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INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES · 2021 ·Vol. 22 ·期 8 ·4136 · IF 5.924

Chemical, Thermal, Time, and Enzymatic Stability of Silk Materials with Silk I Structure

Meihui Zhao,Zhenzhen Qi,Xiaosheng Tao,Chad Newkirk,Xiao Hu,Shenzhou Lu

The crystalline structure of silk fibroin Silk I is generally considered to be a metastable structure; however, there is no definite conclusion under what circumstances this crystalline structure is stable or the crystal form will change. In this study, silk fibroin solution was prepared from B. Mori silkworm cocoons, and a combined method of freeze-crystallization and freeze-drying at different temperatures was used to obtain stable Silk I crystalline material and uncrystallized silk material, respectively. Different concentrations of methanol and ethanol were used to soak the two materials with different time periods to investigate the effect of immersion treatments on the crystalline structure of silk fibroin materials. X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FTIR), Raman scattering spectroscopy (Raman), Scanning electron microscope (SEM), and Thermogravimetric analysis (TGA) were used to characterize the structure of silk fibroin before and after the treatments. The results showed that, after immersion treatments, uncrystallized silk fibroin material with random coil structure was transformed into Silk II crystal structure, while the silk material with dominated Silk I crystal structure showed good long-term stability without obvious transition to Silk II crystal structure. α-chymotrypsin biodegradation study showed that the crystalline structure of silk fibroin Silk I materials is enzymatically degradable with a much lower rate compared to uncrystallized silk materials. The crystalline structure of Silk I materials demonstrate a good long-term stability, endurance to alcohol sterilization without structural changes, and can be applied to many emerging fields, such as biomedical materials, sustainable materials, and biosensors.Keywords:silk fibroin;porous material;crystalline structure;stability

CAS / MDL: 64-17-5 67-56-1
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BIOMACROMOLECULES · 2020 · IF 6.092

Hierarchical Incorporation of Surface-Functionalized Laponite Clay Nanoplatelets with Type I Collagen Matrix

Jiabo Shi,Ruizhen Zhang,Na Yang,Yi Zhang,Bradley W. Mansel,Sujay Prabakar,Jianzhong Ma

Unraveling the interaction mechanisms of type I collagen with various inorganic nanoparticles is of pivotal importance to construct collagen-based bionanocomposites with hierarchical structures for biomedical, pharmaceutical, and other industrial applications. In this study, synthetic two-dimensional Laponite nanoplatelets (LAP NPs) are surface-functionalized with tetrakis(hydroxymethyl) phosphonium sulfate (THPS) for reinforcing their incorporation with type I collagen matrix by focusing on the influences of the interactions on the hierarchical structures of the collagen. Our results indicate that the LAP NPs can be successfully surface-functionalized with THPS via covalent bonds between the amine-functionalized NPs and the hydroxymethyl groups of THPS. Moreover, the resulting NPs can be well dispersed into the collagen matrix and evenly bound onto the collagen fiber strands and between the collagen fibrils, preserving the native D-periodic banding patterns of the collagen fibrils. The formation of covalent and hydrogen bonds between the collagen and the functionalized NPs can stabilize the intrinsic triple-helical conformation of the collagen, conferring the resulting collagen-based nanocomposites with improved thermal stability and enhanced mechanical properties. We anticipate that a fundamental understanding of the interactions between the collagen and functionalized inorganic nanoparticles would contribute to the design, fabrication, and further application of hierarchical collagen-based bionanocomposites with multifunctions.

CAS / MDL: 919-30-2 989-38-8
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CRYSTAL GROWTH & DESIGN · 2020 · IF 4.089

Low-Temperature Solution Growth and Characterization of Halogen (Cl, I)-Doped CsPbBr3 Crystals

Fangbao Wang,Hongjian Zhang,Qihao Sun,Ahmed Ben Hafsia,Zhangxuan Chen,Binbin Zhang,Yadong Xu,Wanqi Jie

