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Journal of Materials Chemistry A · 2018 ·Vol. 6 ·期 44 ·21969-21977 · IF 9.931

Solid-phase hot-pressing synthesis of POMOFs on carbon cloth and derived phosphides for all pH value hydrogen evolution

Yu-Jia Tang,Yifa Chen,Hong-Jing Zhu,A.-Man Zhang,Xiao-Li Wang,Long-Zhang Dong,Shun-Li Li,Qiang Xu,Ya-Qian Lan

Designing an all pH value hydrogen evolution reaction (HER) electrocatalyst with low cost and high activity is urgently needed for future energy storage and conversion systems. Metal–organic frameworks (MOFs) with well-defined pore structures and various metal sources provide feasible platforms for the design of efficient electrocatalysts. However, MOFs as crystalline materials are mostly in crystal or powder form, which would hinder their practical application. Herein, polyoxometalate-based MOFs (POMOFs) were synthesized on carbon cloth (CC) through a facile and general solid-phase hot-pressing method for the first time. The thus-obtained POMOFs/CC can be converted into three phase bimetallic phosphides coated with porous carbon on CC through a phosphidation process, show high electrocatalytic stability over a wide pH range (pH, 0–14) and possess excellent HER performance with low overpotential (e.g., 90.5 mV at 10 mA cm−2 in 1 M KOH). Moreover, the POMOFs/CC derived phosphides present high selectivity for H2 production (nearly 100% faradaic efficiency) and ultra-low charge-transfer resistance (0.96 Ω) in alkaline medium, which hold promise for practical applications. This work provides a powerful strategy for the facile production of fast nucleating MOF-derived electrodes with potential for industrial-scale application in energy storage and conversion.

研究领域: 材料科学 · 能源化学
✓ 已验证 DOI 高影响因子
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Journal of Materials Chemistry B · 2023 ·Vol. 11 ·期 19 ·4308-4317 · IF 7

Sub-50 nm core–shell nanoparticles with the pH-responsive squeezing release effect for targeting therapy of hepatocellular carcinoma

Jian-Bo Qu,Huan-Jie Che,Bo Gao,Gang-Feng Li,Xue-Fei Zhang,Yi-Bo Zhang,Xiaojuan Wang

The development of drug delivery systems with high drug loading capacity, low leakage at physiological pH, and rapid release at the lesion sites remains an ongoing challenge. In this work, core–shell poly(6-O-methacryloyl-D-galactose)@poly(tert-butyl methacrylate) (PMADGal@PtBMA) nanoparticles (NPs) of sub-50 nm are facilely synthesized by reversible addition–fragmentation chain transfer (RAFT) soap-free emulsion polymerization with the assistance of 12-crown-4. A hydrophilic poly(methacrylic acid) (PMAA) core can then be revealed after deprotection of the tert-butyl groups, which is negatively charged and can adsorb nearly 100% of incubated doxorubicin (DOX) from a solution at pH 7.4. The physical shrinkage of PMAA chains below pH 6.0 endows the core with the squeezing effect, therefore realizing rapid drug release. It is demonstrated that the DOX release rate of PMADGal@PMAA NPs at pH 5 was 4 times that at pH 7.4. Cellular uptake experiments confirm the high targeting ability of the galactose modified PMADGal shell to human hepatocellular carcinoma (HepG2) cells. The fluorescence intensity of DOX in HepG2 cells is 4.86 times that of HeLa cells after 3 h incubation. Moreover, 20% cross-linked NPs show the highest uptake efficiency by HepG2 cells due to their moderate surface charge, size and hardness. In summary, both the core and the shell of PMADGal@PMAA NPs promise the rapid site-specific release of DOX in HepG2 cells. This work provides a facile and an effective strategy to synthesize core–shell NPs for hepatocellular carcinoma targeting therapy.

