JOURNAL OF HAZARDOUS MATERIALS
·
2021
·
IF 10.588
Qingdong Qin,Ting Liu,Jiaxuan Zhang,Rui Wei,Shijie You,Yan Xu
Hematite (α-Fe 2 O 3 ) has been commonly used as an eco-friendly catalyst for peroxymonosulfate (PMS) to generate free radicals (SO 4 •- and/or •OH). However, the activation efficiency of PMS relies heavily on the conversion of Fe(III) to Fe(II) that is slow and rate-limiting. In this study, oxygen vacancies enriched α-Fe 2 O 3 was prepared from thermally treated goethite (α-FeOOH) and employed as a PMS activator. Systematic characterization demonstrated that α-Fe 2 O 3 with most abundant oxygen vacancies could be obtained by heating α-FeOOH at 300 °C. The as-prepared α-Fe 2 O 3 exhibited excellent catalytic activity in activation of PMS for oxidation of sulfamethoxazole (SMX, k = 0.04 min −1 ). The SMX degradation rate was found to be positively correlated with the concentration of oxygen vacancies. Quenching experiments, EPR, LC/MS and XPS analysis revealed that singlet oxygen ( 1 O 2 ) was the predominant reactive oxygen species . The effects of pH, PMS dosage, catalyst loading, temperature, and anions on SMX degradation were comprehensively investigated. Moreover, the plausible degradation pathways of SMX in the α-Fe 2 O 3 /PMS system were proposed. This work not only provides a valuable insight into the mechanism of PMS activation by α-Fe 2 O 3 but also establishes a new strategy for the design of more efficient and practical iron-based catalyst for PMS activation.
研究领域:
环境科学
·
催化化学
✓ 已验证
DOI
高影响因子
JOURNAL OF CATALYSIS
·
2022
·
IF 8.047
Tianliang Lu,Zhiyun Yang,Hongji Li,Haijun Chen,Jun Xu,Chunbao Charles Xu,Jianshe Wang,Zhongjun Li,Yongsheng Zhang
Selective oxidation of ethyl lactate (EL) with molecular oxygen as oxidant is an alternative route to produce ethyl pyruvate (EP). However, to obtain pyruvate with high yield under mild conditions remains challenging due to the troublesome over oxidation issue. Here, a highly efficient photocatalytic strategy was firstly developed to obtain EP at room temperature. ZnIn sulfides (ZIS) with different Zn/In ratios were synthesized as the catalysts. Under the irradiation of visible light, 100% EL conversion with 88.4% EP yield could be obtained. The optimized ZIS catalyst shows the highest surface area (215.7 m 2 g −1 ) as well as much higher separation and transport efficiency of the electron-hole pairs. Combining radical trapping experiments with characterization results, a reaction mechanism was proposed. The mild reaction conditions with efficient generation of singlet oxygen contribute the high yield of EP. Kinetic isotope experiments indicate that the cleavage of C(OH)−H bond probably was involved in the rate determining step.
研究领域:
化学工程
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材料科学
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环境科学
✓ 已验证
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
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
✓ 已验证
DOI
高影响因子
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
·
2024
·Vol. 121
·期 30
·e2401452121
·
IF 9.4
Shujun Liu,Hong Wang,Zehui Hu,Xin Zhang,Yanjuan Sun,Fan Dong
Nitrophenols present on the surface of particulates are ubiquitous in the atmosphere. However, its atmospheric photochemical transformation pathway remains unknown, for which the crucial effect of visible light is largely overlooked, resulting in an incomplete understanding of the effects of nitrophenols in the atmospheric environment. This study delves into the photolysis mechanism of 4-nitrophenol (4NP), one of the most abundant atmospheric nitrophenol compounds, on the surface of photoactive particulates under visible light irradiation. Unexpectedly, the nonradical species (singlet oxygen, 1O2) was identified as a dominant factor in driving the visible photolysis of 4NP. The pathways of HONO and p-benzoquinone (C6H4O2) generation were clarified by acquiring direct evidence of C–N and O–H bond breakage in the nitro (–NO2) and hydroxyl (–OH) groups of 4NP. The further decomposition of HONO results in the generation of NO and hydroxyl radicals, which could directly contribute to atmospheric oxidizing capacity and complicate the PM2.5 composition. Significantly, the behavior of 1O2-induced visible photolysis of 4NP was universal on the surface of common particulates in the atmosphere, such as A1 dust and Fe2O3. This work advances the understanding of the photochemical transformation mechanism of particulate-phase atmospheric nitrophenols, which is indispensable in elucidating the role of nitrophenols in atmospheric chemistry.
