ACS Applied Polymer Materials
·
2022
·
IF 4.855
Xue Lan,Wenjing Sun,Xin Wang,Wei Xu,Yoji Horii,Jiandang Liu,Hongjun Zhang,Bangjiao Ye,Tiancheng Mu,Xiaozheng Lan
We demonstrate anion (chloride and fluoride ions) transfer in an organic ionic plastic crystal (OIPC), diethyldimethylammonium d-camphorsulfonate, and the role of defects in ion conduction. The phase transitions, crystalline structures, dynamics, and ion transfer mechanisms of the pure material and the doped mixtures were investigated using a combination of differential scanning calorimetry, X-ray diffraction, solid-state nuclear magnetic resonance spectroscopy, and electrochemical impedance spectroscopy. The doped mixtures show minor modifications in thermal behaviors and solid phase structures to the host material. The ion mobility of the pure material in the plastic phase was assigned mainly to cations. The fluoride salt-doped mixture has drastically enhanced conductivity at all tested temperatures, and the chloride salt-doped mixture displays a strong temperature-dependent behavior. Ionic conductivity measurements suggest transfer mechanisms through crystalline phases. The pure material and doped mixtures exhibit similar defect volumes and concentrations, and both factors are phase-dependent, as determined using positron annihilation lifetime spectroscopy. The conductivity displays dependence on not only the defect volume but also the target ion volume. The relationships between the defect volume and the conductivity qualitatively follow the Cohen–Turnbull free volume model, while critical volumes were very large. For the first time in OIPCs, the size of the target ions was found to significantly influence ionic conductivity.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Shaoda Huang,Jinyan Wang,Hongyin Hu,Yang Li,Fangping Xu,Fang Duan,Han Zhu,Shuanglong Lu,Mingliang Du
The methanol-poisoning of electrocatalysts at the cathodic part of direct methanol fuel cells (DMFCs) can severely degrade the overall efficiency. Therefore, engineering cathodic catalysts with outstanding oxygen reduction activity, and simultaneously, superior methanol tolerance is greatly desired. Herein, bimetallic palladium-copper (PdCu) nanoplates with the optimized d-band center are designed as promising cathodic catalysts for DMFCs. It shows outstanding oxygen reduction activity with a mass activity (MA) of 0.522 A mg Pd −1 in alkaline electrolyte, overwhelming the benchmarked commercial Pt/C and Pd/C. Meanwhile, it has prominent stability with only 4.0 % loss in MA after continuous 20 K cycles. More importantly, the PdCu nanoplates are almost inert toward methanol oxidation and show excellent anti-methanol capability. The theoretical calculations reveal that the downshift of d-band center in PdCu nanoplates and the electronic interaction between Pd and Cu atoms could effectively lower the methanol adsorption energy, thus leading to enhanced methanol tolerance. This work highlights the important role of tuning the electronic structure and optimized geometry of electrocatalysts to simultaneously boost their oxygen reduction activity, stability, and methanol tolerance for their future application in DMFCs.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Chaobo Feng,Bing-Qiang Lu,Yunshan Fan,Haijian Ni,Yunfei Zhao,Shuo Tan,Zhi Zhou,Lijia Liu,Jordan A. Hachtel,Demie Kepaptsoglou,Baohu Wu,Denis Gebauer,Shisheng He,Feng Chen
Amorphous inorganic solids are traditionally isotropic, thus, it is believed that they only grow in a non-preferential way without the assistance of regulators, leading to the morphologies of nanospheres or irregular aggregates of nanoparticles . However, in the presence of (ortho)phosphate (Pi) and pyrophosphate ions (PPi) which have synergistic roles in biomineralization , the highly elongated amorphous nanowires (denoted ACPPNs) form in a regulator-free aqueous solution (without templates, additives, organics, etc). Based on thorough characterization and tracking of the formation process (e.g., Cryo-TEM, spherical aberration correction high resolution TEM, solid state NMR , high energy resolution monochromated STEM-EELS), the microstructure and its preferential growth behavior are elucidated. In ACPPNs, amorphous calcium orthophosphate and amorphous calcium pyrophosphate are distributed at separated but close sites. The ACPPNs grow via either the preferential attachment of ∼2 nm nanoclusters in a 1-dimension way, or the transformation of bigger nanoparticles, indicating an inherent driving force-governed process. We propose that the anisotropy of ACPPNs microstructure, which is corroborated experimentally, causes their oriented growth. This study proves that, unlike the conventional view, amorphous minerals can form via oriented growth without external regulation, demonstrating a novel insight into the structures and growth behaviors of amorphous minerals.
