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Journal of Materials Chemistry B · 2017 ·Vol. 5 ·期 22 ·4052-4059 · IF 4.543

Facile synthesis of magnetic covalent organic frameworks for the hydrophilic enrichment of N-glycopeptides

Heping Wang,Fenglong Jiao,Fangyuan Gao,Junjie Huang,Yan Zhao,Yehua Shen,Yangjun Zhang,Xiaohong Qian

Protein glycosylations play important roles in various biological processes and in the disease progression of organisms. The development of specific enrichment materials and strategies before mass spectrometric analysis was a prerequisite to glycoproteomic analysis due to the difficulty caused by substoichiometric levels of glycoproteins. In this work, novel magnetic covalent organic frameworks (denoted as Fe3O4@TpPa-1) were first developed using only a two-step solvothermal reaction and then applied in the hydrophilic enrichment of glycopeptides. Sea urchin-type composites with super-paramagnetic properties were constructed by in situ growth of TpPa-1 covalent organic frameworks on the surface of magnetic nanoparticles. A total of 37 and 22 glycopeptides could be easily detected from IgG and HRP digests, respectively, by hydrophilic enrichment with the newly developed materials. An ultralow detection limit (28 fmol), satisfactory selectivity and high recovery could be achieved using Fe3O4@TpPa-1. The material's excellent enrichment performance was also demonstrated using glycopeptide analysis in real complex samples. Within three independent replicates, 228 glycopeptides corresponding to 114 glycoproteins could be detected from human serum digests, which is better than the performance obtained by commercial HILIC materials. The results suggest that covalent organic frameworks show potential for application in glycoproteomic studies.

CAS / MDL: 106-50-3
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ADVANCED FUNCTIONAL MATERIALS · 2016 ·Vol. 26 ·期 9 ·1400-1410 · IF 11.382

An Interface Engineered Multicolor Photodetector Based on n-Si(111)/TiO2 Nanorod Array Heterojunction

Tao Ji,Qian Liu,Rujia Zou,Yangang Sun,Kaibing Xu,Liwen Sang,Meiyong Liao,Yasuo Koide,Li Yu,Junqing Hu

A multicolor photodetector based on the heterojunction of n-Si(111)/TiO 2 nanorod arrays responding to both ultraviolet (UV) and visible light is developed by utilizing interface engineering. The photodetector is fabricated via a consecutive process including chemical etching, magnetron sputtering, hydrothermal growth, and assembling. Under a small reverse bias (from 0 to ≈−2 V), only the photogenerated electrons in TiO 2 are possible to tunnel through the low barrier of Δ E C , and the device only responses to UV light; as the reverse bias increases, the photogenerated holes in Si also begin to tunnel through the high barrier of Δ E V . As a result, the device is demonstrated to have the capacity to detect both UV and visible lights, which is useful in the fields of rapid detection and multicolor imaging. It has been also observed that the crystal orientation of Si affects the characteristics of bias-controlled spectral response of the n-Si/TiO 2 heterojunctions.

CAS / MDL: 5593-70-4 9022-96-2
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ACS Applied Materials & Interfaces · 2016 · IF 7.145

Highly Functional Bioinspired Fe/N/C Oxygen Reduction Reaction Catalysts: Structure-Regulating Oxygen Sorption

Yingfang Yao,Yong You,Gaixia Zhang,Jianguo Liu,Haoran Sun,Zhigang Zou,Shuhui Sun

Tuna is one of the most rapid and distant swimmers. Its unique gill structure with the porous lamellae promotes fast oxygen exchange that guarantees tuna’s high metabolic and athletic demands. Inspired by this specific structure, we designed and fabricated microporous graphene nanoplatelets (GNPs)-based Fe/N/C electrocatalysts for oxygen reduction reaction (ORR). Careful control of GNP structure leads to the increment of microporosity, which influences the O2 adsorption positively and desorption oppositely, resulting in enhanced O2 diffusion, while experiencing reduced ORR kinetics. Working in the cathode of proton-exchange membrane fuel cells, the GNP catalysts require a compromise between adsorption/desorption for effective O2 exchange, and as a result, appropriate microporosity is needed. In this work, the highest power density, 521 mW·cm–2, at zero back pressure is achieved.