研究领域:
环境科学
·
大气化学
✓ 已验证
DOI
高影响因子
Journal of Water Process Engineering
·
2024
·
IF 6.3
S. Jafari,A.R. Faraji,A. Gil,F. Ashouri
Valorizing single-use plastic waste as an effective activator in environmental protection has gained great interest from policymakers, legislators, and scientific research communities. Herein, low-cost and highly porous alkali Fe/Mn-doped carbon nanomaterials derived from polyethylene terephthalate (PET) waste (MF/ c PET- x ) were fabricated via facile pyrolysis and alkali-metal impregnation methods. Detailed characterizations of MF- c PET- x demonstrated that the ratio of alkaline impregnation and pyrolysis temperature affects the porous characteristics, content, and size of active sites, specific surface area, and yield of carbon residue/nanocomposite. The main aim of this study was to evaluate and optimize the MF/ c PET- x applied for the detoxification of various kinds of pharmaceutical drugs ( tetracycline , naproxen , paracetamol , and levofloxacin ) and various dyestuff in their single, binary, ternary, and quaternary solutions. The magnetic porous MF/ c PET-1 was found to show a most effective PMS activation for single/multiple toxic pollutants removal attaining levels >91.0 % in a wide range of temperatures (5–35 °C) and pH (3.0–9.0), without significant detectable metal leaching (>0.16 mg L −1 ). The outstanding catalytic performance in complex water environments was mainly attributed to the deposition of Mn/Fe nanoparticles with small grain size on a polymeric scaffold, bimetal synergistic effect, high specific surface area, high stability, and excellent anti-interference capability against coexisting substances. Physicochemical properties of the recycled composite, masking, and EPR analyses confirmed that the dominant reactive species in the following order: 1 O 2 > OH > SO 4 − > O 2 − . This work offers a new and straightforward approach for preparing porous alloy composite from plastic waste for pollutant degradation in various water matrices.
研究领域:
环境科学
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材料科学
✓ 已验证
DOI
高影响因子
BIOCONJUGATE CHEMISTRY
·
2018
·
IF 4.485
Zheng Ruan,Wei Miao,Pan Yuan,Liu Le,Lijuan Jiao,Erhong Hao,Lifeng Yan
NIR photosensitizer is attractive for photodynamic therapy (PDT). Low-power light irradiation and imaging-guided PDT makes it possible to increase tissue penetration depth. The pyrrole-substituted iodinated BODIPY (BDPI) molecule was designed and synthesized, and it possesses an intense NIR absorption and emission band, and exhibits a high singlet oxygen quantum yield (ΦΔ = 0.80) which leads remarkable cytotoxicity upon low power illumination (IC50 = 0.60 μg/mL, 6.1 mW/cm2). After being encapsulated with biocompatibility polypeptide PEG–PLys, polymeric micelles nanoparticles (PBDPI NPs) was obtained that are water-dispersed and passively tumor-targetable. Such enhanced accumulation in tumor area makes it easily traced in vivo due to its NIR fluorescence. In addition, such nanoparticles offer an unprecedented photodynamic therapeutic effect by using a low-power irradiation light, which makes it possible to kill cancer cells in deep tissue efficiently.
