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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS · 2023 · IF 5.2

Role of oil polarity on myofibrillar protein emulsions stability: A multi-scale research

Weiyi Zhang,Haozhen Zhang,Xinglian Xu,Xue Zhao

The oil polarity was hypothesized to significantly influence the microscopic conformation of interfacial myofibrillar protein (MP) and thus the mesoscopic interfacial rheology of MP film , which ultimately tuned the macroscopic stability of MP-stabilized emulsions. In this research, the inner mechanism was revealed hierarchically based on emulsions multi-scale properties, by a combination of in vitro interfacial concentration measurement, dynamic interfacial tension measurement and interfacial dilatational rheology (highlighting Lissajous plots). Then, the above conclusion was verified through in silico molecular dynamic simulation. At macroscopic level, the light scattering results showed that emulsion prepared with higher polarity oil exhibited higher physical stability. This could be explained from the mesoscopic perspective that: (1) the adsorption dynamics of MP was faster (though lower diffusion rate, but higher penetration and rearrangement rate) on the higher polarity interface, which decreased interfacial tension more efficiently; (2) adsorption ratio, surface load and desorption ratio indicated that ‘multilayer interfacial film’ was formed by loosely-bound MP on the lower polarity interface, which decreased the effective interfacial coverage to impair emulsions stability; (3) Lissajous plots showed that interfacial structure with higher stability against large deformation was formed on the higher polarity oil interface. Finally, the microscopic molecular mechanism for explaining the above findings was revealed by in silico molecular dynamic simulation: though MP was less unfolded on the higher polarity interface leading to weaker intermolecular hydrophobic interactions, this compact molecular structure with stronger intramolecular rigidity predominantly contributed to steadier interfacial film structure. This multi-scale study provides a deep insight into the inner relationship between oil polarity and emulsions stability.

研究领域: 食品科学 · 胶体与界面化学 · 蛋白质构象 · 软物质物理 · 分子模拟
✓ 已验证 DOI 高影响因子
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BIORESOURCE TECHNOLOGY · 2015 · IF 4.494

Effect of the molecular structure of lignin-based polyoxyethylene ether on enzymatic hydrolysis efficiency and kinetics of lignocelluloses

Xuliang Lin,Xueqing Qiu,Duming Zhu,Zihao Li,Ningxin Zhan,Jieyi Zheng,Hongming Lou,Mingsong Zhou,Dongjie Yang

Effect of the molecular structure of lignin-based polyoxyethylene ether (EHL–PEG) on enzymatic hydrolysis of Avicel and corn stover was investigated. With the increase of PEG contents and molecular weight of EHL–PEG, glucose yield of corn stover increased. EHL–PEG enhanced enzymatic hydrolysis of corn stover significantly at buffer pH 4.8–5.5. Glucose yield of corn stover at 20% solid content increased from 32.8% to 63.8% by adding EHL–PEG, while that with PEG4600 was 54.2%. Effect of EHL–PEG on enzymatic hydrolysis kinetics of cellulose film was studied by quartz crystal microbalance with dissipation monitoring (QCM-D) and atomic force microscopy (AFM). An enhancing mechanism of EHL–PEG on enzymatic hydrolysis kinetics of cellulose was proposed. Cellulase aggregates dispersed by EHL–PEG excavated extensive cavities into the surface of cellulose film, making the film become more loose and exposed. After the maximum enzymatic hydrolysis rate, the film was mainly peeled off layer by layer until equilibrium.