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MOLECULES
·
2020
·Vol. 25
·期 23
·5778
·
IF 3.267
Yangke Wanyan,Xixi Xu,Kehang Liu,Huidan Zhang,Junai Zhen,Rong Zhang,Jumei Wen,Ping Liu,Yuqing Chen
Inhibition of the glycolytic pathway is a critical strategy in anticancer therapy because of the role of aerobic glycolysis in cancer cells. The glycolytic inhibitor 2-Deoxy-d-glucose (2-DG) has shown potential in combination with other anticancer agents. Buforin IIb is an effective antimicrobial peptide (AMP) with broad-spectrum anticancer activity and selectivity. The efficacy of combination treatment with 2-DG and buforin IIb in prostate cancer remains unknown. Here, we tested the efficacy of buforin IIb as a mitochondria-targeting AMP in the androgen-independent human prostate cancer cell line DU145. Combining 2-DG with buforin IIb had a synergistic toxic effect on DU145 cells and mouse xenograft tumors. Combination treatment with 2-DG and buforin IIb caused stronger proliferation inhibition, greater G1 cell cycle arrest, and higher apoptosis than either treatment alone. Combination treatment dramatically decreased L-lactate production and intracellular ATP levels, indicating severe inhibition of glycolysis and ATP production. Flow cytometry and confocal laser scanning microscopy results indicate that 2-DG may increase buforin IIb uptake by DU145 cells, thereby increasing the mitochondria-targeting capacity of buforin IIb. This may partly explain the effect of combination treatment on enhancing buforin IIb-induced apoptosis. Consistently, 2-DG increased mitochondrial dysfunction and upregulated Bax/Bcl-2, promoting cytochrome c release to initiate procaspase 3 cleavage induced by buforin IIb. These results suggest that 2-DG sensitizes prostate cancer DU145 cells to buforin IIb. Moreover, combination treatment caused minimal hemolysis and cytotoxicity to normal WPMY-1 cells. Collectively, the current study demonstrates that dual targeting of glycolysis and mitochondria by 2-DG and buforin IIb may be an effective anticancer strategy for the treatment of some advanced prostate cancer.Keywords:buforin IIb;2-Deoxy-d-glucose;mitochondria;glycolysis;prostate cancer
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Membranes
·
2021
·Vol. 11
·期 8
·612
·
IF 4.106
Zhan Gao,Zhihao Yu,Xiaoli Zhang,Shougang Fan,Huiyu Gao,Caini Liu,Qixing Zhou,Huaiqi Shao,Lan Wang,Xiaoyan Guo
The thorny issue of membrane biofouling in membrane bioreactors (MBR) calls for new effective control measures. Herein, D-amino acid (DAA) was employed to mediate MBR membrane biofouling by inhibiting biofilm information and disintegrating formed biofilm. Different DAA control ways involving membrane property, DAA-adding timing, and DAA-control mode were explored through experiments and the multiple linear regression model and the response surface methodology. The optimized DAA control ways were acquired, involving DAA used as an active agent, and the DAA-adding timing of 4 h cultured before running, as well as both hydrophilic and hydrophobic membrane, resulting in an approximately 40.24% decrease in the membrane biofouling rate in comparison with the conventional MBR. DAA is an efficient membrane biofouling mediating approach for MBR under optimized control ways combination and a facile solution for solving membrane biofouling in actual membrane systems.Keywords:membrane bioreactor;membrane biofouling;D-amino acid;control way;model evaluation
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Journal of Materials Chemistry A
·
2019
·Vol. 8
·期 1
·369-379
·
IF 10.733
Chun Li,Lingling Shi,Lili Zhang,Peng Chen,Junwu Zhu,Xin Wang,Yongsheng Fu
Organic two-dimensional (2D) materials with unique optic-electronic properties are attracting great interest for application in functional electronic devices. However, low electronic conductivity and poor stability still are major defects of 2D organic systems. Herein, we demonstrated ultrathin 2D conductive cobalt–hexaaminobenzene metal–organic coordination polymer nanosheets (Co–HAB-NSs) with a thickness of ∼4.5 nm. The as-prepared Co–HAB-NSs exhibit a low overpotential (310 mV @ 10 mA cm−2) and high durability in 1 M KOH. The experimental and computational results show that the high electrocatalytic activity is ascribed to the enhanced electrochemically active surface area as well as the dense and stable catalytic active sites of Co–HAB-NSs.