研究领域:
生物医学工程
·
肿瘤学
·
材料科学
✓ 已验证
DOI
高影响因子
DYES AND PIGMENTS
·
2019
·
IF 4.018
Jinjin Guo,Xiaoyu Wang,Shuxian Zhu,Lu Liu,Xiaofeng Jiang,Dongdong Ban,Lidong Li
We combined the unique natural oxygen transporting function of red blood cells (RBCs) with photosensitive nanocomposites to create biomaterials with strong singlet oxygen ( 1 O 2 ) generation. During cold storage for a long time, structural changes to RBCs may occur, which reduce their oxygen carrying capacity. The nanocomposite developed herein featured dual emission characteristic, which enabled evaluation of the status of the RBCs. On the basis of energy transfer from the conjugated polymer to iridium(III) complexes, the formed nanocomposites show intense, long-lived and oxygen-sensitive emission. When modified with 1,2-distearoyl- sn -glycero-3-phosphoethanolamine- N -[methoxy(polyethyleneglycol)-2000], the nanocomposites non-invasively entered RBCs through hydrophobic interactions . We measured the quenching effect of oxygen on the emission of the iridium(III) complexes. The differential fluorescent signals and fluorescence lifetime images indicated the storage history of the RBCs. RBCs in good condition stored oxygen. When engineered with nanocomposites, RBCs generated large amounts of cytotoxic 1 O 2 upon irradiation. These decorated RBCs might serve as a new kind of photosensitive biomaterial.
研究领域:
生物材料学
·
医学工程
·
光动力治疗
✓ 已验证
DOI
高影响因子
CARBOHYDRATE RESEARCH
·
2021
·
IF 2.104
Xinyan He,Jun Hong,Shengping Liu,Defeng Xu,Hang Hu
In the present work, hydroxyethyl starch-new indocyanine green (HES-IR-820) conjugates were developed for enhanced cancer photodynamic therapy . HES-IR-820 conjugates were prepared by the condensation reaction between IR-820 and amino groups modified HES. HES-IR-820 conjugates with IR-820 loading content of 2.0% (HES-IR-820 2.0 ) and 3.2% (HES-IR-820 3.2 ) were prepared and characterized by 1 H NMR, FT-IR, HPLC, and UV–Vis. HES-IR-820 2.0 and HES-IR-820 3.2 are monomolecular nanosized particles with hydrodynamic diameters of around 10 nm. HES-IR-820 2.0 and HES-IR-820 3.2 exhibit significantly enhanced stability in pH 7.4 PBS buffer and pH 7.4 PBS buffer containing 10% fetal bovine serum as compared to free IR-820. HES-IR-820 2.0 and HES-IR-820 3.2 show limited drug release in pH 7.4 and pH 5.0 PBS buffer. HES-IR-820 2.0 and HES-IR-820 3.2 exhibit enhanced singlet oxygen generation under 808 nm laser irradiation and reduced cellular uptake amount as compared to free IR-820. The cellular uptake pathway study reveals that the lipid raft-mediated endocytosis and macropinocytosis are involved in the cellular uptake of HES-IR-820 2.0 and HES-IR-820 3.2 . Compared to free IR-820, HES-IR-820 2.0 and HES-IR-820 3.2 show reduced cytotoxicity, enhanced in vitro antitumor effect under 0.3 W/cm 2 808 nm laser irradiation, and similar in vitro antitumor effect under 0.6 W/cm 2 808 nm laser irradiation. HES-IR-820 conjugates show significant potential for cancer photodynamic therapy.
研究领域:
肿瘤学
·
药剂学
·
生物医学工程
✓ 已验证
DOI
高影响因子
JOURNAL OF BIOMATERIALS APPLICATIONS
·
2024
·
IF 2.3
Yang Sheng,Danni Qing,Naijun Li,Peng Zhang,Yixin Sun,Rong Zhang
Zn-Ag-In-S (ZAIS) quantum dots (QDs) were synthesized with various Ag-to-In ratios and used as novel photosensitizers for photodynamic therapy (PDT) on cancer cell inhibition and bacterial sterilization, and their structural, optical, and photodynamic properties were investigated. The alloyed QDs displayed a photoluminescence quantum yield of 72% with a long fluorescence lifetime of 5.3 μs when the Ag-to-In ratio was 1:3, suggesting a good opportunity as a dual functional platform for fluorescence imaging and PDT. The ZAIS QDs were then coated with amphiphilic brush copolymer poly(maleic anhydride-alt-1-octadecene) (PMAO) before application. The 1O2 quantum yield of the ZAIS/PMAO was measured to be 8%, which was higher than previously reported CdSe QDs and comparable to some organic photosensitizers. Moreover, the ZAIS QDs showed excellent stability in aqueous and biological media, unlike organic photosensitizers that tend to degrade over time. The in vitro PDT against human melanoma cell line (A2058) and Staphylococcus aureus shows about 30% inhibition rate upon 20 min light irradiation. Cell staining images clearly demonstrated that co-treatment with ZAIS QDs and light irradiation effectively killed A2058 cells, demonstrating the potential of ZAIS QDs as novel and versatile photosensitizers for PDT in cancer and bacterial treatment, and provides useful information for future designing of QD-based photosensitizers.
