Small
·
2023
·Vol. 19
·期 40
·2303227
·
IF 13.3
YuanZhe Wu,Quan Zong,Chaofeng Liu,Yanling Zhuang,Daiwen Tao,Jiangying Wang,Jingji Zhang,Qilong Zhang,Guozhong Cao
Vanadyl phosphate (VOPO 4 ·2H 2 O) has been regarded as one of the most promising cathode materials for aqueous Zn-ion batteries due to its distinct layered structure. However, VOPO 4 ·2H 2 O has not yet demonstrated the exceptional Zn ion storage performance owing to the structural deterioration during repeated charging/discharging process and poor intrinsic conductivity. In this work, 2D sodium vanadyl phosphate (NaVOPO 4 ·0.83H 2 O, denoted as NaVOP) is designed as a cathode material for Zn-ion batteries, in which sodium ions are preinserted into the interlayer, replacing part of water. Benefiting from the in situ surface oxidization, improved electronic conductivity, and increased hydrophobicity, the NaVOP electrode exhibits a high discharge capacity of 187 mAh g −1 at 0.1 A g −1 after activation, excellent rate capability and enhanced cycling performance with 85% capacity retention after 1500 cycles at 1 A g −1 . The energy storage mechanism of the NaVOP nanoflakes based on the rapid Zn 2+ and H + intercalation pseudocapacitance are investigated via multiple ex situ characterizations.
研究领域:
材料科学
·
电化学
·
能源存储
·
无机化学
·
纳米材料
✓ 已验证
DOI
高影响因子
Journal of Environmental Sciences
·
2024
·
IF 5.9
Xixian Huang,Bing Yang,Ye Dou,Yang Ding
The abiotic oxidation of divalent manganese (Mn(II)) and the formation of Mn oxides are important geochemical processes, which control the mobility and availability of Mn as well as element cycling and pollutant behavior in soils. It was found that iron (oxyhydr)oxides can catalyze Mn(II) oxidation , but the effects of the coexisting dissolved organic matter (DOM) molecules on the catalysis of different iron (oxyhydr)oxides for Mn(II) oxidation are poorly understood. Herein, we investigated Mn(II) oxidation under the impacts of the interactions between iron (oxyhydr)oxides (i.e., ferrihydrite, goethite and hematite) and DOM molecules. Simultaneously, we elucidated the variations of DOM composition and properties. Our results indicated that the catalysis of iron (oxyhydr)oxides for Mn(II) oxidation was significantly inhibited by DOM. Moreover, DOM had less inhibiting effect on the catalysis of ferrihydrite for Mn(II) oxidation and the formation of Mn oxides (e.g., hausmannite and buserite) relative to goethite and hematite, which was partially because of the higher electron transfer capacities of ferrihydrite. Meanwhile, DOM molecules with high nominal oxidation state of carbon (NOSC), molecular weight, unsaturation and aromaticity were selectively adsorbed and oxidized by Mn oxides , including the oxygenated phenols and polyphenols. The newly formed molecules mainly belonged to phenols depleted of oxygen and aliphatics. Furthermore, NOSC was a key molecular characteristic for controlling DOM composition during DOM adsorption and oxidation by Mn oxides when iron minerals were present. Overall, our research contributes to understanding Mn(II) oxidation mechanisms under heterogeneous systems and behaviors of DOM molecules in the environment.
研究领域:
环境地球化学
·
土壤化学
·
水文地球化学
·
有机-矿物相互作用
·
元素生物地球化学循环
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DOI
高影响因子
POLYMER
·
2019
·
IF 3.771
Feng Chen,Ziqing Tang,Shaoping Lu,Lin Zhu,Qilin Wang,Qin Gang,Jia Yang,Qiang Chen
Double network hydrogels (DN gels) are one of most extensively investigated high strength hydrogels. However, most of DN gels are concern to macromolecules , low-molecular-weight gelators (LMWG)-based supramolecular hydrogels are rarely reported to fabricate recoverable DN gels. Owing to the low mechanical properties, LMWG-based supramolecular hydrogels are hardly fabricated as conductive materials for human motion monitoring. Herein, we report a general strategy to fabricate strong, tough and conductive cholate-based supramolecular gels with double network (DN) structure (i.e. La-cholate/PAAm DN gels), consisting of La-cholate supramolecular gel as first network and covalent polyacrylamide gel (PAAm gel) as second network, in which La-cholate supramolecular gel was self-assembled by La 3+ ions and sodium cholate under sonication via the synergistic effect of hydrogen bonds , hydrophobic interactions and metal-coordination. At optimal condition, La-cholate/PAAm DN gel exhibited high tensile properties (fracture stress of 0.314 MPa, fracture strain of 29.85 mm/mm, elastic modulus of 90 kPa, and work of extension of 5.678 MJ/m 3 ) and high toughness (tearing energy of 1098 J/m 2 ), which are comparable to conventional chemical or hybrid DN gels. Meanwhile, La-cholate/PAAm DN gel also showed rapid self-recovery property (stiffness recovery of 84% and toughness recovery of 46% after resting for 3 min) at room temperature and λ-dependent luminescent property under UV-light. More importantly, cholate-based supramolecular gels with DN structure could be prepared with various metal ions and monomers . Interestingly, our cholate-based DN gels were ionically conductive, which could be used as strain sensor to finely detect the human motions. We hope our design principles, along with the simple method and cholate-based DN gels, can be generally applied to develop a new generation of strong and tough LMWG-based supramolecular hydrogels with various functionalities.
