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Polymer Chemistry · 2020 ·Vol. 11 ·期 31 ·5057-5066 · IF 5.342

Synthesis of novel Co(II) complexed bipyrimidine polyimide and preparation of thin film composite membranes

Jianrui Zhang,Xiaocui Han,Cheng Yue,Di Liu,Ziyu Lin,Yirong Sun,Liyuan Chen,Jinhui Pang,Zhenhua Jiang

A new diamine monomer with a dioxinyl bipyrimidine group was synthesized. Polyimide containing a bipyrimidine group was successfully homopolymerized by chemical imidization. Analyses to determine the structure and properties of these polymers were conducted using 1H NMR and FTIR spectroscopy and gel permeation chromatography (GPC). For the first time, cobalt acetate was incorporated into the synthesized polyimide to fabricate cobalt-complexed polyimide thin film composite membranes (TFCMs) by spin coating. To fully understand the behavior of cobalt complexed TFCMs, these membranes were synthesized and then characterized by FTIR spectroscopy, X-ray diffraction (XRD), and differential scanning calorimetry (DSC) to survey the effects of cobalt acetate on polyimide. The morphologies of TFCMs were determined using scanning electron microscopy (SEM) and energy dispersive X-ray spectroscopy (EDS). Phase separations and defects were absent in all cobalt-complexed TFCMs; the average thickness of the films ranged from 550 to 600 nm. This strongly suggested that cobalt acetate has good compatibility with bipyrimidine polyimide. The gas separation performance for TFCMs was also determined with the following results: the CO2 permeance of DMD-PI-3.0 (mixing 3.0 wt% cobalt acetate) TFCMs was 69.9 GPU at 35 °C and 1.5 bar while the selectivity of CO2/CH4 was 44.79 for DMD-PI-15 TFCMs. In short, this work reports a promising method to utilize the separation characteristics of polyimide TFCMs by incorporating cobalt ions.

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SOLAR ENERGY MATERIALS AND SOLAR CELLS · 2019 · IF 6.019

AIE-active electrochromic materials based on tetraphenylethylene cored benzoates with high optical contrast and coloration efficiency

Zhen-jie Huang,Hong-rong Mou,Jia-ping Xie,Feng Li,Cheng-Bin Gong,Qian Tang,Xiang-Kai Fu

In this work, a series of dual functional materials , 4,4′,4″,4‴-(ethene-1,1,2,2-tetrayl)tetrabenzoates (ETBAs), were developed with an aggregation-induced emission (AIE) luminogenic center (tetraphenylethylene) and electrochromically active moieties (benzoates). The highest occupied molecular orbital and lowest unoccupied molecular orbital energy levels of the ETBAs were determined via density functional theory calculations. The fluorescent, electrochemical, and electrochromic performances of the ETBAs were characterized via fluorescence spectroscopy , cyclic voltammetry , UV–Vis spectroscopy, and chronoamperometry . All the ETBAs demonstrated an AIE effect in water/N-methyl pyrrolidone. The ETBAs underwent a quasi-reversible reduction-oxidation. Electrochromic devices based on the ETBAs exhibited a significant color change from a transparent bleached state to a colored blue state, high optical contrast (ca. 80%), and large coloration efficiency. The used substituents markedly influenced the cyclability and response time, and compounds with a larger conjugation degree had lower energy gap values and faster response time. Compound c with a longer alkyl chain length had the best performance with regards to coloration efficiency and cyclability. In summary, this work demonstrated a strategy for the design of novel high-performance ECMs and could extend the applications of such multi-functional materials.