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INTERNATIONAL JOURNAL OF POLYMER ANALYSIS AND CHARACTERIZATION
·
2018
·
IF 1.333
Qiao Zhang,Jianjun Fang,Wenjuan Liu,Yunhui Zhao,Tianlong Huang,Jiale Cui,Yun Yang,Zhihua Zhou
Bone tissue engineering is sought to apply strategies for bone defects healing biodegradable porous scaffolds without limitations and shortcomings. In this work, we have developed a novel maleic anhydride (MAH) and 1,4-butanediamine modified poly(lactide-co-glycolide) polymer (BMPLGA). The synthesized polymer was characterized by Fourier transform infrared spectrometry (FTIR), Nuclear magnetic resonance spectra (1H NMR), gel permeation chromatography (GPC) and contact angle measurements. In addition, cell morphologies in the extracts and cell cytotoxity were also studied. The results showed that the BMPLGA was successfully obtained by introducing MAH and 1,4-butanediamine into PLGA in bulk. The introduction of anhydride and amino groups improved the hydrophilicity of PLGA. Fibroblastic cells showed normal morphologies in BMPLGA extracts, and the BMPLGA materials showed no cell cytotoxicity. The synthetic BMPLGA material may have potentials for biomedical applications due to improving hydrophilicity.
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ADVANCED FUNCTIONAL MATERIALS
·
2015
·Vol. 25
·期 18
·2754-2762
·
IF 11.805
Yujing Zuo,Jinfeng Cao,Shengyu Feng
The increasing pursuit of biocontained elastic materials led the investigation of the potential use of the monoterpene limonene in film synthesis via thiol–ene reaction. Poly[(mercaptopropyl)methylsiloxane] (PMMS) is first synthesized. By controlling the molar ratio of PMMS and functional monomers, such as polyethylene glycol allyl methyl ether or rhodamine-B, PMMS is partially functionalized while leaving spare mercapto groups that could be further used as cross-linking sites. On the basis of the functionalized PMMS, novel transparent silicone luminescent films with hydrophilic tunable properties are prepared by natural-sunlight-triggered thiol–ene “click” chemistry by using d -limonene as a cross-linker. Their structures and properties are thoroughly characterized. Transparent luminescent films are coated on commercially available UV-light emitting diode (LED) cell from solution medium followed by an in situ cross-linking step; a colorful LED cell is obtained through this facile and efficient method. The UV-LED coated by films show very intense photoluminescence under normal visible light or the light is on, and has very high coloric purity.
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BIOCATALYSIS AND BIOTRANSFORMATION
·
2016
·
IF 0.892
Danping Qi,Wei Wei,Mingming Diao,Fengxia Lv,Zhaoxin Lu,Xiaomei Bie,Haizhen Zhao
Lipase-catalyzed synthesis of mono- and diesters of 3-O-β-D-galactopyranosyl-sn- glycerol (β-GG) with caproic acid was performed in acetone. The simultaneous production of 1(6’)-monoesters and 1,6’-diesters of β-GG was achieved in this reaction. In order to improve the yield of β-GG esters, four process parameters, enzyme concentration (15 ∼ 25 mg/mL), and substrate molar ratio (caproic acid: β-GG= 1.60 ∼ 2.00 mmol: 0.10 mmol), reaction temperature (40 ∼ 60 °C), and reaction time (8 ∼ 12 h), were optimized via response surface methodology (RSM) employing a three-level-four-variable central composite design. Results showed that enzyme concentration had the most significant (p < 0.0001) effect on the synthesis of β-GG esters. The optimal reaction conditions in acetone were given as follows: Novozyme435 concentration 18.65 mg/mL, molar rate of caproic acid to β-GG 19.46:1, reaction temperature 48 °C, and reaction time 9.83 h. The yield of β-GG esters reached 88.08% under above optimized conditions, which was very close to the predicted value 87.95%. The molar ratio of monoester to diesters was 0.39:0.61. β-GG esters with other fatty acyl chains were synthesized based on the optimized conditions. In vitro antitumor activity indicated that the antitumor activity of β-GG esters was dependent on the nature of fatty acids, such as the length of acyl chain, the degree of saturation, as well as the number of acyl chain.