The all-inorganic halide perovskite CsPbBr3 exhibited extraordinary photoelectric properties as well as great potential for various optic-electronic devices. The introduction of a Cl/I dopant is an effective method to optimize their properties. However, it is still a challenge to grow doped CsPbBr3 single crystals from solution. In this work, we report on the crystal growth of Cl/I-doped CsPbBr3 crystals using the modified inverse temperature crystallization (ITC) method. The components of raw materials and solvent in precursors were precisely tailored. The resulting doping ratio between the actual content and the nominal content are 0.99 and 0.046 for Cl and I, respectively. It indicates that I ion doped crystals exhibit more severe stoichiometric deviation due to the lower decomposition energy. The crystal structure, morphology, and optical properties of doped crystals were also investigated systematically. The {101} and {010} facets of as-grown crystals were influenced by the doping process. PL and UV transmittance spectra exhibited changes in the band gap in Cl/I-doped crystals. Finally, the phase diagram of basic photoelectric properties was determined for CsPb(Br1–nCln)3 crystals and it reveals conductive type changes from the P type to N type with an increase in the doping content of the Cl element. The optimum component of CsPb(Br0.93Cl0.07)3 demonstrates the highest resistivity of 4.3 × 109 Ω cm, an on/off ratio of ∼40, and a mobility of 414 cm2 V–1 s–1 as well as the lowest carrier concentration of 3.57 × 107 cm–3. Our work provides a strategy to grow doped halide perovskite crystals and tailor their optical and electrical properties.

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ACS Applied Nano Materials · 2020 · IF 0

Ultrathin BiOX (X = Cl, Br, I) Nanosheets with Exposed {001} Facets for Photocatalysis

Zidong Wang,Zhe Chu,Chunwei Dong,Ze Wang,Shiyu Yao,Hang Gao,Zhaoyu Liu,Yi Liu,Bai Yang,Hao Zhang

As a family of semiconductor photocatalysts, Sillén-type bismuth oxyhalides (BiOX, X = Cl, Br, I) have attracted widespread interest due to their excellent photocatalytic activity and photoconductivity. However, most current strategies on synthesizing ultrathin 2D BiOX nanosheets (NSs) rely on high temperature and pressure and complex procedures, which seriously confine their large-scale applications. Herein, we develop a simple and facile two-phase method for the synthesis of ultrathin 2D BiOX NSs with highly exposed {001} facets. On the basis of systematically studying the effects of various reaction parameters on the size, thickness, morphology, and composition of the products, the growth mechanism of ultrathin 2D BiOX NSs is presented, which indicates that the suppression of Bi3+ hydrolysis is required for the growth of 2D BiOX NSs with highly exposed {001} facets. The acidic condition prefers the growth of BiOX NSs with ultrathin structure and high crystallinity along the [001] zone axis. By using BiOBr NSs as the example, the photocatalytic activities of ultrathin 2D BiOX NSs are evaluated upon photodegradation of organic compounds and photocatalytic water oxidation. The results show that the organic compound photodegradation is mainly determined by the specific surface area of BiOBr NSs, while the O2 evolution rate of BiOBr NSs for water oxidation is dependent on their photogenerated charge separation efficiency. Because of the larger specific surface area and higher photogenerated charge separation efficiency, BiOBr-acid-0.5 ultrathin 2D NSs exhibits the fastest organic compound photodegradation rate and O2 evolution rate of 445.6 μmol g–1 h–1.

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ENZYME AND MICROBIAL TECHNOLOGY · 2019 · IF 3.553

Eco-efficient biphasic enzymatic hydrolysis for the green production of rare baohuoside I

Yuping Shen,Man Wang,Jinwei Zhou,Yufei Chen,Lili Xu,Mengru Wu,Guohua Xia,James P. Tam,Jiangnan Yu,Xiying Teng,Huan Yang,Xiaobin Jia

Baohuoside I, a rare secondary glycoside from Epimedii Folium, has anti-osteoporosis and other pharmacological effects. In addition, it exhibits improved bioactivities compared with its original glycoside icariin. Conventional methods for the production of baohuoside I, such as acid hydrolysis, exhibit very low efficiency with serious pollution and substantial byproducts. The aim of this study was to develop an eco-efficient biphasic enzymatic hydrolysis system for the green production of rare baohuoside I. β -glucanase was selected to hydrolyze icariin and showed better performance than β -glucosidase. The biphasic system was constructed using HAc-NaAc buffer (pH 4.5) containing β -glucanase/icariin (C icariin  = 100 mg/mL; 1:1, w/w ) and propyl acetate (1:2, v/v ), and the hydrolysis was performed at 60℃ for 6 h. The hydrolysis capacity of icariin in the system was largely increased from 0.5 mg/mL to 100 mg/mL. The conversion ratio of icariin was greater than 99% in a 100-fold scale-up pilot test, demonstrating its strong potential for industrial applications. Furthermore, a process flow and production plant were designed to produce 1 ton of baohuoside I annually, and the profit would be approximately 4.5-fold its total cost. Biphasic enzymatic hydrolysis is an eco-efficient technology to produce baohuoside I and represents a promising method in the pharmaceutical industry.

