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JOURNAL OF NANOBIOTECHNOLOGY · 2024 ·Vol. 22 ·期 1 ·1-15 · IF 10.6

A continuously efficient O2-supplying strategy for long-term modulation of hypoxic tumor microenvironment to enhance long-acting radionuclides internal therapy

Li Jingchao,Wang Tingting,Shi Yuanfei,Ye Zichen,Zhang Xun,Ming Jiang,Zhang Yafei,Hu Xinyan,Li Yun,Zhang Dongsheng,Xu Qianhe,Yang Jun,Chen Xiaolan,Liu Nian,Su Xinhui

Radionuclides internal radiotherapy (RIT) is a clinically powerful method for cancer treatment, but still poses unsatisfactory therapeutic outcomes due to the hypoxic characteristic of tumor microenvironment (TME). Catalase (CAT) or CAT-like nanomaterials can be used to enzymatically decompose TME endogenous H 2 O 2 to boost TME oxygenation and thus alleviate the hypoxic level within tumors, but their effectiveness is still hindered by the short-lasting of hypoxia relief owing to their poor stability or degradability, thereby failing to match the long therapeutic duration of RIT. Herein, we proposed an innovative strategy of using facet-dependent CAT-like Pd-based two-dimensional (2D) nanoplatforms to continuously enhance RIT. Specifically, rationally designed 2D Pd@Au nanosheets (NSs) enable consistent enzymatic conversion of endogenous H 2 O 2 into O 2 to overcome hypoxia-induced RIT resistance. Furthermore, partially coated Au layer afford NIR-II responsiveness and moderate photothermal treatment that augmenting their enzymatic functionality. This approach with dual-effect paves the way for reshaping TME and consequently facilitating the brachytherapy ablation of cancer. Our work offers a significant advancement in the integration of catalytic nanomedicine and nuclear medicine, with the overarching goal of amplifying the clinical benefits of RIT-treated patients. Graphical abstract

研究领域: 肿瘤学 · 纳米医学 · 核医学
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COMBUSTION AND FLAME · 2018 · IF 4.494

Investigation on laminar flame propagation of n-butanol/air and n-butanol/O2/He mixtures at pressures up to 20 atm

Guoqing Wang,Yuyang Li,Wenhao Yuan,Yizun Wang,Zhenbiao Zhou,Yingzheng Liu,Jianghuai Cai

Bio-butanol is an important alternative fuel and has many advantages in engine combustion . In the present work, laminar flame propagation of n- butanol/air and n- butanol/(14% O 2 /86% He) mixtures was investigated using a constant-volume combustion vessel at the unburnt temperature of 423 K, initial pressures of 1–20 atm and a series of equivalence ratios. Flame instabilities of n -butanol, including cellular instability and pulsating instability, were studied based on flame morphology. The unsteady transition from weak flame to normal flame was investigated based on the flame trajectories and this phenomenon became less perceptible in the flame with stronger combustion intensity and smaller Lewis number. The accelerated laminar burning velocity (LBV), thickened flame thickness, larger Markstein length and Markstein number indicate that the thermal diffusivity of n- butanol/O 2 /He flames are greatly enhanced by helium addition. The smaller densities and lower reactant concentrations result in the smaller laminar burning fluxes of n- butanol/O 2 /He flames than those of n -butanol/air flames. The high temperature kinetic model of n -butanol reported by Cai et al. was further developed with recent theoretical progresses on n -butanol reactions. The updated high temperature model was validated on the present experimental data and a vast amount of previous n -butanol combustion data . Sensitivity analysis was performed using the updated model under wide pressure and equivalence ratio ranges. The similarity in the sensitivities indicates that the sensitive reactions in n- butanol/air flames can be validated by using n- butanol/O 2 /He flames, which greatly compensates the problem that the n- butanol/air flames are susceptible to flame instabilities at high pressures. The weaker pressure dependence of the LBVs of n -butanol/O 2 /He flames indicates that their flame chemistry changes less to resist the pressure variation.