研究领域: 药剂学 · 肿瘤学 · 生物材料学
✓ 已验证 DOI PubMed 高影响因子
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Journal of Biobased Materials and Bioenergy · 2016 ·Vol. 10 ·期 4 ·284-289 · IF 0.635

pH- and Temperature-Responsive Chitosan-g-PDMAEMA as an Active Coating Material and Its Effects on the Storing of Grape

Jiang Ping,Jia Shan Shan,Wang Shuang,Xiao Jun Hua,Liu Wenjie,Wu Yiqiang

The pH- and temperature-responsive chitosan-graft-poly(2-(dimethylamino) ethyl methacrylate) (CS-g-PDMAEMA) were synthesized via atom transfer radical polymerization (ATRP) and evidenced by FTIR spectroscopy. Chitosan macroinitiator (CS-Br) was prepared by phthaloylation of amino groups of chitosan and acylation of hydroxyl groups of chitosan with 2-bromoisobutyryl bromide. The pH and temperature responses of the copolymer micelles were characterized by particle diameter and particle size analyzers. The film prepared from CS-g-PDMAEMA was used as a coating film on the surface of the grape. And the film prepared from 1 wt% CS-g-PDMAEMA solution was able to slow the loss of water in grape. The results revealed that the CS-g-PDMAEMA had potential application as active coating materials in the storage of fresh grape.

研究领域: 食品科学 · 高分子化学
✓ 已验证 DOI 高影响因子
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CHEMICAL ENGINEERING JOURNAL · 2020 · IF 10.652

Multifunctional hydrogel microsphere with reflection in near-infrared region for in vivo pH monitoring and drug release in tumor microenvironment

Xing Dong,Junjie Chi,Changmin Shao,Lanjie Lei,Lei Yang,Chao Zhao,Hong Liu

Tumor microenvironment (TME) is a pivotal factor in tumor progression. Here we report an injectable multifunctional hydrogel microsphere with responsive photonic structure for in vivo monitoring of TME pH. The pH determination is based on measurement of the characteristic reflection peak of the hydrogel microsphere in near-infrared (NIR) region that is sensitive to pH, and decreasing pH leads to a blue shift of the peak. With deep tissue penetration ability of the NIR light, the pH of normal and tumor tissues of mice are continuously monitored in vivo using the microspheres injected subcutaneously. The biocompatibility and the cytotoxicity of the material is investigated based on MTT assays to evaluate its potential for long-term continuous in vivo monitoring of TME pH. A drug for cancer treatment is also preloaded into the hydrogel microsphere for simultaneous drug release in TME and monitoring of the treatment effectiveness of drug by the TME pH tests.

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
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PHARMAZIE · 2018 ·Vol. 73 ·期 10 ·594-597 · IF 1.016

Andrographolide inhibits proliferation and induces apoptosis of nasopharyngeal carcinoma cell line C666-1 through LKB1-AMPK-dependent signaling pathways

Wu Bo,Chen Xi,Zhou Ying,Hu Pingjun,Wu Dan,Zheng Guodong,Cai Yi

Background: Andrographolide (Andro) belongs to the main bioactive ingredients of Andrographis paniculata. Many studies have shown that andro has a variety of pharmacological activities such as anti-inflammatory, anti-bacterial, anti-virus, anti-oxidant, immune regulation and liver protective effects. Moreover andro has been reported to have anticancer activity in multiple types of cancer, including gastric cancer, breast cancer, lung cancer and so on. However, there is no report about the effect of andro on the human NPC cell line C666-1 and the molecular mechanisms of andro-mediated apoptosis in C666-1 cells remain to be clarified. Methods: Cell proliferation was measured by a CCK8 assay, cell apoptosis rate was evaluated by flow cytometric analysis, and the protein expression of LKB1/AMPK signaling pathways was detected by Western blotting. Results: Treatment with andro inhibited cell proliferation and induced apoptosis of C666-1 cells. Moreover, andro could activate LKB1-AMPK signaling. We also demonstrated that Ca2+/calmodulin-dependent protein kinase kinaseβ (CaMKKβ) was not involved in the regulation of andro on AMPK activation in C666-1 Cells. Conclusions: Andro suppressed proliferation and induced apoptosis of C666-1 cells through regulating the LKB1/AMPK/mTOR signal pathway.

✓ 已验证 DOI PubMed 高影响因子
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MICROPOROUS AND MESOPOROUS MATERIALS · 2021 · IF 5.455