CAS / MDL: 108-78-1 89-32-7
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JOURNAL OF MOLECULAR LIQUIDS · 2016 · IF 2.74

Kinetics of a hydrolysis reaction in critical surfynol465/n-butanol/ethyl acetate/water microemulsion

Jinshou Wang,Jing Jin,Yanbin Tan,Zhen Shi,Shenghu Zhang

We have constructed the pseudoternary phase diagram of surfynol465/ n -butanol/ethyl acetate/water with mass ratio of surfynol465 to n -butanol being 1.0. In the O/W microemulsion region, we have measured the rate of a first-order hydrolysis reaction of tert-butyl bromide near and far away from the critical point. In the noncritical region, the rate constants of the reaction obey respective Arrhenius equation. In the critical region, the rate constants did not deviate from Arrhenius equation, and no critical effect was apparent, which agreed with the Griffiths–Wheeler rule. This work extended the studies of critical effect on the chemical reaction to more complicated O/W microemulsion media and added to the current interest in microemulsion system functioning as media for chemical reactions.

CAS / MDL: 507-19-7
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JOURNAL OF CHROMATOGRAPHY A · 2016 · IF 3.926

Synthesis of magnetic zwitterionic–hydrophilic material for the selective enrichment of N-linked glycopeptides

Yiman Zhao,Yajing Chen,Zhichao Xiong,Xudong Sun,Quanqing Zhang,Yangyang Gan,Lingyi Zhang,Weibing Zhang

In consideration of the close connection between glycopeptides and human diseases, the efficient method to separate and enrich glycopeptides from complex biological samples is urgently required. In the work, we developed a magnetic zwitterionic-hydrophilic material for highly effective separation and analysis of glycopeptides from complex samples. The Fe 3 O 4 particles were covered with a thick layer of polymer by one-step reflux-precipitation polymerization (RPP), subsequently decorated by Au nanoparticles (Au NPs) through in situ reduction and finally modified with zwitterionic groups. The abundant zwitterionic sites facilitate the selective enrichment of glycopeptides. Besides, the prepared Fe 3 O 4 @PGMA@Au- l -cys showed high detection sensitivity (5 fmol IgG digest), approving enrichment capacity (75   mg   g −1 ), satisfactory enrichment recovery (89.8%), and great performance in the analysis and profiling of low-abundance N-linked glycopeptides. Furthermore, the prepared material was employed in the enrichment of glycopeptides in intricate biological samples, and 774 unique N -glycosylation sites from 411 N -glycosylated proteins were reliably identified in three replicate analyses of a 75   μg protein sample extracted from mouse liver, suggesting wide application prospect in glycoproteomics.

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JOURNAL OF BIOMATERIALS SCIENCE-POLYMER EDITION · 2016 · IF 1.733

Fabrication of magnetic nanoparticles armed with quaternarized N-halamine polymers as recyclable antibacterial agents

Xi Wang,Qian Xiang,Weiwei Cao,Feng Jin,Xuefeng Peng,Bingcheng Hu,Xiaodong Xing

Magnetic recyclable bactericidal nanocomposites (Fe3O4@PDMC) were well-designed and prepared by coating of Fe3O4 nanoparticles with quaternarized N-halamine polymers via the free radical polymerization process. In which, 5,5-dimethylhydantoinyl-(3-ethyl-methacrylamine)propyl dimethylammonium bromide (DEMPA), a new monomeric N-halamine precursor, was used as a coating material as well as the dual-functional bactericidal agent. The developed Fe3O4@PDMC nanocomposites exhibited suitable size and super-paramagnetic responsibility. The antibacterial results showed that the Fe3O4@PDMC nanocomposites had excellent biocidal abilities against Staphylococcus aureus (gram-positive) and Escherichia coli (gram-negative). Furthermore, the TTC (Triphenyl Tetrazolium Chloride)–dehydrogenase activity assay confirmed that the reductions of the bacteria were mainly attributed to powerful biocidal effects of the coating polymer instead of bacteria capture by the cationic surface. Interestingly, due to the magnetic responsive performance of Fe3O4, the as-prepared Fe3O4@PDMC nanocomposites can be recycled by a magnet and reused for antibacterium through the quenching/rechlorination procedure. All the results presented in this study show that the proposed Fe3O4@PDMC nanocomposites could be a competitive candidate for water purification systems and household sanitation.