CAS / MDL: 71-36-3
研究领域: 燃烧学 · 化学反应动力学
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INORGANIC CHEMISTRY COMMUNICATIONS · 2021 · IF 2.495

A novel nickel complex with 3-Hydroxyflavone: Synthesis, CrystalStructure and reactivity towards O2 of Ni4(C15O3H9)4(CH3O)4(H2O)4

Qian-Qian Huang

A novel tetranuclear nickel(II)-flavonolate complex [Ni II 4 (fla) 4 (CH 3 O) 4 (H 2 O) 4 ] (flaH: 3-Hydroxyflavone, flavonol) was synthesized. Its crystal structure and spectroscopic features have been investigated in details by physicochemical methods and single crystal X-ray diffraction. Different from other mononuclear metal-flavonolate complexes, this complex demonstrates a cluster molecular structure which has four Ni II centers, and each Ni II centre is coordinated by a bidentate flavonolate, three methanol and a water molecule. The crystal of this complex is tetragonal crystal system: space group I 41/a, a = 24.4361(14), b = 24.4361(14), c = 12.7972 (14), α = β  =  γ =  90 ° , V = 7641.5 (12), Z = 4. The complex can react with O 2 , in other words, it has enzymatic reactivity just like enzyme-substrate model of quercetin 2,3-dioxygenase, and the reaction products are similar with the other reported enzyme-substrate models.

CAS / MDL: 577-85-5 6018-89-9
研究领域: 化学 · 材料科学 · 生物化学
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Advanced Materials Interfaces · 2018 ·Vol. 5 ·期 22 ·1801070 · IF 4.834

A Novel AuNP-Based Glucose Oxidase Mimic with Enhanced Activity and Selectivity Constructed by Molecular Imprinting and O2-Containing Nanoemulsion Embedding

Lin Fan,Doudou Lou,Haoan Wu,Xizhi Zhang,Yefei Zhu,Ning Gu,Yu Zhang

In spite of the competitive advantages, inorganic nanoparticle mimic enzymes exhibit inherent disadvantages of limited catalytic efficiency and lacking selectivity. Here, a gold nanoparticle (AuNP)-based mimic enzyme with significantly enhanced glucose selectivity and catalytic activity is constructed and demonstrated for the first time. Aminophenylboronic acid is employed to increase the affinity to glucose, as well as build molecular imprinted polymer shells to realize the selectivity for template molecules of glucose. Besides that, heptadecafluoro- n -octyl bromide nanoemulsion with the function of providing oxygen is introduced to gain a further improvement in catalytic activity, which successfully enhances the catalytic efficiency ( k cat / K m ) up to about 270-fold. Based on the demonstrated catalytic properties, AuNP-based glucose oxidase mimics are successfully applied in practical glucose detection of drinks and blood glucose.

研究领域: 纳米技术 · 生物化学 · 催化 · 分析化学
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Nano Research · 2023 ·Vol. 16 ·期 5 ·6278-6289 · IF 9.9

Au/TS-1 catalyst for propylene epoxidation with H2 and O2: Effect of surface property and morphology of TS-1 zeolite

Xu Jialun,Zhang Zhihua,Yu Daiyi,Du Wei,Song Nan,Duan Xuezhi,Zhou Xinggui

The catalytic performances over propylene epoxidation with H 2 and O 2 (HOPO process) are significantly affected by the properties (e.g., surface properties, Ti coordination, and morphology) of titanosilicate zeolite. Introducing urea into zeolite synthesis is a simple and convenient method to modify these properties of titanosilicate zeolite. Uncalcined pore-blocked titanium silicalite-1 (TS-1, i.e., TS-1-B) with the lower urea dosage possesses more defective structure and unsaturated coordinated Ti sites verified by 29 Si nuclear magnetic resonance (NMR) and X-ray photoelectron spectroscopy (XPS) analysis, which results in a high initial activity and hydrogen efficiency; while the high surface acidity generated by these Ti species leads to a continuous decrease in the activity and the propylene oxide (PO) selectivity during the reaction. As the amount of urea gradually increases, the TS-1-B samples present the reduced surface defects and defective and unsaturated Ti species. Specially, TS-1-B-0.30U presents the weaker PO adsorption on PO-diffusion reflectance infrared Fourier transform spectra (DRIFTS), and thus results in the high stable PO formation rate and selectivity over its Au catalyst. Furthermore, a flat-plate-like shape with a shorter thickness of 100 nm along the b-axis direction is observed on the urea-modified TS-1. Compared with the conventional ellipsoidal TS-1 with crystal sizes of 200 and 500 nm, the flat-plate-like TS-1-0.30U displays the less surface defects, unsaturated Ti species, and the weaker Lewis acid, which is favorable for the desorption and intracrystalline diffusion of PO, thus reduces the occurrence of side reactions for the improved selectivity and stability. This work may provide a reference for developing titanium-containing materials with high activity and stability over HOPO reaction.