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Small
·
2016
·Vol. 13
·期 3
·1602494
·
IF 8.315
Yu Zhang,Yifei Lu,Feng Wang,Sai An,Yujie Zhang,Tao Sun,Jianhua Zhu,Chen Jiang
Inflammation has been reported as one significant hallmark of breast cancer in relation to tumor development, metastasis, and invasion. The bradykinin receptor 1 (B1R) is highly expressed on inflammatory breast tumor cells thus providing a promising targeting site for tumor recognition and sufficient receptor mediated endocytosis. In this study, the authors evaluate the targeting efficiency of l -form and d -form [des-Arg 10 ]kallidin both in vitro and in vivo. To further improve the drug delivery efficiency, the authors establish a dandelion like nanoparticle by combining the polymeric drug conjugates and aptamer complex together. The doxorubicin conjugated polymer is complexed with adenosine-5′-triphosphate (ATP) sensitive hybridized aptamer in self-assembly process by intercalating into the double strand scaffolds. The acid labile conjugating bond and ATP sensitive aptamer endow the nanoparticle with dual responsiveness to intracellular milieu, thus triggering a quick drug release in tumor cells. Remarkable therapeutic effects and tuned in vivo pharmacokinetics profiles are shown by the aptamer complexed drug conjugates nanoparticle with B1R active targeting modification. Therefore the strategies of B1R targeting and ATP/pH dual-responsiveness nanoparticle help achieve enhanced drug accumulation within tumor cells and efficient chemotherapy for breast cancer.
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Molecular Catalysis
·
2025
·
IF 4.9
Sixia Liu,Xiaobo Zhang,Nidu Wang,Nagimovich Karimov,Yujie Wang,Zihan Gao,Dongguang Wang,Baikang Zhu,Shuying Gao,Fu Yang
The electrochemical nitrogen reduction reaction (e-NRR) is a promising energy-efficient and low-emission alternative to the traditional Haber–Bosch process, but the sluggish kinetic and difficult activation of nitrogen impede the reaction activity. In particular, addressing the weak interaction of nitrogen with catalysts is very challenging in this field. Here, a surface oxygen vacancies tailored method was proposed to shift the d -band center of iron-based electrocatalysts to Femi energy level, by leveraging molecule self-assembly strategy to obtain Fe-base gels followed by ultrafast calcined process. The optimal electrocatalysts (Fe 3 O 4 -xGO) possess a hierarchical porous architecture (coral-like morphology), thereby endowed with outstanding structural properties (329.1 cm 2 g⁻ 1 ). Meanwhile, interfacial oxygen vacancies could be constructed during the ultrafast heat-pyrolysis process, and their concentration could be tailored with the assistance of graphene oxide (GO). Benefiting from these structure characters, the d -band center of Fe in coral-like iron oxide can be shifted to a higher energy level, which is conducive to trapping and activating the intermediate in the e-NRR process. The results of the electrocatalytic NRR test, as anticipated, indicated that Fe 3 O 4 –10GO achieved a high Faradaic efficiency of 28 % and an NH 3 production rate of 30.45 μg h⁻¹ mg cat ⁻¹ at −0.3 V vs. RHE in a 0.1 M Na 2 SO 4 , positioning it comparably to most iron-based electrocatalytic materials used in e-NRR applications. This work could provide new insight for moldering the d band center of the electrocatalyst.
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Contrast Media & Molecular Imaging
·
2018
·
IF 2.934
Shengjuan Luo,Jinsong Ding,Peiqi Wang,Zheng Wang,Xiaoqian Ma,Cejun Yang,Qi Liang,Pengfei Rong,Wei Wang
Perfluorooctyl bromide (PFOB) enclosed nanoparticles (NPs) as ultrasonic contrasts have shown promising results in the recent years. However, NPs display poor contrast enhancement in vivo. In this work, we used the copolymers poly(lactide-co-glycolide) carboxylic acid (PLGA-COOH) and poly(lactide-co- glycolide) poly(ethylene glycol) carboxylic acid (PLGA-PEG-COOH) as a shell to encapsulate PFOB to prepare a nanoultrasonic contrast agent. The NPs were small and uniform ( nm with a polydispersity index of ) with a complete shell nuclear structure under the transmission electron microscopy (TEM). In vitro, when concentration of NPs was ≥10 mg/ml and clinical diagnostic frequency was ≥9 MHz, NPs produced intensive enhancement of ultrasonic gray-scale signals. NPs could produce stable and obvious gray enhancement with high mechanical index (MI) (MI > 0.6). In vivo, the NPs offered good ultrasound enhancement in tumor after more than 24 h and optical imaging also indicated that NPs were mainly located at tumor site. Subsequent analysis confirmed that large accumulation of fluorescence was observed in the frozen section of the tumor tissue. All these results caused the conclusion that NPs encapsulated PFOB has achieved tumor-selective imaging in vivo.
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