Efficient phosphate capture of Fe3O4/UiO-66-NH2/CeO2 in wide pH spectrum

Liyu Yang,Xiangcheng Shan,Yumeng Zhao,Zuoyi Xiao,Qingda An,Shangru Zhai

Eutrophication has long been one of the environmental pollution problems, and excess phosphate in water bodies is the main cause of this phenomenon. To solve this problem, magnetic adsorbent with Fe/Ce-loaded zirconium-based metal-organic framework (Fe 3 O 4 /UiO-66-NH 2 /CeO 2 ) was prepared by co-precipitation, microwave assisted and hydrothermal method . The results showed that different molar ratios of cerium and zirconium were the main influencing factors for phosphate adsorption, and the adsorbent exerted its maximum capturing capacity of 260.8 mg/g of phosphate when Ce:Zr = 4:1. The newly synthesized Fe 3 O 4 /UiO-66-NH 2 /CeO 2 was characterized by SEM, XRD , FT-IR, XPS, VSM and TGA . The adsorption process was found to be consistent with the Langmuir adsorption isotherm model and the pseudo-second-order model by batch experiments, indicating that the monolayer chemisorption dominated the adsorption process. Thermodynamic parameters obtained from temperature experiments proved that the phosphate adsorption process is a spontaneous endothermic absorption process and the adsorption experiments with coexisting ions (F − , Cl − , NO 3 − , SO 4 2− , HCO 3 − ) showed that the adsorbent has a unique selectivity for phosphate. Unlike most adsorbents previously studied, Fe 3 O 4 /UiO-66-NH 2 /CeO 2 exhibited consistently efficient adsorption performance over the pH spectrum tested (2 < pH < 10). After five cycles, the adsorbent still maintained favourable adsorption performance. Mechanism of Fe 3 O 4 /UiO-66-NH 2 /CeO 2 adsorption on phosphate was attributed to electrostatic attraction, ligand exchange and inner-sphere complexation. Therefore, the prepared Fe 3 O 4 /UiO-66-NH 2 /CeO 2 with wide pH suitability will be a promising option for capturing phosphate from wastewater.

研究领域: 环境科学 · 水处理 · 材料科学
✓ 已验证 DOI 高影响因子
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JOURNAL OF NANOBIOTECHNOLOGY · 2021 ·Vol. 19 ·期 1 ·1-17 · IF 10.435

pH-sensitive dual drug loaded janus nanoparticles by oral delivery for multimodal analgesia

Liu Lin,Yao Wendong,Xie Xiaowei,Gao Jianqing,Lu Xiaoyang

Background Based on the concept of “multimodal analgesia”, a novel dual drug delivery system was designed to achieve synergistic analgesia between najanajaatra venom protein (αCT) and resveratrol (Res). In order to meet the joint loading of two drugs with different physicochemical properties without affecting each other, an oral Janus nanoparticle (JNP) with a unique cavity structure and synergistic drug delivery was constructed using an improved double emulsion solvent evaporation method, and combined with low-molecular-weight chitosan/sodium alginate and PLGA to achieve its pH-responsive.Results The synthesized αCT/Res-JNPs are homogeneous in shape, with a two-compartment structure, approximately 230 nm in size, and zeta potential of 23.6 mV. Drug release assayed in vitro show that JNP was stable in simulated gastric juice (pH = 1.2) but was released in phosphate buffer saline (pH = 7.4). After intragastric administration in rats, PK evaluation showed that αCT/Res-JNPs could significantly improve the oral bioavailability, and the simultaneous encapsulation of the two drugs had no significant interaction on PK parameters. An obvious synergistic analgesic effects of αCT/Res-JNPs was confirmed in a spinal cord injury and acute pain model. Confocal laser scanning microscopy and single-pass intestinal perfusion model provided strong evidence that αCT/Res-JNPs could pass through intestinal epithelial cells, and the endocytosis pathway was mainly involved in the mediation and pinocytosis of reticulin. The concentrations of αCT and Res from αCT/Res-JNP in lymphatic transport were only about 8.72% and 6.08% of their blood concentrations at 1 h, respectively, which indicated that lymphatic transport in the form of JNP has limited advantages in improving the oral bioavailability of Res and αCT. Cellular uptake efficiency at 4 h was about 10–15% in Caco-2 cell lines for αCT/Res-JNP, but was reduced to 7% in Caco-2/HT29-MTX co-culture models due to the hindrance by the mucus layers. Approximately 12–17% of αCT/Res-JNP were transported across Caco-2/HT29-MTX/Raji monolayers. The cumulative absorption of JNP in three cell models was higher than that of free drug.Conclusion sThis study investigated the contribution of Janus nanoparticles in oral absorption, and provide a new perspective for oral administration and analgesic treatment of dual drug delivery system containing peptide drugs.Graphic Abstract

研究领域: 药剂学 · 纳米技术 · 药物递送 · 疼痛管理 · 生物药剂学
✓ 已验证 DOI PubMed 高影响因子
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Environmental Science-Nano · 2019 ·Vol. 6 ·期 7 ·2129-2140 · IF 7.704