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NEW JOURNAL OF CHEMISTRY · 2019 ·Vol. 43 ·期 48 ·19223-19231 · IF 3.069

Effective ways to enhance the photocatalytic activity of ZnO nanopowders: high crystalline degree, more oxygen vacancies, and preferential growth

Yingying Lv,Jiayu Lin,Siyan Peng,Laijun Zhang,Leshu Yu

The practical application of ZnO nanopowders (NPs) in purifying wastewater could be determined by some issues, such as low-cost and scalable preparation, high photocatalytic activity, antiphotocorrosion, and convenient recycling. In this contribution, a series of ZnO NPs were prepared in a scalable way in the 220 °C, 250 °C and 280 °C autoclaves, respectively. The structural, morphological and surface details of the samples were systematically examined by XRD, SEM, FT-IR, TEM, Raman, PL, and UV-visible spectroscopy. Along with the increase of the reaction temperature, the mean diameter of ZnO NPs increased in the range of 110–130 nm, and the color of the products was lighter, resulting in a smaller surface area but a stronger UV absorbance in the region of 200–400 nm. Moreover, the preferential growth along the (002) plane, the crystalline degree and the green emission intensity of ZnO 280 are more overt than those of ZnO 250 and ZnO 220. Some other parameters including stretching vibration and E2(high) mode of Zn–O bonding or diffraction peaks of ZnO 280 also shifted to lower wavenumbers or lower angles when compared to those of ZnO 220, revealing the existence of more oxygen vacancies in ZnO 280. As expected, ZnO 280 showed the best photocatalytic activity and antiphotocorrosion among the three samples in the degradation of rhodamine B due to the availability of abundant oxygen vacancies, preferential growth along the (002) direction and the high crystalline degree. This suggests that, along with the increase of the preparation temperature, the obtained ZnO nanopowders exhibit better photocatalytic activity. Therefore this work could provide a route to synthesize well crystalline ZnO nanopowders and open up an avenue for commercial applications of ZnO NPs in the treatment of organic wastewater.

CAS / MDL: 7440-66-6
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ACS Omega · 2019 · IF 2.584

Fluorescent Porous Silica Microspheres for Highly and Selectively Detecting Hg2+ and Pb2+ Ions and Imaging in Living Cells

Wei Sun,Qi Sun,Qiang Zhao,Luminita Marin,Xinjian Cheng

In this work, SiO2 microspheres were first prepared by a conventional Stöber method and then etched by NaOH solution to obtain porous ones. By tuning the degree of etching, specific surface area of SiO2 microspheres could be controlled. Then, small fluorescent molecules are synthesized and incorporated onto the surface and/or pores of the SiO2 via layer-by-layer reaction to obtain fluorescent microspheres, namely, SiO2–NH2–BODIPY (SiNBB), SiO2–NH2–BODIPY–indole–benzothiazole (SiNBIT), and SiO2–NH2–BODIPY–indole–benzoxazole (SiNBIO). The as-prepared microspheres SiNBB exhibit highly sensitive and selective recognition ability for Hg2+ and Pb2+. When SiNBB encounters Hg2+ and Pb2+, the fluorescence intensity of SiNBB is increased up to fivefold. SiNBIT and SiNBIO are solely sensitive to Hg2+, and both have a single high sensitivity to recognize Hg2+. The adsorption efficiency of Hg2+ by the three fluorescent microspheres SiNBB, SiNBIT, and SiNBIO reached 2.91, 0.99, and 0.98 g/g of microspheres, respectively. Experimental results of A549 cells and zebrafish indicate that the fluorescent microspheres are permeable to cell membranes and organisms. The distribution of Hg2+ in the brain of zebrafish was obtained by the fluorescence confocal imaging technique, and Hg2+ was successfully detected in A549 cells and zebrafish.

✓ 已验证 产品关联 DOI PubMed 高影响因子
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BIORESOURCE TECHNOLOGY · 2019 · IF 6.669

Promotion of short-chain fatty acids production and fermented sludge properties via persulfate treatments with different activators: Performance and mechanisms

Jingyang Luo,Ying Zhu,Qin Zhang,Miao Cao,Wen Guo,Han Li,Yang Wu,Hui Wang,Yinglong Su,Jiashun Cao