研究领域:
高分子科学
·
生物材料
·
软物质物理
·
纳米医学
·
组织工程
·
智能响应材料
·
生物传感
✓ 已验证
DOI
高影响因子
RSC Advances
·
2022
·Vol. 12
·期 19
·11715-11721
·
IF 4.036
Baokang Zou,Yipeng Zhan,Xiuli Xie,TongTong Zhang,Runkai Qiu,Fangming Zhu
Two salalen titanium(IV) complexes ((H-salalen)TiCl2 and (F-salalen)TiCl2) containing hydrogen and fluorine respectively on the phenolate ring close to the imine were synthesized for the copolymerization of ethylene with 1-octene to prepare poly(ethylene-co-1-octene) in the presence of methylaluminoxane (MAO). The (F-salalen)TiCl2/MAO showed higher catalytic activity and better copolymer characteristics such as a higher molecular weight, narrower molecular weight distribution, and higher 1-octene incorporation than (H-salalen)TiCl2/MAO, which revealed that the electron-withdrawing conjugated effect introduced by fluorine substituents led to improvements on catalytic performance and thermal stability. The influences of copolymerization conditions including temperature, Al/Ti molar ratios and comonomer feed ratios on the copolymerization behavior of (F-salalen)TiCl2/MAO and the copolymer microstructure were investigated in detail. Under the activation of MAO, the (F-salalen)TiCl2 could produce ultrahigh molecular weight poly(ethylene-co-1-octene) with 1-octene incorporation ratios in the range of 0.9–3.1 mol% and exhibit relatively high activity. It could be inferred that long ethylene sequences in the copolymer were segregated by the isolated 1-octene units based on the 13C NMR characterization of the copolymer. Moreover, the thermal properties and crystallization of copolymers were determined by DSC and XRD and correlated to the ethylene sequence length distribution. The reactivity ratios calculated by the triad distribution in 13C NMR revealed the random comonomer distribution in the copolymer chain.
研究领域:
高分子化学
·
配位聚合
·
催化化学
·
材料科学
·
高分子物理
✓ 已验证
DOI
高影响因子
RSC Advances
·
2016
·Vol. 6
·期 112
·111217-111225
·
IF 3.289
Sijie Zhao,Huiru Yang,Cai Zuo,Lu Sun,Liwei Ma,Hua Wei
Star-shaped polymers are attractive as drug carriers due to the integration of relatively easy synthesis compared to the preparation of hyper-branched dendrimers and their potential ability to form unimolecular nanoparticles with enhanced stability to survive the high dilution-associated deformation and subsequently premature drug release in the body fluids and blood during circulation. Clearly, the star structure exerts a significant effect on their bioproperties and potential applications. In this study, three star-shaped amphiphilic copolymers with the same polymer compositions but different star structures were synthesized to investigate the effect of star architecture on their properties as well as potential applications as drug carriers. Three different branched alcohols, 2-(hydroxymethyl) propane-1,3-diol, pentaerythritol and dipentaerythritol with 3, 4, and 6 respective hydroxyl groups were chosen as the starting core to generate the target star-shaped amphiphilic block copolymers composed of hydrophobic poly(ε-caprolactone) (PCL) and hydrophilic poly(oligoethyleneglycol methacrylate) (POEGMA) with 3, 4, and 6 corresponding star arms by a combination of ring-opening polymerization (ROP) and atom transfer radical polymerization (ATRP). Dynamic light scattering (DLS) measurements and pyrene fluorescence probe technique confirmed the capability of the resultant star-shaped amphiphilic copolymers to form unimolecular micelles with average diameters smaller than 50 nm in an aqueous phase. A comparison of the drug loading capacity revealed that the micelles of 4-star-PCL–POEGMA (4s-PCL–POEGMA) exhibited the highest drug loading content (DLC) of all the three formulations. More importantly, in vitro doxorubicin (DOX) release study showed unique pH-mediated drug release behaviors, i.e., dramatically accelerated release at pH 6.0 but a much slower profile at pH 7.4, from these generally recognized “pH-insensitive” 4-arm star-shaped micelles. An acid-triggered degradation and an acid–base titration were performed to further reveal that such interesting pH-responsive drug release behaviors were attributed primarily to the hydrophilic corona of OEG brushes. This study is believed to provide a new insight into the structure–bioproperties relationship of star-shaped polymers, thus should be useful for the future design and development of novel star-shaped polymers for controlled drug delivery.