研究领域:
生物医学工程
·
材料科学
·
肿瘤学
·
微生物学
✓ 已验证
DOI
PubMed
高影响因子
OPTICAL MATERIALS
·
2017
·
IF 2.238
Jinxue Liu,Tingbin Zhang,Xiaoyan Song,Jinfeng Xing
With the aim to enhance the upconversion luminescence (UCL) intensity, much attention was paid to reduce the energy-back transfer from Er 3+ ions to Nd 3+ ions by constructing various kinds of multilayer upconversion nanoparticles (UCNPs). However, the energy-back transfer was difficult to be completely eliminated. Also, the thick shell of multilayer UCNPs is not favourable for effective Förster resonance energy transfer (FRET) in photodynamic therapy (PDT) system. Herein, an effective and facile method was applied to prepare UCNPs by optimizing the composition to largely enhance the red emission (at 660 nm) for efficient generation of singlet oxygen ( 1 O 2 ). In detail, the concentrations of Nd 3+ ions and Yb 3+ ions doped in the sensitizing shell were systematically researched to balance the energy back-transfer and the light harvest ability. The optimal emission and a relatively high Red/Green (R/G) ratio of NaYF 4 :Yb,Er,Nd@NaYF 4 :Yb 0.1 Nd 0.2 UCNPs were obtained simultaneously. Furthermore, the emission under 980 nm excitation demonstrated the energy back-transfer from Er 3+ to Yb 3+ ions was also notable which was largely ignored previously. Then, UCNPs were encapsulated into mesoporous silica shell, and the photosensitizer Chlorin e6 (Ce6) was covalently conjugated to form a non-leaking nanoplatform. The efficiency of 1 O 2 generation obviously increased with the enhanced emission of UCNPs.
研究领域:
材料科学
·
生物医学工程
·
纳米技术
✓ 已验证
DOI
高影响因子
ACS Applied Bio Materials
·
2021
·
IF 0
Xiaoxiao Hu,Qiang Zhang,Xiaomei Dai,Junyong Sun,Feng Gao
The pH environment in cancer cells has been demonstrated to display vital influences on the therapeutic effect of photodynamic therapy (PDT). It is very interesting to develop pH-responsive probes for simultaneous pH sensing and dynamics monitoring of the effects of PDT, and therefore assessing the correlation between them. In this study, a multifunctional fluorescence probe, dual-emission carbonized polymer dot (CPD) in blue and red regions, which uses ethylene imine polymer (PEI) and 4,4′,4″,4‴-(porphine-5, 10, 15, 20-tetrayl) tetrakis (benzoic acid) (TCPP) as precursors through a one-step hydrothermal amide reaction, has been designed for ratiometric pH sensing, generating pH-dependent 1O2 for PDT of cancer cells, and investigating the dynamics effects of PDT through pH-guided imaging. The prepared CPDs were successfully used for ratiometric pH response, pH-dependent generation of 1O2, and dynamics monitoring PDT in HeLa cells. This study may provide an alternative strategy to prepare CPD-based theranostic integrated nanoprobes for PDT through the rational design of precursors.
研究领域:
生物医学工程
·
肿瘤学
·
纳米医学
✓ 已验证
DOI
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
·
生物医学工程
·
免疫学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）