This study explored the influences of peroxydisulfate (PDS) and peroxymonosulfate (PMS) activated with different catalysts on the anaerobic fermentation of waste activated sludge (WAS). All the treatments were effective in promoting short-chain fatty acids (SCFAs) production, particularly acetic acid, in the order of PMS/MnO 2  > PMS/Zn > PDS/Zn > PMS/Fe > PDS/Fe > PDS/MnO 2 . Mechanistic investigations demonstrated that WAS disintegration was intensely induced by the free radicals ( i.e., SO 4 − and OH) generated in PDS and PMS treating reactors. It significantly promoted the solubilization and hydrolysis processes and thereby provided sufficient bioavailable substrates for further acidogenic metabolisms. Additionally, it enlarged the abundance of functional bacteria responsible for SCFAs production. The simultaneous promotion of bioavailable substrates and fermentative microorganisms markedly contributed to the SCFAs enhancement. Moreover, the dewaterability and stabilization of fermented sludge were both improved with the PDS and PMS treatments, which were beneficial to the final disposal of WAS.

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Sustainable Energy & Fuels · 2019 ·Vol. 4 ·期 4 ·1621-1629 · IF 4.912

Heterovalent Ga3+ doping in solution-processed Cu2ZnSn(S,Se)4 solar cells for better optoelectronic performance

Yachao Du,Qingwen Tian,Jin Huang,Yuechao Zhao,Xiaohuan Chang,Afei Zhang,Sixin Wu

Additional elements in Cu2ZnSn(S,Se)4 (CZTSSe) absorber layers present a viable strategy to improve the performance of thin film solar cells. In this study, heterovalent cation doping by partially substituting metal cations with Ga3+ is explored by constructing a sandwich-like configuration. We demonstrated that a low doping level of Ga3+ can be successfully incorporated into the host lattice of CZTSSe to form a homogeneous Cu2ZnSn(Ga) (S,Se)4 (CZTGSSe) alloy material. Characterization was performed using SEM, EDS, XRD, Raman spectroscopy, and XPS, which showed that the material fabricated by this heterovalent cation doping method expressed high phase purity, appropriate valence components, and suitable optical bandgap, which are vital for high performance solar cells. As a result, the champion device achieves stabilized efficiency as high as 10.80%, improved by nearly 28% compared with only 8.43% for the reference device.

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Biomass Conversion and Biorefinery · 2020 ·Vol. 11 ·期 4 ·1245-1253 · IF 2.602

Expression and characterization of a cold-adapted, salt- and glucose-tolerant GH1 β-glucosidase obtained from Thermobifida halotolerans and its use in sugarcane bagasse hydrolysis

Yin Yi-Rui,Sang Peng,Xiao Min,Xian Wen-Dong,Dong Zhou-Yan,Liu Lan,Yang Li-Quan,Li Wen-Jun

A β-glucosidase obtained from Thermobifida halotolerans YIM 90462 T was expressed in Escherichia coli BL21 and subsequently characterized. The recombinant enzyme ThBGL1A showed optimal activity at 45 °C and pH 6, but also showed high activity from 40 to 55 °C and pH 5.6–6.6. Its half-life activity was 58 min at 50 °C. ThBGL1A exhibited notable cold-adapted activity, retaining 13.1%, 49.4%, and 83.5% of its optimal activity at 5, 25, and 30 °C, respectively. Kinetic characterization revealed an enzymatic turnover (Kcat) of 30 s −1 (cellobiose), 41.8 s −1 (p-nitrophenyl-β- d -glucopyranoside), and 52.6 s −1 (p-nitrophenyl-β- d -galactopyranoside). Moreover, ThBGL1A had high tolerance for salt, xylose, and glucose, which are extremely desirable features for industrial applications. Interestingly, its Ki for glucose was 932 mM and more than 80% of its optimal activity in the presence of 2000 mM xylose. After the addition of ThBGL1A (0.05 mg/ml) to a commercial cellulase reaction system, glucose yields from sugarcane bagasse were increased 20% and 18% after 1 day at 30 °C and 45 °C, respectively. Overall, this work identifies a cold-adapted, salt- and glucose-tolerant β-glucosidase with potential applications in commercial cellulose utilization and the bioenergy industry.