The pH and concentration dependent interfacial interaction and heteroaggregation between nanoparticulate zero-valent iron and clay mineral particles

Yanlong Wang,Kun Yang,Benny Chefetz,Baoshan Xing,Daohui Lin

Heteroaggregation with clay mineral particles (CMPs) is significant to the environmental application and fate of increasingly produced nanoparticulate zero-valent iron (nZVI). Co-settling, kinetic aggregation, calculation of the classical Derjaguin–Landau–Verwey–Overbeek interaction energy, and electron microscopic observation were carried out to investigate the interaction between nZVIs (three naked nZVIs of different sizes and one carboxymethyl cellulose (CMC) coated nZVI) and CMPs (kaolinite and montmorillonite). Under pH 6.5 and 9.5 conditions, Lewis acid–base interaction contributed to the attachment between nZVIs and CMPs, while electrostatic attraction was involved in nZVI–CMP attachment under pH 3.5. Compared with the heteroaggregates formed by nZVIs attaching to CMP edges and faces under pH 6.5 and 3.5 conditions, the heteroaggregates were smaller with nZVIs mainly connecting to CMP edges under pH 9.5. Small nZVI homoaggregates were bound to CMP edges at low nZVI concentrations (nZVI/CMP mass ratio at 0.015) with CMP concentrations of 330 mg L−1 and large nZVI–CMP heteroaggregates formed by nZVI bridging with increasing nZVI concentrations. The smallest nZVI exhibited the strongest heteroaggregation with CMPs; the CMC coating inhibited the interfacial interaction and heteroaggregation between nZVIs and CMPs; kaolinite had higher potential to interact with nZVIs under neutral conditions. These findings are helpful for understanding the interaction between nZVIs and minerals and of significance to environmental remediation using nZVIs.

研究领域: 环境科学 · 胶体化学
✓ 已验证 DOI 高影响因子
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FOOD HYDROCOLLOIDS · 2022 · IF 11.504

pH-sensitive self-assembled nanofibers based on electrostatic interaction and Schiff base bonding for controlled release of curcumin

Peng Wang,Yucheng Zou,Yang Li,Zeyu Qin,Xingquan Liu,Hui Zhang

In this study, chitosan-dialdehyde-β-cyclodextrin-curcumin (CS-DCD-CUR) and alginate dialdehyde (ADA) were alternately deposited on the surface of electrospun cellulose acetate (CA) nanofibers driven by Schiff base bonding and electrostatic attraction. With the increasing number of bilayers, the self-assembled nanofibers showed an increased average fiber diameter from 441 to 576 nm and had relatively rough surfaces. The improved thermal stability and tensile strength of self-assembled nanofibers were attributed to the interactions between CS-DCD-CUR and ADA. The self-assembled nanofibers exhibited pH-sensitive release characteristics under acidic conditions due to the weakening of the electrostatic interaction and the hydrolysis of Schiff-base. Moreover, the self-assembled nanofibers could be used for sustained and controlled release of the curcumin within 620 min and maintained the antioxidant activities . The highest radical scavenging activities against ABTS and DPPH radicals of the nanofibers were 24.75% and 83.56%, respectively. These results suggested that the layer-by-layer self-assembled nanofibers provided a pH-responsive sustained delivery system for bioactive substances with potential applications in functional foods.

研究领域: 材料科学 · 药物递送 · 食品科学
✓ 已验证 DOI 高影响因子
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JOURNAL OF MOLECULAR LIQUIDS · 2022 · IF 6.633

pH-responsive water-in-oil emulsions with reversible phase inversion behavior stabilized by a novel dynamic covalent surfactant