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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES · 2019 · IF 4.784

Efficient expression of chondroitinase ABC I for specific disaccharides detection of chondroitin sulfate

Xingyu Lu,Qian Zhong,Jian Liu,Fulin Yang,Chenghui Lu,Huan Xiong,Sha Li,Yibo Zhu,Lingtian Wu

Chondroitinase ABC I (ChSase ABC I) is a key enzyme of chondroitin sulfate (CS) degradation and widely used for CS detection in the medicine filed. However, the recombinant ChSase ABC I was weakly expressed in Escherichia coli because the forms of it were mostly inclusion bodies. In this study, a signal peptide ( pel B) was used for the soluble form expression of ChSase ABC I in E. coli . Then the culture condition for ChSase ABC I expression was optimized through response surface methodology. Results revealed that the expression level of ChSase ABC I in a 7.5 L fermentor (29.03 mL −1 ) was approximately 1.65-fold higher than that of the shake flask level (17.55 mL −1 ). The enzymatic properties and kinetic constants of recombinant ChSase ABC I were also studied. Recombinant ChSase ABC I was also used to detect the specific disaccharides content of CS from different sources. This study not only eliminates the problem of the enzyme expressed as an inclusion body, but also solves the current problem of expensive ChSase ABC. In a word, it would be an ideal strategy for ChSase ABC high-efficiency expression and a great method to detect specific disaccharides of CS in biomedical field.

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JOURNAL OF BIOMATERIALS SCIENCE-POLYMER EDITION · 2019 · IF 2.121

Bioactive nanoparticle embedded microcapsules for improving the efficacy of type I diabetes therapy

Mingzhi Zhu,Hongwei Wu,Weiji Weng,Ranjith Kumar Kankala,Pei Wang,Xia Zhou,Ruimin Long,Shibin Wang,Haiwang Huang,Yanhua Xia,Yuangang Liu

In order to overcome the side effects of pancreatic transplantation and insulin injection treatment for type I diabetes, we established a drug delivery system employing nanoparticle embedded microcapsules (NEMs). The system co-encapsulated chitosan nanoparticles with γ-aminobutyric acid and β-TC-6 cells for combined drug and cell therapy in diabetes mellitus (DM). The NEMs, which were formed via high-voltage electrostatic method, had an excellent sphericity with a smooth surface. The average size NEM was 245.52 ± 22.00 μm, which indicated a good size for cell encapsulation. Haemolysis rate of NEMs at concentrations of 100, 200 or 300 mg/mL were all below 5%. Relative viability rates of L929 cells with the same concentrations at 24, 48 or 72 h were all above 80%. We implanted bioactive NEMs into type 1 DM mice to evaluate the effect of the combined therapy. The level of blood glucose in the group receiving the combined therapy decreased during the first 2 weeks of treatment. During the next week, the level of blood glucose stayed in a safe range. Body weight continuously increased during the postoperative period after combined therapy group. Oral glucose tolerance test (OGTT) performed after 24 d showed that the level of blood glucose combined therapy reached the maximum peak of 13.04 mmol/L, lower than 16.56 mmol/L for the cell therapy group. This primary study indicated that microencapsulation technology and combined therapy are promising for the treatment of type I diabetes mellitus.

CAS / MDL: 9012-76-4
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NEW JOURNAL OF CHEMISTRY · 2019 ·Vol. 43 ·期 34 ·13408-13417 · IF 3.069

Syntheses and photoluminescence of copper(I) halide complexes containing dimethylthiophene bidentate phosphine ligands

Qiong Wei,Hong-Ting Chen,Li Liu,Xin-Xin Zhong,Lei Wang,Fa-Bao Li,Heng-Jiang Cong,Wai-Yeung Wong,Khalid A. Alamry,Hai-Mei Qin

High efficiency copper(I) halide complexes containing rigid diphosphine ligands have attracted much attention. However, rigid bidentate phosphine ligands have been rarely reported so far. Here, an electron-rich heteroaryl ring grafted with two electron donating methyl groups was first included to construct a rigid bidentate phosphine ligand, three four-coordinate dinuclear copper(I) halide complexes, [CuX(dpmt)]2 (dpmt = 3,4-bis(diphenylphosphino)-2,5-dimethylthiophene, X = I (1), Br (2) and Cl (3)), were synthesized, and their molecular structures and photophysical properties were investigated. The structural analysis reveals that two copper(I) centers are bridged by two halogen ligands to form a dinuclear structure with a four-membered Cu2X2 ring. These complexes exhibit intense bluish green to yellow green emission in the solid state at room temperature and have peak emission wavelengths at 490–543 nm with microsecond lifetimes (τave = 3.9–13.6 μs, Φ = 0.26–0.35). The emission of complex 1 mainly originates from MLCT and ligand-centered transitions. Similar emissive behaviors for complexes 2 and 3 are possibly due to ligand-centered transition. The solution-processed devices of complex 3 exhibit stable yellow emission with CIE(x, y) of (0.42, 0.52) for doped and nondoped devices.

