OPTICAL MATERIALS
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2017
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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
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生物医学工程
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纳米技术
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CHEMOSPHERE
·
2023
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IF 8.8
Yifeng Zeng,Fan Wang,Dongqin He,Jun Li,Hongwei Luo,Xiangliang Pan
The activity of iron-based catalysts in advanced oxidation processes (AOPs) is limited by the redox cycle of Fe(III) and Fe(II). In this work, iron oxychloride (FeOCl) with a unique layered structure was loaded on the bone char (BC) to enhance the activation of peroxymonosulfate (PMS). Characterization of the FeOCl-BC catalyst reveals that the loading of FeOCl changed the composition and structure of BC and BC reduced the bond gap of FeOCl. Acetaminophen (APAP) as a target pollutant could be almost completely degraded at neutral pH, and the removal rate reached 0.6597 min −1 . APAP could also be selectively oxidized by FeOCl-BC/PMS system in the presence of some inorganic anions (SO 4 2− , NO 3 − , and Cl − ) and humic acid . Quenching experiments, electron paramagnetic resonance (EPR), chemical probes, and linear sweep voltammetry (LSV) confirm that the primary oxidation mechanism of the FeOCl-BC/PMS system was dominated by 1 O 2 . The 1 O 2 was generated from the conversion of O 2 •− and the self-dissociation of PMS, involving the formation of metastable iron intermediates and the redox cycle of Fe(III) and Fe(II). The unique structure of FeOCl, the transport of lattice oxygen and the enrichment of electrons by carbon defects play an essential role in generating reactive species. In this work, the limitation of the redox cycle of Fe(III) and Fe(II) was broken by loading FeOCl on the surface of BC, and a new catalytic mechanism was proposed. This work provides a new perspective for the construction of efficient iron-based catalysts and the practical application of PMS-based AOPs.
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Biomaterials Science
·
2023
·Vol. 11
·期 20
·6894-6905
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IF 6.6
Wei Zhang,Lu Chen,Xianbin Zhang,Peng Gong,Xiyu Wang,Zhiying Xu,Ganyu Nie,Lu Xu
The application of hybrid nanocarriers is expected to play an active role in improving treatment of chemotherapy and phototherapy. Herein, a nanohybrid with a core of mesoporous silica nanorods and shell of folate-functionalized zeolite imidazole framework (ZIF-8/FA) was synthesized via polydopamine (PDA)-mediated integration. A chemotherapeutic drug (DOX), bubble generator (NH4HCO3, ABC), and photosensitive agent (ICG) were simultaneously loaded into the delivery system to construct smart ZIF-8/FA-coated mesoporous silica nanorods (IDa-PRMSs@ZF). We found that ICG endowed the designed delivery system with a moderate photothermal conversion efficiency of 26.06% and the capacity to release 1O2. The produced hyperthermia caused ABC to decompose and further generate carbon dioxide bubbles, thereby facilitating DOX release, sequentially. Importantly, the underlying mechanism was also investigated using mathematical kinetic modeling. The tumor inhibition rate of IDa-PRMSs@ZF under NIR irradiation reached 83.8%. This study provides a promising strategy based on rod-shaped nanohybrids for effective combination antitumor therapy.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2022
·Vol. 30
·期 7
·17854-17864
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IF 5.19
Li Yi,Xie Shiwei,Yao Jiaxiong
The decay of free radicals involved in side reactions is one of the challenges faced by electrochemical degradation of organic pollutants. To this end, a non-radical oxidation system was constructed by a natural air diffusion cathode (ADC) and a Ti-based dimensional stable anode coated by RuO 2 (RuO 2 -Ti anode) for cathodic hydrogen peroxide activation by anodic chlorine evolution. The ADC fabricated by the carbon black of BP2000 produced a stable concentration of hydrogen peroxide of 339.94 mg L −1 (current efficiency of 73.4%) without aeration, which was superior to the cathode made by the XC72 carbon black. The flow-by ADC-RuO 2 system consisted of an ADC and a RuO 2 -Ti anode showed high selectivity to aniline (AN) compared to benzoate (BA) in a NaCl electrolyte, whose degradation efficiencies were 97.72% and 1.3%, respectively. Rapid degradations of a mixture of emerging pollutants and AN were also observed in the ADC-RuO 2 system, with pseudo-first-order kinetic constants of 0.51, 1.29, 0.89, and 0.99 min −1 for Bisphenol A (BPA), tetracycline (TC), sulfamethoxazole (SMX) and AN, respectively. Quenching experiments revealed the main reactive oxygen species for the pollutant degradation was singlet oxygen ( 1 O 2 ), which was also identified by the electron spin resonance (ESR) analysis. Finally, the steady-stable content of 1 O 2 was quantitatively determined to be 6.25 × 10 −11 M by the method of furfuryl alcohol (FFA) probe. Our findings provide a fast, low energy consumption and well controlled electrochemical oxidation method for selective degradation of organic pollutants. Graphical abstract H 2 O 2 generated on an air diffusion cathode by naturally diffused O 2 , reacts with ClO − produced from chloride oxidation on the RuO 2 -Ti anode to form singlet oxygen ( 1 O 2 ). The electrochemical system shows an efficient oxidation to electron-rich emerging pollutants including bisphenol A, tetracycline, sulfamethoxazole and aniline, but a poor performance on the electron-deficient compounds (e.g., benzoate).