研究领域:
高分子药剂学
·
纳米医学
·
药物控释
·
生物材料
·
药剂学
·
肿瘤治疗
·
纳米载体
✓ 已验证
DOI
高影响因子
JOURNAL OF POLYMER SCIENCE PART A-POLYMER CHEMISTRY
·
2015
·Vol. 54
·期 3
·368-380
·
IF 3.113
Jingang Li,Yixin Xiang,Sixun Zheng
In this contribution, we reported the synthesis of a hyperbranched block copolymer composed of poly(ε-caprolactone) (PCL) and polystyrene (PS) subchains. Toward this end, we first synthesized an α-alkynyl- and ω,ω′-diazido-terminated PCL- b -(PS) 2 macromonomer via the combination of ring-opening polymerization and atom transfer radical polymerization. By the use of this AB 2 macromonomer, the hyperbranched block copolymer ( h -[PCL- b -(PS) 2 ]) was synthesized via a copper-catalyzed Huisgen 1,3-dipolar cycloaddition (i.e., click reaction) polymerization. The hyperbranched block copolymer was characterized by means of 1 H nuclear magnetic resonance spectroscopy and gel permeation chromatography. Both differential scanning calorimetry and atomic force microscopy showed that the hyperbranched block copolymer was microphase-separated in bulk. While this hyperbranched block copolymer was incorporated into epoxy, the nanostructured thermosets were successfully obtained; the formation of the nanophases in epoxy followed reaction-induced microphase separation mechanism as evidenced by atomic force microscopy, small angle X-ray scattering, and dynamic mechanical thermal analysis. © 2015 Wiley Periodicals, Inc. J. Polym. Sci., Part A: Polym. Chem. 2016 , 54 , 368–380
研究领域:
高分子化学
·
材料科学
·
纳米结构功能材料
·
聚合物自组装
·
热固性树脂改性
✓ 已验证
DOI
高影响因子
RSC Advances
·
2017
·Vol. 7
·期 36
·22485-22491
·
IF 3.108
Hailiang Zhao,Shanshan Tang,Qun Zhang,Lin Du
The weak intermolecular interaction between 2,2,2-trifluoroethanol (TFE) and 3-chloro-2-methyl-1-propene (CMP) has been investigated by gas phase FTIR spectroscopy and DFT calculations. CMP offers two hydrogen bond docking sites to the hydrogen bond donor: the chlorine atom (O–H⋯Cl) and the CC π electron system (O–H⋯π). DFT calculations suggest that MeOH approaches CMP in five different orientations. The structural, energetic, and spectroscopic parameters of the most stable structures in each orientation were studied, and their binding energies range from −25.5 to −19.5 kJ mol−1. The docking to the π system is at least 1 kJ mol−1 more favored than the docking to the chlorine atom. The equilibrium constant for complexation (2.3 × 10−2) was determined from the experimental and calculated intensity of the OH-stretching transition. The Gibbs free energy of formation was found to be 9.3 kJ mol−1. The nature of the non-covalent interaction was analyzed with the atoms in molecules (AIM) method.
研究领域:
物理化学
·
结构化学
·
分子光谱学
·
量子化学计算
·
分子间相互作用
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DOI
高影响因子
RSC Advances
·
2014
·Vol. 4
·期 52
·27259-27266
·
IF 3.708
Libin Yang,Feng Xin,Junzhong Lin,Zhuang Zhuang,Rui Sun
In this study, a hydrothermal synthesis was developed to prepare a thin titanium silicalite-1 catalyst layer in the internal channels of the honeycomb cordierite support, which was used in a continuous heterogeneous reaction. The as-prepared thin TS-1 catalyst layer was characterized by SEM, XRD, UV-vis and ATR-FTIR methods. Multiple hydrothermal syntheses were used for controlling the crystalline growth to optimize catalytic activity and lifetime. Moreover, a monolithic TS-1/cordierite reactor with external looping was utilized to investigate the characteristics of the continuous heterogeneous ammoximation reaction without the organic solvent tert-butanol (TBA). The reaction results showed that the conversion of cyclohexanone and selectivity of oxime approached more than 0.96 and 0.98, respectively. When compared with the reaction using TBA as the reaction solvent, the activity of the monolithic TS-1/cordierite showed no differences except for a longer lifetime.