研究领域: 生物质转化 · 酶工程 · 高分子化学 · 表面科学 · 可再生能源
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JOURNAL OF POLYMER SCIENCE PART A-POLYMER CHEMISTRY · 2012 ·Vol. 50 ·期 24 ·5177-5184 · IF 3.919

Dicarboxylic acid promoted immortal copolymerization for controllable synthesis of low-molecular weight oligo(carbonate-ether) diols with tunable carbonate unit content

Yonggang Gao,Lin Gu,Yusheng Qin,Xianhong Wang,Fosong Wang

Low-molecular weight oligo(carbonate-ether) diols are important raw materials for polyurethane formation, which with tunable carbonate unit content (CU) may endow new thermal and mechanical performances to polyurethane. Herein, facile synthesis of oligo(carbonate-ether) diols with number average molecular weight ( M n ) below 2000 g mol −1 and CU tunable between 40% and 75% are realized in high activity by immortal copolymerization of CO 2 /propylene oxide (PO) using zinc-cobalt double metal cyanide complex (Zn-Co-DMCC) in the presence of sebacic acid (SA). M n of the oligomer is in good linear relationship to the mole ratio of PO and SA (PO/SA) and hence can be precisely controlled by adjusting PO/SA. Besides, the molecular weight distribution is quite narrow due to the rapid reversible chain transfer in the immortal copolymerization. High pressure and low temperature are favorable for raising CU. In all the reactions, the weight fraction of propylene carbonate ( W PC ) can even be controlled as low as 2.0 wt %, and the catalytic activity of Zn-Co-DMCC is above 1.0 kgg −1 cat. © 2012 Wiley Periodicals, Inc. J Polym Sci Part A: Polym Chem, 2012

研究领域: 高分子化学 · 催化化学 · 绿色化学 · 功能材料 · 聚合物合成 · 二氧化碳利用
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PHYSICAL CHEMISTRY CHEMICAL PHYSICS · 2016 ·Vol. 18 ·期 29 ·19731-19737 · IF 4.449

Experimental and theoretical studies on compositions, structures, and IR and NMR spectra of functionalized protic ionic liquids

Yingna Cui,Jingmei Yin,Changping Li,Shenmin Li,Ailing Wang,Guang Yang,Yingping Jia

The compositions and structures of amine-based functionalized protic ionic liquids (PILs), namely N,N-dimethyl(cyanoethyl)ammonium propionate (DMCEAP) and N,N-dimethyl(hydroxyethyl)ammonium propionate (DMEOAP) have been investigated systematically by IR and 1H NMR spectroscopy and density functional theory (DFT) calculations. Analysis of the IR spectra suggests that both DMCEAP and DMEOAP are composed of neutral and ionized species in the liquid phase, the former one mainly existing in the state of precursor molecules, and the latter mainly as ion-pairs. The ratio of precursor molecules to ion-pairs in the liquid phase depends on the types of precursors, especially the functional groups of cations. 1H NMR spectra indicate that there is a dynamic equilibrium between the neutral and ionized species, probably due to the formation of some intermediates in the PILs. The DFT calculations have been carried out to reveal the conformation, and obtain the corresponding IR and 1H NMR spectra of the neutral and ionized species, so that the theoretical support to the experimental results can be provided. The present study will help understand the properties of PILs and provide guidance for further applications of PILs.

研究领域: 物理化学 · 离子液体化学 · 光谱学 · 理论化学 · 分析化学 · 材料化学
✓ 已验证 DOI 高影响因子
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Small · 2017 ·Vol. 14 ·期 7 ·1702288 · IF 8.643

Bioadhesive Polymersome for Localized and Sustained Drug Delivery at Pathological Sites with Harsh Enzymatic and Fluidic Environment via Supramolecular Host–Guest Complexation