CAS / MDL: 57-13-6
研究领域: 催化化学 · 材料科学
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Small · 2016 ·Vol. 12 ·期 39 ·5477-5487 · IF 8.315

FeIII-Doped Two-Dimensional C3N4 Nanofusiform: A New O2-Evolving and Mitochondria-Targeting Photodynamic Agent for MRI and Enhanced Antitumor Therapy

Zhifang Ma,Mengchao Zhang,Xiaodan Jia,Jing Bai,Yudi Ruan,Chao Wang,Xuping Sun,Xiue Jiang

Local hypoxia in tumors, as well as the short lifetime and limited action region of 1 O 2 , are undesirable impediments for photodynamic therapy (PDT), leading to a greatly reduced effectiveness. To overcome these adversities, a mitochondria-targeting, H 2 O 2 -activatable, and O 2 -evolving PDT nanoplatform is developed based on Fe III -doped two-dimensional C 3 N 4 nanofusiform for highly selective and efficient cancer treatment. The ultrahigh surface area of 2D nanosheets enhances the photosensitizer (PS) loading capacity and the doping of Fe III leads to peroxidase mimetics with excellent catalytic performance towards H 2 O 2 in cancer cells to generate O 2 . As such tumor hypoxia can be overcome and the PDT efficacy is improved, whilst at the same time endowing the PDT theranostic agent with an effective T 1 -weighted in vivo magnetic resonance imaging (MRI) ability. Conjugation with a mitochondria-targeting agent could further increase the sensitivity of cancer cells to 1 O 2 by enhanced mitochondria dysfunction. In vitro and in vivo anticancer studies demonstrate an outstanding therapeutic effectiveness of the developed PDT agent, leading to almost complete destruction of mouse cervical tumor. This development offers an attractive theranostic agent for in vivo MRI and synergistic photodynamic therapy toward clinical applications.

研究领域: 生物医学工程 · 肿瘤学 · 材料科学
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ACS Earth and Space Chemistry · 2023 · IF 3.4

Differences in the Oxidizing Species on the Surface of Metal-Doped Ferrihydrite and Hematite in the Alkaline S(IV)-O2 Solution

Hao Tian,Xue-Bin Zhang,Yin-Ping Li,Qing He,Na-Na Tian,Song-Hai Wu,Xu Han

Although inorganic Fe(IV)═O oxo and Fe(III)-OOH peroxo have attracted more attention in aqueous environments, direct evidence for the characterization and identification of those oxidizing species is still lacking. In this study, the doped Cu/Co increases the reactivity of ferrihydrite/hematite in oxidizing As(III) by S(IV)-O2 under alkaline and dark conditions. Quenching experiments exclude the contributions of ·OH, O2•–, SO3•–, SO4•–, SO5•–, HSO5–, and H2O2 and confirm that peroxo and oxo are primary oxidizing species in As(III) oxidation. Electrochemical analyses indicate that Fe(IV)═O oxo and Fe(III)-OOH peroxo are primarily located on the surface of ferrihydrite and hematite. Selective oxidation of methyl phenyl sulfoxide and methyl phenyl sulfide to the corresponding oxidation products further reveals the presence of ≡Fe(IV)═O oxo on both ferrihydrite and hematite, and the doped Cu/Co significantly decreases the produced ≡Fe(IV)═O oxo on ferrihydrite, while increases the produced ≡Fe(IV)═O oxo on hematite. Meanwhile, selective oxidation of benzyl alcohol to benzaldehyde indicates the presence of ≡Fe(III)-OOH peroxo on both ferrihydrite and hematite, and the doped Cu/Co apparently increases the produced ≡Fe(III)-OOH peroxo on ferrihydrite and hematite. Raman analysis further reveals the presence of ≡Fe(IV)═O oxo and ≡Fe(III)-OOH peroxo on pure and metal-doped ferrihydrite/hematite, which also confirms that the doped Cu/Co decreases the produced ≡Fe(IV)═O oxo on ferrihydrite and increases ≡Fe(IV)═O oxo on hematite, while apparently increasing ≡Fe(III)-OOH peroxo on both ferrihydrite and hematite. This study enriches our understanding on the oxidizing species in the S(IV)-mediated oxidation processes under alkaline conditions, providing new insight on the oxidation reactivity of surface peroxo and oxo species mediated by the doped metal ions.

