Small
·
2016
·Vol. 12
·期 39
·5477-5487
·
IF 8.315
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
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肿瘤学
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材料科学
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PubMed
高影响因子
JOURNAL OF CATALYSIS
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2026
·
IF 6
Chaosi Liu,Yijing Gao,Yixiang Niu,Yumei Zhang,Cheng Wang,Tengda Li,Chunhui Xu,Weidong Zhu,Xinqing Lu
Develop Pd-based catalysts for propylene epoxidation with H 2 and O 2. • Sn species in PdSn/Ti-MWW increase the electron density of Pd. • Increased electron density of Pd enhances the H 2 utilization. • Sn significantly promotes the catalytic propylene epoxidation. The low-temperature epoxidation of propylene with H 2 and O 2 to propylene oxide (PO), commonly referred to as the low-temperature HOPO process, over titanosilicate zeolite-supported Pd catalysts is economically attractive and environmentally friendly. However, PO selectivity remains a major challenge for these systems and is comparatively low, because this process is commonly accompanied with propylene hydrogenation to propane. In the present study, a novel and efficient Ti-MWW-supported PdSn catalyst (PdSn/Ti-MWW) was developed for this low-temperature HOPO process, displaying a substantially high PO selectivity. The results on extensive characterizations, in combination with Density Functional Theory (DFT) calculations, for PdSn/Ti-MWW and Pd/Ti-MWW verify that the introduction of Sn species into Pd/Ti-MWW can boost the electron density of Pd species while does not affect the coordination states of Ti species and the textural properties of the zeolite. Interestingly, the enhanced Pd electron density will weaken the adsorption of propylene on the Pd active sites, resulting in inhibiting propylene hydrogenation, which is beneficial for the selective production of PO. Catalytic tests reveal that the optimal 0.33Pd0.22Sn/Ti-MWW catalyst achieves a PO selectivity of 68.4 % and a maximum PO productivity of 7.5 mol g Pd -1 h −1 , far exceeding monometallic Pd/Ti-MWW, while the undesired propane selectivity drops sharply. Moreover, PdSn/Ti-MWW shows an excellent stability and reusability as key catalytic traits. Thus, this work establishes an effective electronic modulation strategy for designing high-performance bimetallic Pd catalysts, and lays solid experimental and theoretical foundations for the industrial application of sustainable low-temperature HOPO technology. Download: Download high-res image (81KB) Download: Download full-size image
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Advanced Materials Interfaces
·
2018
·Vol. 5
·期 22
·1801070
·
IF 4.834
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
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生物化学
·
催化
·
分析化学
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高影响因子
ChemSusChem
·
2023
·
IF 8.4
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.
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高影响因子
COMBUSTION AND FLAME
·
2018
·
IF 4.494
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.
研究领域:
燃烧学
·
化学反应动力学
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高影响因子
Carbon Energy
·
2023
·
IF 20.5
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.
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Nano Research
·
2023
·Vol. 16
·期 5
·6278-6289
·
IF 9.9
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.
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ACS Earth and Space Chemistry
·
2023
·
IF 3.4
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.
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高影响因子
Acta Biomaterialia
·
2022
·
IF 10.633
Furong Liu,Tao He,Songlin Gong,Meiling Shen,Shuang Ma,Xianzhou Huang,Lu Li,Li Wang,Qinjie Wu,Changyang Gong
Combining the internal force-driven chemodynamic therapy (CDT) and the external energy-triggered photodynamic therapy (PDT) holds great promise to achieve an advanced anticancer effect based on reactive oxygen species (ROS). However, the insufficient oxy-substrates supply in tumor microenvironment, like hydrogen peroxide (H 2 O 2 ) and oxygen (O 2 ), is the Achilles heel that greatly restricts the efficacy of this ROS-based treatment. Herein, the construction of a c opper p e roxide-based tumor pH-re s ponsive a utocatalytic nano r eactor (CESAR), via an albumin-mediated biomimetic mineralization strategy is described. The decoration of human serum albumin endows the nanoreactor good hydrophilicity and biocompatibility, which is highly desired for the metal-based materials. Upon exposure to acidic tumor microenvironment, CESAR presents a pH-triggered disintegration with Cu 2+ , H 2 O 2 and O 2 generated instantly. The generated H 2 O 2 complements the hyperoxide deficiency and initiates a localized Fenton-like reaction with the assistance of Cu 2+ for highly toxic hydroxyl radicals (•OH) production for improving CDT. The evolved O 2 gas enables hypoxia relief for enhanced Ce6-mediated PDT. This H 2 O 2 /O 2 self-supplying strategy significantly amplifies the tumor oxidative damage and gains an optimal treatment outcome, which offers a new paradigm for optimizing the tumor therapeutic options limited by oxide or hyperoxide deficiency, not only for CDT/PDT, but also other oxy-substrates involved strategies. Statement of significance The shortage of oxy-substrates in the tumor microenvironment remains a great challenge for ROS-based cancer therapy. Herein, we introduce human serum albumin as a scaffold to stabilize copper peroxide nanomaterials for constant production of H 2 O 2 and O 2 to enhance chemodynamic/photodynamic therapy. The tumor pH-triggered H 2 O 2 /O 2 production and Cu 2+ release are confirmed, assuring the strategy of a highly precise, effective way to destroy tumor without any side effects. This work lends new and exciting insights into the engineering design of autocatalytic oxy-substrates self-supply nanoreactor for overcoming the bottlenecks, like the oxy-substrates deficiency of CDT/PDT and the poor stability of metal peroxides, to achieve highly effective chemodynamic/photodynamic therapy.
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高影响因子
INORGANIC CHEMISTRY COMMUNICATIONS
·
2021
·
IF 2.495
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.
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高影响因子
Science Bulletin
·
2024
·
IF 18.8
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
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电化学
·
能源存储
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高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2022
·
IF 5.518
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
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材料科学
·
化学
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高影响因子
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