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MATERIALS CHEMISTRY AND PHYSICS · 2022 · IF 4.778

Perfluorocyclobutyl aryl ether-inserted vinyl silicone oil for crosslinking of fluorosilicone rubber

Shen Diao,Mingying Wang,Yuqiang Zhang

Vinyl silicone oil containing perfluorocyclobutyl aryl ether in the backbone (PFCB–VSO) was prepared by polycondensation of silane monomer containing perfluorocyclobutyl aryl ether (M 4 ), dimethyldimethoxysilane, and methyl vinyl dimethoxysilane in the acetic acid system. Fluorosilicone rubber was designed by using PFCB-VSO as a non-telechelic crosslinker. The effects of PFCB-VSO on the mechanical properties , thermal properties , and hydrophobic properties of fluorosilicone rubber were studied. The cross-link network of fluorosilicone rubber was investigated. The cross-link point was concentrated by the introduction of PFCB-VSO, which was demonstrated by cross-link density. The mechanical properties were enhanced by the growth of the non-telechelic cross-link network. The tensile strength was 10.35 MPa, the tear strength was 21.78 kN/m, and the elongation at break was 735%. The thermal stabilities and the hydrophobic properties of fluorosilicone rubber were increased by PFCB-VSO.

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MEDICINAL CHEMISTRY RESEARCH · 2022 ·Vol. 32 ·期 2 ·288-313 · IF 2.351

Study on structure-activity relationship (SAR) of simplified mirogabalin derivatives as voltage-gated calcium channel α2δ ligands for the treatment of chronic neuropathic pain

Zhang Yuanwen,Zheng Yueming,Wu Qingqing,Tian Fuyun,Ma Chuanjun,Xu Haiyan,Zhan Li,Gao Zhaobing,Zhao Guilong,Ti Huihui

A clinical therapy for chronic neuropathic pain is urgently needed, and the voltage-gated calcium channel (VGCC) α2δ subunit is among the most promising therapeutic targets. To intensively explore the structure-activity relationship (SAR) of the lipophilic moiety in VGCC α2δ subunit ligands (gabapentinoids), we designed and synthesized 11 bicyclic and monocyclic derivatives based on mirogabalin, a third-generation VGCC α2δ subunit ligand. The competitive binding of the synthesized compounds to the human VGCC α2δ-1 subunit was measured in vitro, and the results demonstrated that the lipophilic moiety size was strictly limited in gabapentinoids, in which conformationally rigid bicylo[3.2.0]heptane/heptene with a cis -fusion was the most preferred structure. In contrast, monocyclic cyclobutane was associated with a markedly decreased binding affinity except in 4 (IC 50  = 15.2 nM), in which the substituents could mimic the rigid conformation of bicylo[3.2.0]heptane/heptene; heteroatoms in the lipophilic moiety were detrimental to the binding affinity ( 2 , IC 50  > 729 nM). The SAR findings obtained in the present study will be valuable for designing novel gabapentinoid drugs to treat chronic neuropathic pain in the future. Graphical abstract

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ANALYTICA CHIMICA ACTA · 2022 · IF 6.911

A dual-responsive fluorescent turn-on sensor for sensitively detecting and bioimaging of hydrazine and hypochlorite in biofluids, live-cells, and plants

Ruiming Chen,Tingting Hu,Shu Xing,Tao Wei,Jianbin Chen,Tianduo Li,Qingfen Niu,Zhengyang Zhang,Huijun Ren,Xiaoxu Qin