研究领域: 环境科学 · 化学
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ChemSusChem · 2023 · IF 8.4

Elastic and Conductive Cross-linked Anion Exchange Membranes Based on Polyphenylene Oxide and Poly(vinyl alcohol) for H2-O2 Fuel Cells

Juanjuan Han,Yangyang Zhang,Xiumeng Zheng,Yuyang Lu,Wanting Li,Xiaorong Zhou,Zhandong Ren,Yi Liu,Meixue Hu,Li Xiao,Lin Zhuang

Graphical A novel AEM with good strength and flexibility was synthesized by combining rigid PPO and flexible PVA. Dual cationic groups were added to improve ion concentration and create ion channels, enhancing ion conductivity. Cross-linking and phase separation improved the AEM's resistance to alkali. A series of cross-linked AEMs ( c -DQPPO/PVA) are synthesized by using rigid polyphenylene oxide and flexible poly(vinyl alcohol) as the backbones. Dual cations are grafted on the PPO backbone to improve the ion exchange capacity (IEC), while glutaraldehyde is introduced to enhance compatibility and reduce swelling ratio of AEMs. In addition to the enhanced mechanical properties resulting from the rigid-flexible cross-linked network, c -DQPPO/PVA AEMs also exhibit impressive ionic conductivity, which can be attributed to their high IEC, good hydrophilicity of PVA, and well-defined micro-morphology. Additionally, due to confined dimension behavior and ordered micro-morphology, c -DQPPO/PVA AEMs demonstrate excellent chemical stability. Specifically, c -DQPPO/PVA-7.5 exhibits a wet-state tensile strength of 12.5 MPa and an elongation at break of 53.0 % at 25 °C. Its OH − conductivity and swelling degree at 80 °C are measured to be 125.7 mS cm −1 and 8.2 %, respectively, with an IEC of 3.05 mmol g −1 . After 30 days in a 1 M NaOH solution at 80 °C, c -DQPPO/PVA-7.5 experiences degradation rates of 12.8 % for tensile strength, 27.4 % for elongation at break, 14.7 % for IEC, and 19.2 % for ion conductivity. With its excellent properties, c -DQPPO/PVA-7.5 exhibits a peak power density of 0.751 W cm −2 at 60 °C in an H 2 -O 2 fuel cell.

CAS / MDL: 9002-89-5
研究领域: 材料科学 · 能源工程
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Carbon Energy · 2023 · IF 20.5

Evolution of the porous structure for phosphoric acid etching carbon as cathodes in Li–O2 batteries: Pyrolysis temperature-induced characteristics changes

Feiyang Yang,Ying Yao,Yunkai Xu,Cong Wang,Meiling Wang,Jingjie Ren,Cunzhong Zhang,Feng Wu,Jun Lu

Although biomass-derived carbon (biochar) has been widely used in the energy field, the relation between the carbonization condition and the physical/chemical property of the product remains elusive. Here, we revealed the carbonization condition's effect on the morphology, surface property, and electrochemical performance of the obtained carbon. An open slit pore structure with shower-puff-like nanoparticles can be obtained by finely tuning the carbonization temperature, and its unique pore structure and surface properties enable the Li–O 2 battery with cycling longevity (221 cycles with 99.8% Coulombic efficiency at 0.2 mA cm −2 and controlled discharge–charge depths of 500 mAh g −1 ) and high capacity (16,334 mAh g −1 at 0.02 mA cm −2 ). This work provides a greater understanding of the mechanism of the biochar carbonization procedure under various pyrolysis conditions, paving the way for future study of energy storage devices.

CAS / MDL: 9014-63-5
研究领域: 材料科学 · 能源存储
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS · 2022 · IF 5.518

Fabrication of beta zeolite supported Ti3+-TiO2/CdS composite for ultrahigh-performance photodegradation of tetracycline under visible-light illumination

Wenjing Shen,Dandan Xiang,Junnan Yang,Yanting Tang,Changhui Xin,Quanhui Guo,Xin Yu