CAS / MDL: 7758-89-6
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DALTON TRANSACTIONS · 2018 ·Vol. 47 ·期 29 ·9845-9849 · IF 4.099

Ultrathin CsPbX3 (X = Cl, Br, I) nanoplatelets: solvothermal synthesis and optical spectroscopic properties

Daqin Chen,Xiao Chen,Junni Li,Xinyue Li,Jiasong Zhong

The preparation of CsPbX3 nanoplatelets and the investigation of their optical properties have been rarely reported. Herein, the successful development of all-inorganic CsPbX3 (X = Cl, Br, or I) perovskite quantum dots has been achieved and their unique optical and electrical properties are discussed. Apre-dissolution assisted solvothermal reaction was developed to synthesize ultrathin (∼3 nm) CsPbBr3 nanoplatelets with strong exciton absorption, with a 0.41 eV blue-shifted emission relative to that of CsPbBr3 nanocrystals and a high quantum yield of 28%. Anion exchange allowed the variation of the halogen content of the nanoplatelets and allowed them to retain their shape and size and achieve multi-color emission.

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FOOD CHEMISTRY · 2018 · IF 4.946

Ultrasensitive detection of Sudan I in food samples by a quantitative immunochromatographic assay

Diandian Deng,Hong Yang,Chang Liu,Kang Zhao,Jianguo Li,Anping Deng

An immunochromatographic assay (ICA) based on surface-enhanced Raman scattering (SERS) for ultrasensitive determination of Sudan I in food samples was reported. Gold-silver core-shell bimetallic nanorods (referred to as [email protected] NRs) were synthesized, characterized and used as the substrate for preparation of the ICA. Polyclonal antibody against Sudan I was immobilized on the surface of the [email protected] NRs carrying the Raman reporter 5,5′-dithiobis (2-nitrobenzoic acid). The Raman scattering intensity on the test line was used for quantitation of Sudan I. The assay was completed in 15 min. IC 50 and limit of detection (LOD) were 30 pg mL −1 and 0.2 pg mL −1 , respectively. There was no cross-reactivity (CR) of the assay with Sunset Yellow, Lemon Yellow and Brilliant blue FCF, but only 3.53%-9.74% CR with Sudan II, III and IV. The recoveries of Sudan I from spiked food samples were in the range of 88.9–107.6% with relative standard deviation of 3.7–8.7% (n = 3).

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ORGANIC & BIOMOLECULAR CHEMISTRY · 2018 ·Vol. 16 ·期 48 ·9402-9408 · IF 3.423

A pH responsive fluorescent probe based on dye modified i-motif nucleic acids

Pan Li,Zhe Chen,Yishun Huang,Jing Li,Fan Xiao,Shiyao Zhai,Zhiming Wang,Xuanjun Zhang,Leilei Tian

A new DNA-based fluorescent probe, which is a hybrid molecule of an i-motif forming sequence (IFS) and mono-functionalized tetraphenylethene (TPE), has been synthesized and investigated. A distinct pH-responsive aggregation-induced emission (AIE) effect has been observed from this hybrid molecule, i.e. the fluorescence of TPE will be turned on when the IFS part folds up under acidic conditions. According to the fact that a hybrid molecule with a relatively rigid structure shows a more obvious AIE effect, and whose nano-sized aggregates are formed at a high concentration, we assume that the solubility of the hybrid molecule in water will be reduced due to IFS folding, resulting in aggregation and the resultant AIE effect. Finally, due to its excellent pH responsiveness, this DNA-based probe employing an AIEgen has been applied in monitoring intracellular pH.

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JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS · 2019 ·Vol. 30 ·期 16 ·14977-14986 · IF 2.195

Effect of I/Ag molar ratio on silver thick films below 550 °C

Tang Hongbo,Li Qiuyue,Zhou Jian

The effect of low I/Ag ratios on the performance of silver thick films containing micro-sized silver particles treated with surface iodination has been investigated. The film with I/Ag ratio of 1:100 exhibited high electrical conductivity and densification, while that of 2:100 presented better adhesion. The conductivity and densification of the film reached the highest at 550 °C. Optimal conductivity of the film with I/Ag ratio of 1:100 and 2:100 was 11.45 and 15.85 mΩ/sq., respectively. In addition, the film adhesion was enhanced by heating. Different trends observed in electrical conductivity and adhesion as functions of temperature is primarily attributed to shrinkage of modified particles. This work suggested that the I/Ag ratio plays a vital effect on the performance of the silver thick film.

CAS / MDL: 7761-88-8
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