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高影响因子
CARBON
·
2022
·
IF 11.307
Bin Li,Biao Ma,Mengying Wei,Yang Li,Xiaobin Fan,Fengbao Zhang,Guoliang Zhang,Qing Xia,Wenchao Peng
Recycle of the spent lithium-ion batteries (LIBs) can reuse the toxic heavy metals for the synthesis of useful materials. In this study, the cobalt metal is obtained by recycling the cathodes of spent LIBs, which is then used as cobalt source for the synthesis of highly porous Co-NC composites. Attributing to the addition of EDTA-2Na and NaNO 3 as chelate agent and activation agent respectively, very large surface areas (>3700 m 2 /g) and highly porous structure can be achieved. These composites can activate peroxymonosulfate (PMS) effectively for the degradation of bisphenol A (BPA) in aqueous solution. The optimized Co-NC/PMS system also shows good performance in a wide pH range and great tolerance to different inorganic ions and NOMs. Radical scavenging experiments and EPR results prove that 1 O 2 is the only functional reactive oxidation species (ROS) for BPA degradation. A generation route of PMS – *OH – *O – 1 O 2 for 1 O 2 is also simulated and proved by DFT calculation. This work provides a novel way to synthesize effective catalysts for PMS activation from the environmental wastes.
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iScience
·
2022
·
IF 6.107
Zhicong Lu,Peng Zhang,Chun Hu,Fan Li
Summary Persulfate-based nonradical oxidation processes are appealing in water treatment for the efficient and selective degradation of trace contaminants in complex water matrices. However, there is still lacking of systematic understanding of the relationship between multiple nonradical pathways and the active sites of catalyst. Herein, a single-atom Cu catalyst with saturated Cu-N 4 sites on a carbon substrate (SA-Cu-NC) was constructed to activate peroxymonosulfate (PMS), which exhibited high catalytic performance and selectivity for pollutant degradation in different water conditions. Combined with the results of density functional theory (DFT) calculations, the electron-rich area around Cu site and the electron-poor area around C site in the saturated Cu-N 4 configuration could efficiently adsorb and activate PMS, which promoted pollutant degradation through the oxidation of singlet oxygen ( 1 O 2 ) and electron transfer process, respectively. This study advances the understanding of the saturated coordination structure of metals and the superiority of multiple nonradical pathways in wastewater treatment.
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CHEMICAL ENGINEERING JOURNAL
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2021
·
IF 13.273
Zhiqun Xie,Zhiping Lyu,Jinnan Wang,Aimin Li,Philippe François-Xavier Corvini
Ultrafine-Mn 2 O 3 @N-doped porous carbon hybrids [Mn 2 O 3 @NC] derived from Mn-MOFs was constructed with 1 O 2 and O 2 −• as main Reactive oxygen species (ROS). Cation-π bonds and N-Mn complexation induced the formation of electron-rich Mn centre which provided electron for peroxymonosulfate activation to produce radicals, accompanying with generation of 1 O 2 via chain reaction. Notably, the porous structure of N-doped carbon shell could not only facilitate free radical recombination for generation of 1 O 2 but also provide adsorption sites for organics. On the other hand, as electron-poor centre, N-doped carbon shell could improve the electrons transfer from organic intermediate radicals to electron-rich Mn centre via π -π reaction, C-O-Mn and C-N-Mn bonds, which promote the redox of Mn to avoid peroxymonosulfate invalid decomposition. Being attributed to synergistic effects of dual-reaction centres and strong oxidation ability of 1 O 2 , Mn 2 O 3 @NC achieved high mineralization of BPA at low-dose peroxymonosulfate (0.033 g/L).