Meiling Zhu,Kongchang Wei,Sien Lin,Xiaoyu Chen,Chia-Ching Wu,Gang Li,Liming Bian

Targeted and sustained delivery of drugs to diseased tissues/organs, where body fluid exchange and catabolic activity are substantial, is challenging due to the fast cleansing and degradation of the drugs by these harsh environmental factors. Herein, a multifunctional and bioadhesive polycaprolactone-β-cyclodextrin (PCL-CD) polymersome is developed for localized and sustained co-delivery of hydrophilic and hydrophobic drug molecules. This PCL-CD polymersome affords multivalent crosslinking action via surface CD-mediated host–guest interactions to generate a supramolecular hydrogel that exhibits evident shear thinning and efficient self-healing behavior. The co-delivery of small molecule and proteinaceous agents by the encapsulated PCL-CD polymersomes enhances the differentiation of stem cells seeded in the hydrogel. Furthermore, the PCL-CD polymersomes are capable of in situ grafting to biological tissues via host–guest complexation between surface CD and native guest groups in the tissue matrix both in vitro and in vivo, thereby effectively extending the retention of loaded cargo in the grafted tissue. It is further demonstrated that the co-delivery of small molecule and proteinaceous drugs via PCL-CD polymersomes averts cartilage degeneration in animal osteoarthritic (OA) knee joints, which are known for their biochemically harsh and fluidically dynamic environment.

研究领域: 药物递送 · 生物材料 · 组织工程 · 纳米医学 · 再生医学 · 关节生物学 · 转化医学
✓ 已验证 DOI 高影响因子
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JOURNAL OF POLYMER SCIENCE PART A-POLYMER CHEMISTRY · 2012 ·Vol. 50 ·期 23 ·4871-4878 · IF 3.919

Synthesis of crosslinked poly(butyl methacrylate-co-pentaerythritol triacrylate) gel by single electron transfer-living radical polymerization and its oil-absorbing properties

Lijun Fan,Hou Chen,Zhihai Hao,Zhi Tan

A novel high oil-absorbing crosslinked gel was synthesized by copolymerization of butyl methacrylate (BMA) with a small amount of pentaerythritol triacrylate (PETA) crosslinker using single electron transfer-living radical polymerization (SET–LRP) initiated with carbon tetrachloride (CCl 4 ) and catalyzed by Cu(0)/hexamethylenetetramine (HMTA) in N, N-dimethylformamide (DMF). The polymerization followed first-order kinetics as indicated by linear increase of monomer concentration with reaction time. Effects of reaction temperature, crosslinker, initiator, and catalyst on the oil-absorbing properties of the crosslinked gel were investigated in detail. The oil absorptions of the crosslinked gel to chloroform, toluene could reach 51.9, 34.5 g/g, respectively. © 2012 Wiley Periodicals, Inc. J Polym Sci Part A: Polym Chem, 2012

研究领域: 高分子化学 · 功能材料 · 环境修复 · 石油泄漏处理 · 聚合物科学
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Journal of Energy Chemistry · 2022 · IF 13.599

Hyperbranched phthalocyanine enabling black-phase formamidinium perovskite solar cells processing and operating in humidity open air

Rong Li,Jiale Ding,Xijiao Mu,Yifei Kang,Anran Wang,Weihui Bi,Yunhe Zhang,Jing Cao,Qingfeng Dong

The extreme instability of pure α-phase FAPbI 3 under high humidity conditions restricts the high-throughput fabrication in unmodified air environments, resulting in poor performance of α-phase FAPbI 3 perovskite devices obtained by scalable fabrication methods. Here we synthesized hyperbranched copper phthalocyanine (HCuPc) as a supramolecular additive with twisted phthalocyanine units to realize the molecular-level encapsulation at the grain boundaries through supramolecular interaction, which greatly broadened the processing window of FAPbI 3 under high humidity. At the same time, unlike traditional encapsulation layer that carrier can only be collected by tunneling effect, the twisted phthalocyanine ring of HCuPc in perovskite films is more conducive to hole extraction. Finally, a record efficiency was achieved in pure FAPbI 3 based inverted structured solar cell by blade-coating to the best of our knowledge, even under unmodified humid air conditions (relative humidity of 65%–85%). The best operational stability of 3D pure FAPbI 3 devices can also be achieved at the same time and unencapsulated HCuPc-FAPbI 3 device can even operate with negligible degradation for 100 h in the open air (RH 30%–40%).

研究领域: 材料科学 · 纳米科技 · 能源化学 · 光伏技术 · 表面与界面化学
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