In this work, beta zeolite supported Ti 3+ -TiO 2 /CdS heterojunction was prepared for photodegradation of tetracycline under visible-light irradiation, and zeolite served as a support for the high dispersions of the Ti 3+ -TiO 2 nanoparticles . The obtained zeolite/Ti 3+ -TiO 2 /CdS heterojunction showed a relatively high surface areas of approximately 63.2 m 2 g −1 , much higher than those of the prepared Ti 3+ -TiO 2 /CdS (27.1 m 2 g −1 ), Ti 3+ -TiO 2 (36.5 m 2 g −1 ), and CdS (31.1 m 2 g −1 ), strongly demonstrating the significant of zeolite for high dispersion of the Ti 3+ -TiO 2 /CdS composite. Besides, the experimental results also showed that the photocatalytic degradation efficiency could reach 78 % in 3 min for the zeolite/Ti 3+ -TiO 2 /CdS heterojunction, and the corresponding rate constant was as high as 0.788 min −1 , which was 26.90 times that of pristine Ti 3+ -TiO 2 , 2.24 times of pristine CdS , and 2.04 times of the Ti 3+ -TiO 2 /CdS composite, mainly because of the supporting effects of zeolite and the formation of Ti 3+ -TiO 2 /CdS heterostructure for highly enhanced charge separation. In addition, the trapping experiment revealed that the main reactive species involved in tetracycline degradation were attributed to the photo-generated holes and ⸱O 2 - species.

研究领域: 环境科学 · 材料科学 · 化学
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Science Bulletin · 2024 · IF 18.8

Hybrid ion/electron interfacial regulation stabilizes the cobalt/oxygen redox of ultrahigh-voltage lithium cobalt oxide for fast-charging cyclability

Zhihong Bi,Anping Zhang,Gongrui Wang,Cong Dong,Pratteek Das,Xiaoyu Shi,Zhong-Shuai Wu

High-voltage and fast-charging LiCoO 2 (LCO) is key to high-energy/power-density Li-ion batteries. However, unstable surface structure and unfavorable electronic/ionic conductivity severely hinder its high-voltage fast-charging cyclability. Here, we construct a Li/Na-B-Mg-Si-O-F-rich mixed ion/electron interface network on the 4.65 V LCO electrode to enhance its rate capability and long-term cycling stability. Specifically, the resulting artificial hybrid conductive network enhances the reversible conversion of Co 3+/4+ /O 2−/ n − redox by the interfacial ion–electron cooperation and suppresses interface side reactions, inducing an ultrathin yet compact cathode electrolyte interphase. Simultaneously, the derived near-surface Na + /Mg 2+ /Si 4+ -pillared local intercalation structure greatly promotes the Li + diffusion around the 4.55 V phase transition and stabilizes the cathode interface. Finally, excellent 3 C (1 C = 274 mA g −1 ) fast charging performance is demonstrated with 73.8% capacity retention over 1000 cycles. Our findings shed new insights to the fundamental mechanism of interfacial ion/electron synergy in stabilizing and enhancing fast-charging cathode materials.

研究领域: 材料科学 · 电化学 · 能源存储
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Environmental Science and Ecotechnology · 2021 · IF 0

Fabrication of AQ2S/GR composite photosensitizer for the simulated solar light-driven degradation of sulfapyridine

Shuang-Yang Zhao,Cheng-Xin Chen,Jie Ding,Shan-Shan Yang,Ya-Ni Zang,Xu-Dong Qin,Xin-Lei Gao,Zhao Song,Nan-Qi Ren

Chlorination has been intensively investigated for use in water disinfection and pollutant elimination due to its efficacy and convenience; however, the generation and transportation of chlorine and hypochlorite are energy-consuming and complicated. In this study, a novel binary photosensitizer consisting of anthraquinone-2-sulfonate (AQ2S) and graphene was synthesized via a π-π stack adsorption method; this compound could allow for the chlorination of organic pollutants using on-site chlorine generation. In this photosensitive degradation process, sulfapyridine (SPY) was selected as a model pollutant and was decomposed by the reactive species (Cl 2 •- , Cl • and O 2 •- ) generated during the photosensitive oxidation of chloride. The synthesized AQ2S/graphene exhibited superior activity, and the degradation rate of SPY was over 90 % after 12 h of visible light irradiation with a kinetic constant of 0.2034h −1 . Results show that 20 mg AQ2S/GR at a 21 % weight percentage of AQ2S in a pH 7 SPY solution with 1 mol/L Cl − achieved the highest kinetics rate at 0.353 h −1 . Free radical trapping experiments demonstrated that Cl 2 •- and O 2 •- were the dominant species involved in SPY decomposition under solar light. The reusability and stability of this composite were verified by conducting a cycle experiment over five successive runs. The capacity of photodegradation still remained over 90 % after these 5 runs. The current study provides an energy-efficient and simple-operational approach for water phase SPY control.

研究领域: 环境科学 · 水处理 · 光催化 · 污染物降解
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