 , such as quinones, aromatic ketones, aromatic aldehydes, quinolines, indoles, aromatic amino acids and derivatives, were present in the extracellular metabolites. This work uncovered an overlooked transformation pathway of emerging contaminants by non-photosynthetic microorganisms, favoring a more accurate evaluation of their fate in environments.
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DOI
PubMed
高影响因子
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