研究领域:
化学工程
·
催化化学
·
材料科学
·
工业化学
·
绿色化学
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DOI
高影响因子
MICROCHEMICAL JOURNAL
·
2014
·
IF 3.583
Haiyun Zhai,Jiangmei Li,Zuanguang Chen,Zihao Su,Zhenping Liu,Xiao Yu
A simple glass/PDMS microfluidic chip for on-line sample pretreatment and contactless conductivity detection, which consisted of a 0.17 mm-thick glass cover and a PDMS substrate embedded with an SPE monolithic column, was presented in this paper. Using this integrated microchip system, sample extraction, injection, separation and detection were automatically performed in sequence. A sample of auramine O was concentrated by molecularly imprinted SPE (MISPE), eluted to sample reservoir, and injected by electromigration into separation channel for electrophoresis separation and contactless conductivity detection, with the calculated detection limit (S/N = 3) being 2.5 μg mL − 1 . The monolithic column was utilized to quantitatively extract auramine O , yielding an on-line enrichment factor of about 12. The microchip system is reliable and applicable to the analysis of auramine O in food sample.
研究领域:
分析化学
·
微流控技术
·
食品安全
·
分子印迹技术
·
电泳学
·
生物医学工程
✓ 已验证
DOI
高影响因子
CHEMICAL RESEARCH IN CHINESE UNIVERSITIES
·
2015
·Vol. 31
·期 4
·585-589
·
IF 0.875
Wei Qi,Wang Liyuan
Molecular glass resist has been considered as one of the best choices for a new generation of lithography. In this work, a new type of photoactive compound was obtained by the esterification of tannic acid with 2-diazo-1-naphthoquinone-4-sulfonyl chloride(2,1,4-DNQ-Cl) and ditertbutyl dicarbonate. The new obtained compound possessed both a photosensitive group of diazonaphthoquinone sulfonate(2,1,4-DNQ) and a group of acidolytic protection. Upon the irradiation of the compound under 365 nm light, the former group was photolyzed and converted into indene carboxylic acid along with a small amount of sulfonic acid, which could lead to the deprotection of the latter group. As a result, a novel i-line molecular glass photoresist was formed with the chemical modification of tannic acid. The experimental results show that the modificated compound had a fair solubility in many organic solvents. The lithographic performance of the resist was evaluated on an i-line exposure system with high photosensitivity and resolution as well.
研究领域:
材料科学
·
微纳加工
·
高分子化学
·
光电子学
·
半导体工艺
✓ 已验证
DOI
高影响因子
TETRAHEDRON
·
2019
·Vol. 75
·期 31
·4174-4179
·
IF 2.379
Yingying Zuo,Feng Xiong,Jing Zhao
Organic sulfur compounds have broad applications in biology, medicine and material sciences and intensive efforts have been devoted to developing mild and general C–S bond-forming methods. However, a mild, transition-metal-free, direct C–H bond functionalization method remains elusive. Here, we report the use of an internal oxidant-directing strategy to achieve this goal. The cascade reactions described here show excellent chemoselectivity and a wide substrate scope for both oxyamines and sulfenylation reagents. This study enlarges the synthesis toolbox for preparing structurally diverse sulfilimines under mild conditions.
研究领域:
有机化学
·
合成化学
·
药物化学
·
生物医学材料
·
分子生物学
✓ 已验证
DOI
高影响因子
Small
·
2022
·Vol. 18
·期 29
·2202622
·
IF 15.153
Hao Zhu,Zixuan Chen,Yun Chen,Jun-Jie Zhu
Quantifying the binding kinetics and affinities of protein–small molecule interactions is critical for biomarker validation, drug discovery, and deep understanding of various biological processes at the molecular-scale. Novel approaches are demanded as most common label-free techniques are mass-sensitive, which are not suitable for the detection of small molecule interactions. Here, an optical imaging platform is developed to measure the binding kinetics of both protein–small molecules and protein–ions based on monolayer MoS 2 , an ultra-thin 2D material whose optical absorption is extremely sensitive to charge. A model is established to calibrate the optical response due to the charged analyte binding and it is applied to quantify the interactions between abl1 kinase and different small-molecule inhibitors. Such a presented method is capable of distinguishing different inhibitors binding to a wild or mutated kinase, which provides guidance for drug evaluation and drug mechanism exploration. The binding kinetics of calcium ions to calmodulin is also measured, further broadening the application field of the method. In addition, the imaging capability allows mapping the local binding kinetics of the molecular interactions with a high resolution, which reveals visible spatial variability and offers a promising tool for studying heterogeneous local interfacial interactions.
研究领域:
分子生物学
·
药物发现
·
生物传感器
·
化学生物学
·
生物物理
·
转化医学
·
纳米生物技术
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）