Hydrazine (N 2 H 4 ) and hypochlorite (ClO − ) are extremely harmful to the public health, so it is vitally necessary to detect them in living system. Herein, we developed a new phenthiazine-thiobarbituric acid based dual-analyte responsive fluorescent sensor PT for visually distinguishing and detecting N 2 H 4 and ClO − . PT underwent N 2 H 4 /ClO − -induced C C breakage, achieving olive-drab/brilliant green fluorescence lighting-up response towards N 2 H 4 /ClO − with superb specifity, ultra-sensitivity (detection limit: 15.4 nM for N 2 H 4 , 13.7 nM for ClO − ), and ultra-fast response (N 2 H 4 : <15 s, ClO − : <20 s). The mechanisms for sensing N 2 H 4 and ClO − were investigated with support of spectral measurements and DFT investigation. Sensor based paper-strip/silica-gel device was developed for in-field supervision and on-site monitoring of gaseous and aqueous N 2 H 4 and ClO − solution. In addition, the PT was also applied for quantitatively detecting N 2 H 4 and ClO − in soil, food, plants and bio-fluids. Moreover, PT was utilized to visualize exogenous N 2 H 4 and ClO − in living plants and live-cells, demonstrating this sensor utilized as a powerful tool to detect N 2 H 4 and ClO − in biological fields.

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ANALYTICA CHIMICA ACTA · 2022 · IF 6.911

Highly selective SERS detection of acetylcholinesterase in human blood based on catalytic reaction

Yu Chen,Wenfeng Zhao,Jincheng Si,Yinuo Zheng,Hui Tan,Funa Meng,Guohai Yang,Yingqiu Gu,Lulu Qu

Acetylcholinesterase (AChE) is a key hydrolase in the cholinergic system, which directly determines the degradation of neurotransmitters . Therefore, it is a significant challenge to detect AChE in human blood with high sensitivity and selectivity in physiological and pathological processes. A novel nanoprobe by decorating the surface of gold nanoparticles with neostigmine (NE) AuNPs/NE was constructed for the AChE assay in serum. The principle is based on the specific recognition and cleavage of carbamate bonds in AuNPs/NE by AChE to form hydroxyl groups , resulting in changes of SERS spectra. The results show that 10 nm AuNPs/NE exhibit excellent catalytic activity for this reaction and the reaction rate is six times higher than that of 70 nm AuNPs/NE. Benefiting from the combined advantages of catalytic reaction specificity and molecular finger printing provided by SERS technology , AuNPs/NE exhibit high selectivity for AChE. The limit of detection (LOD) of this method for AChE activity was low to 0.02 U/mL. In addition, the spiked recovery of AChE in serum samples was 75.0%–119.2%. The proposed sensor also exhibits long-term stability and high biocompatibility with the increasing incubation time . More importantly, this work provides a new perspective for elucidating the role of AChE regulated by oxidative stress in the pathology of depression.

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SEPARATION AND PURIFICATION TECHNOLOGY · 2023 · IF 8.6

Sulfur-nitrogen synergistic active sites enable continuous and fast removal of organic pollutants in practical water matrix

Junjie Zhang,Yongjia Hong,Xu Tang,Yong Chen,Wenran Gao,Yuncheng Cai,Ningning Dong,Jiazi Xu,Li Zhang,Quli Fan,Bin Sun

The rational design of active sites in nanocarbons are the long-term pursuit for their practical applications. However, N, as the most potential active site, still encounters the problems of low atom utilization efficiency and stability in practical environmental remediation. Herein, we successfully constructed synergistic active sites consisting of graphitic N, pyridinic N, and thiophene S in heavy S, N co-doped hollow graphene spheres (HSNGS). The HSNGS exhibited exceptional efficiency in degrading tetracycline in real water, with a turnover frequency of 6.24 min −1 , which is among the highest reported. Moreover, tetracycline dissolved in practical water could be continuously and rapidly eliminated by passing through a column filled with HSNGS, maintaining its high performance even after 40 consecutive cycles. In the synergistic active sites, graphitic N and pyridinic N species accepted electrons from peroxymonosulfate, generating singlet oxygen for tetracycline degradation. Simultaneously, thiophene S coordinated with metal ions present in the practical water, synergistically enhancing the degradation of tetracycline. Additionally, the coordinated metal ions provided protection for the synergistic active sites during peroxymonosulfate activation, preventing their oxidation and enabling the continuous and rapid degradation of tetracycline. This work opens up possibilities for the industrial application of nanocarbon materials in environmental remediation.

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