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ANALYTICAL CHEMISTRY
·
2021
·
IF 6.986
Yunhe Lang,Shihong Wu,Qin Yang,Yanju Luo,Xia Jiang,Peng Wu
D2O plays important roles in a variety of fields (such as the nuclear industry and bioorganic analysis), and thus its isotopic purity (H2O contents) is highly concerned. Due to its highly similar physical properties to H2O and large excess amounts of H2O over D2O, it is challenging to distinguish D2O from H2O. On the basis of the characteristic NIR-II phosphorescence of singlet oxygen (1O2), and the fact that H2O is a more efficient quencher for 1O2 than D2O, here, we proposed to simply use the 1275 nm emission of 1O2 for the analysis of the isotopic purity of D2O. In normal cases (a xenon lamp for excitation), such steady-state emission is extremely weak for valid analytical applications, we thus employed laser excitation for intensification. To this goal, a series of photosensitizers were screened, and eventually polythiophene PT10 was selected with high singlet oxygen quantum yield (ΦΔ = 0.51), high H2O/D2O contrast, and excellent photostability. Upon excitation with a 445 nm laser, a limit of detection (LOD, 3σ) of 0.1% for H2O in D2O was achieved. The accuracy of the proposed method was verified by the analysis of the isotopic purity of several D2O samples (with randomly added H2O). More interestingly, the hygroscopicity of D2O was sensitively monitored with the proposed probe in a real-time manner; the results of which are important for strengthening the care of D2O storage and the importance of humidity control during related investigations. Besides D2O isotopic purity evaluation, this work also indicated the potential usefulness of the NIR-II emission of singlet oxygen in future analytical detection.
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高影响因子
ACS Applied Materials & Interfaces
·
2018
·
IF 8.097
Chengcheng Li,Fengming Lin,Wei Sun,Fu-Gen Wu,Hang Yang,Roujing Lv,Ya-Xuan Zhu,Hao-Ran Jia,Chu Wang,Ge Gao,Zhan Chen
It is of great value to develop new antibacterial photodynamic therapy (PDT) strategies to improve antibacterial PDT efficacy of noncationic photosensitizers without introducing cytotoxicity, which is a great challenge for current leading efforts on antimicrobial PDT based on cell surface engineering. In this research, the hydrophobic and anionic photosensitizer rose bengal (RB) was chemically conjugated with bacterial exopolysaccharide (EPS) to generate an amphiphilic and negatively charged compound EPS-RB that could self-assemble into nanoparticles (NPs) in solution. These EPS-RB NPs possessed an increased singlet oxygen generation property in solution. As a result, EPS-RB exhibited improved photoinactivation for both Gram-negative and Gram-positive bacteria, leading to a record low RB working concentration, 8 μM or 500 nM for Escherichia coli or Staphylococcus aureus, respectively. Upon light irradiation, more EPS-RB bound to the cell surface and penetrated into bacteria than RB, with EPS-RB staying around the cell surface of the most irradiated E. coli while entering all irradiated S. aureus. Both scanning electron microscopy and fluorescence confocal imaging results show that the cell membrane of E. coli was damaged heavily but not S. aureus. All of these observations indicate that both the enhanced singlet oxygen production of EPS-RB NPs in solution and their consequently increased membrane binding and cellular penetration into the bacteria through the damaged cell membrane contribute to their significantly improved bacterial photoinactivation efficiency. In addition, EPS-RB has low cytotoxicity and negligible hemolytic activity, showing great biocompatibility. Therefore, the construction of EPS-RB provides a new strategy for the PDT effectiveness improvement of the separated cell/sensitizer systems and thus the design of next-generation antimicrobial agents.