Guoshuai Wang,Guancheng Jiang,Yue Fu,Jun Yang,Yinbo He,Tengfei Dong

The dynamic covalent nature of imine bonds provides a facile avenue to develop stimuli-responsive emulsifiers and has attracted considerable interest. In petroleum engineering, the development of smart emulsifiers that can be switched on demand to achieve the reversible phase inversion of the invert emulsion drilling fluid (IEDF) can effectively aid in its removal during cleanup. To this end, a novel dynamic covalent surfactant (TA-CBA) that can precisely manipulate the emulsion type by responding to acid/base stimuli was synthesized through the Schiff base reaction between 1-tetradecylamine (TA) and 4-carboxybenzaldehyde (CBA). Evaluation of the surface tension and interfacial tension (IFT) showed that the imine-bonded product TA-CBA was a surfactant with strong IFT reduction ability. At pH 7.4, the prepared water-in-oil (W/O) emulsions were stable without any separated phases after storage for 48 h and even after high-temperature aging at 210 °C. As the pH decreased from 7.4 to 4, the emulsion inverted from a higher viscosity W/O emulsion to a lower viscosity oil-in-water (O/W) emulsion. Remarkably, after the pH was adjusted back to 7.4, the rheological parameters and stability of the emulsion could be triggered at the original W/O emulsion level. 1 H NMR and IFT measurements revealed that the reversible formation and breakage of covalent imine bonds led to the production of CBA and cationic amine salt (TA + ), establishing the pH reversibility of the emulsion type and its rheological properties. Finally, we successfully formulated a reversible IEDF using TA-CBA as the sole emulsifier, which not only has reasonable rheological properties, filtration performance, and emulsification stability but also allows for easy cleanup. The IEDF can be phase-inverted into a water-soluble O/W emulsion drilling fluid at pH 4 and achieved a removal efficiency of 98.13 %.

研究领域: 化学工程 · 石油工程 · 材料科学
✓ 已验证 DOI 高影响因子
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JOURNAL OF ALLOYS AND COMPOUNDS · 2021 · IF 5.316

High-performance nickel/iron catalysts for oxygen evolution in pH-near-neutral borate electrolyte synthesized by mechanochemical approach

Tong Wen,Yunliang Zhao,Xiangke Jiao,Qiwu Zhang,Tingting Zhang,Xian Zhang,Jun Qu,Yan Dong,Shaoxian Song

In this work, a novel method of mechanochemistry is used to directly prepare high-performance Ni-Fe based catalysts for oxygen evolution reaction (OER) in an environmental-friendly borate electrolyte with near-neutral pH. Such a procedure is simple, effective, and time-saving. The effect of iron-based raw materials and mechanochemical reaction on OER of catalysts are investigated. It shows that iron nitrate nonahydrate is the best iron resource compared to iron hydroxide and iron oxide due to amorphous iron species in catalysts for strengthening the “Fe inductive effect” and generating active Ni species with high valence. Besides, the grinding time can control the mechanochemical reaction from mixed reaction to solid reaction in the catalyst synthesis process. When the time is 30 min, the catalyst is composed with amorphous Ni(OH) 2 and the precursors of NiFe-LDH. This catalyst only needs 413 mV overpotential to reach 1 mA cm −2 in 0.1 M K-Bi (pH=9.2), which is better than precious RuO 2 . It is proven that the mechanochemical approach is an alternative method for synthesizing superior OER catalysts.

研究领域: 材料科学 · 电化学
✓ 已验证 DOI 高影响因子
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CHINESE JOURNAL OF ANALYTICAL CHEMISTRY · 2022 · IF 1.193

Synthesis of N,S co-doped carbon dots for fluorescence detection of Fe3+ ions and intracellular pH imaging

Xiao-Ping CHEN,Ya-Feng ZHUANG,Jian-Wei LIN,Jing-Hua CHEN,Zhi-Zhong HAN

Using citric acid and thiourea as precursors, sulfur-nitrogen co-doped dual emission carbon dots (DECDs) were prepared by a simple solvothermal method. At the excitation wavelength of 360 nm, DECDs have two emission peaks located at 465 nm (blue) and 592 nm (yellow-green) which are attributed by core and surface of DECDs. It is found that Fe 3+ ions can coordinate with oxygen-containing groups on DECDs, and then the electrons transfer from DECDs to Fe 3+ ions, which quench the fluorescence of DECDs. The fluorescence intensity is linear with the concentration of Fe 3+ ions in the range of 0–100 μM and the detection limit is 0.77 μM. Moreover, the designed sensor can be applied to detect Fe 3+ ions in tap water with high selectivity, which provides a basis for the quantitative detection of Fe 3+ ions. At the same time, DECDs can be used as a pH fluorescence probe. In the pH 2.5–11.5 range, the fluorescence increases with pH whilst the solution color changes, providing a visualization platform for pH detection. Moreover, the pH fluorescence probe can be used for intracellular pH fluorescence imaging in living cells, and DECDs have an excellent biocompatibility (e.g., cell viability remains about 80% after treatment for 24 h at 200 μg·mL −1 of DECDs). Therefore, DECDs has a certain application prospect in food detection, biological detection and determination of intracellular pH change.

研究领域: 化学 · 生物医学工程 · 分析化学
✓ 已验证 DOI 高影响因子
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