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International Journal of Nanomedicine
·
2024
·
IF 6.6
Xuliang Guo,Lefei Han,Wenyu Chen,Huixin He,Weijin Zhang,Chaoqi Huang,Xiu Wang
Introduction Combination therapy provides better outcomes than a single therapy and becomes an efficient strategy for cancer treatment. In this study, we designed a hypoxia- and singlet oxygen-responsive polymeric micelles which contain azo and nitroimidazole groups for enhanced cellular uptake, repaid cargo release, and codelivery of photosensitizer Ce6 and hypoxia-activated prodrug tirapazamine TPZ (DHM-Ce6@TPZ), which could be used for combining Ce6-mediated photodynamic therapy (PDT) and PDT-activated chemotherapy to enhance the therapy effect of cancer.Methods The hypoxia- and singlet oxygen-responsive polymeric micelles DHM-Ce6@TPZ were prepared by film hydration method. The morphology, physicochemical properties, stimuli responsiveness, in vitro singlet oxygen production, cellular uptake, and cell viability were evaluated. In addition, the in vivo therapeutic effects of the micelles were verified using a tumor xenograft mice model.Results The resulting dual-responsive micelles not only increased the concentration of intracellular photosensitizer and TPZ, but also facilitated photosensitizer and TPZ release for enhanced integration of photodynamic and chemotherapy therapy. As a photosensitizer, Ce6 induced PDT by generating toxic singlet reactive oxygen species (ROS), resulting in a hypoxic tumor environment to activate the prodrug TPZ to achieve efficient chemotherapy, thereby evoking a synergistic photodynamic and chemotherapy therapeutic effect. The cascade synergistic therapeutic effect of DHM-Ce6@TPZ was effectively evaluated both in vitro and in vivo to inhibit tumor growth in a breast cancer mice model.Conclusion The designed multifunctional micellar nano platform could be a convenient and powerful vehicle for the efficient co-delivery of photosensitizers and chemical drugs for enhanced synergistic photodynamic and chemotherapy therapeutic effect of cancer.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Guanglan Di,Yuwen Wei,Jiaowei Ding,Yu Zhang,Zefang Chen,Xuede Li,Xiangwei Wu,Xiaoli Zhao
Modulating excitonic effects enables the selective activation of O 2 to singlet oxygen ( 1 O 2 ) for efficient degradation of emerging contaminants (ECs) in complex environmental systems. However, the lack of mechanistic investigation in excitonic effect modulation hinders the efficient O 2 activation towards generating preferred reactive oxygen species (ROS). Taking 2D BiOCl as a prototype, we herein propose a facile aluminum (Al) doping method to enhance the inherent excitonic effects of defective BiOCl (BiOCl OV ) and tailor the O 2 activation pathway for 1 O 2 generation. The Al dopants and surface oxygen vacancies (OVs) cooperatively promote O 2 activation, where OVs mainly promote O 2 absorption while Al mainly promote O 2 activation. A new mechanism for 1 O 2 generation driven by a strong excitonic effect has been proposed via experiments and theoretical investigations. Benefiting from the Al-mediated trapping state for singlet exciton, the intersystem crossing is promoted from singlet excitons to triplet excitons because of a lower singlet–triplet energy gap, thereby leading to a selective activation of O 2 to 1 O 2 by resonance energy transfer between triplet excitons and surface absorbed O 2 . Consequently, Al-doped BiOCl OV exhibits a superior activity and stability toward typical ECs degradation in both simulated and real water matrices. This study elucidates the role of the excitonic effect in selectively activating O 2 to 1 O 2 , offering valuable insights for the optimization of exciton-based photocatalysis through atomic-scale design strategies.
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Journal of Materials Chemistry A
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2024
·
IF 10.7
Yuanzhe Zhao,Xiuheng Wang
Singlet oxygen (1O2) is an excellent active species for eliminating organic pollutants in single-atom catalyst (SAC) catalyzed peroxymonosulfate (PMS)-based Fenton-like systems. However, it is difficult to achieve high efficiency and selectivity in 1O2 generation as a result of the lack of effective SACs. In this work, a Co SAC (Co–N–C) containing highly uniform Co–N4 active sites with an ultralow-level Co loading of 0.34 wt% is fabricated, delivering boosted performance in tetracycline degradation with an extremely rapid rate of 0.573 min, which outperforms most advanced catalysts in reported studies. A vibrating-sample magnetometer is used to preliminarily determine the atomically dispersed Co sites in Co–N–C according to the obvious paramagnetic characteristics of Co–N–C, and this is in good agreement with the test results obtained by using an aberration-corrected high-angle annular dark-field scanning transmission electron microscope and synchrotron radiation facility. Electron spin resonance and free radical quenching experiments prove that Co–N–C facilitates PMS activation with the 1O2 generation of almost 100%. Mechanism analyses suggest that the Co–N4 site strengthens the adsorption of the terminal O of PMS, realizing enhanced electron transfer from Co–N–C to PMS, promoting the simultaneous and spontaneous cleavage of O–O and O–H bonds to produce O*, followed by a reaction with another O* to generate 1O2.
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