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SENSORS AND ACTUATORS B-CHEMICAL · 2016 · IF 4.758

Introducing p-n junction interface into enzyme loading matrix for enhanced glucose biosensing performance

Sisi Fan,Minggang Zhao,Longjiang Ding,Ye Ma,Jingjing Liang,Xingtao Wang,Yawen Song,Shougang Chen

Eggshell membranes were used as biotemplate to fabricate a 3D hierarchical porous Co 3 O 4 /ZnO p-n junction film. Multiple catalysis and accelerated electron transfer were achieved on the Co 3 O 4 /ZnO-GOx electrode by introducing the p-n junction interface into enzyme loading matrix. A stable and well-defined oxidation peak of glucose was obtained with a largely decreased detection potential of 0.25   V. Furthermore, an enhanced sensitivity (116.64   μA·mM −1 ·cm −2 ) was also achieved comparing with the simple biotemplate-synthesized Co 3 O 4 and ZnO film. The results demonstrated it is a novel strategy to improve the biosensing performance by introducing p-n junction interface into enzyme loading matrix.

CAS / MDL: 9012-76-4
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Nanomaterials · 2017 ·Vol. 7 ·期 10 ·338 · IF 3.553

Study of the Photodynamic Activity of N-Doped TiO2 Nanoparticles Conjugated with Aluminum Phthalocyanine

Xiaobo Pan,Xinyue Liang,Longfang Yao,Xinyi Wang,Yueyue Jing,Jiong Ma,Yiyan Fei,Li Chen,Lan Mi

TiO2nanoparticles modified with phthalocyanines (Pc) have been proven to be a potential photosensitizer in the application of photodynamic therapy (PDT). However, the generation of reactive oxygen species (ROS) by TiO2nanoparticles modified with Pc has not been demonstrated clearly. In this study, nitrogen-doped TiO2conjugated with Pc (N-TiO2-Pc) were studied by means of monitoring the generation of ROS. The absorbance and photokilling effect on HeLa cells upon visible light of different regions were also studied and compared with non-doped TiO2-Pc and Pc. Both N-TiO2-Pc and TiO2-Pc can be activated by visible light and exhibited much higher photokilling effect on HeLa cells than Pc. In addition, nitrogen-doping can greatly enhance the formation of1O2and •O2−, while it suppresses the generation of OH•. This resulted in significant photodynamic activity. Therefore, N-TiO2-Pc can be an excellent candidate for a photosensitizer in PDT with wide-spectrum visible irradiation.Keywords:titanium dioxide;phthalocyanine;reactive oxygen species;photodynamic therapy

CAS / MDL: 919-30-2
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ENERGY & FUELS · 2017 · IF 3.091

Kinetics of Carbon Dioxide Hydration Enhanced with a Phase-Change Slurry of n-Tetradecane

Bin Chen,Feng Xin,Xiaofei Song,Xingang Li,Muhammad Zeshan Azam

CO2 capture based on hydrate formation is intensified by an oil-in-water phase-change slurry (PCS) in which the n-tetradecane particles are taken as nucleation centers and are used to directly remove the hydration heat through their solid-to-liquid phase change. In this study, experiments on hydration were conducted at a temperature of 277.6 K and under isobaric pressures in the range of 2.1–2.4 MPa. All measurements were performed at a stirring speed of 450 rpm in PCSs of 25–45 wt % n-tetradecane. Two kinetics models, transport and reversible hydration, were established to regress and analyze the experimental data from the isothermal hydration of CO2 in a semibatch hydrator. For each model, the effects of pressure and PCS composition were examined in detail. As the experimental results show, the induction time before hydration initiated was less than 1 min for all runs, and the duration of the entire hydration process was approximately 13–15 min for each measurement. Furthermore, the average hydration rate reached 197 mol m–3 min–1 at 2.3 MPa in 45 wt % oil-in-water PCS, which demonstrates that the presence of n-tetradecane particles contributes significantly to the enhancement of hydrate formation rate. As the modeling results show, the parameters of the two models were determined by correlating the experimental data, and the interpretations of the measurements by the two models are satisfactory.

CAS / MDL: 629-59-4
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CARBON · 2017 · IF 6.337

Fe-N-doped porous carbon from petroleum asphalt for highly efficient oxygen reduction reaction

Jingyan Liu,Yang Liu,Peng Li,Luhai Wang,Haoran Zhang,Hui Liu,Jialiang Liu,Yixian Wang,Wei Tian,Xiaobo Wang,Zhongtao Li,Mingbo Wu

Fe-N-doped porous carbon derived from petroleum asphalt (NPCA) was prepared via a facile template synthesis method, with urea as nitrogen source while α-Fe 2 O 3 nanoparticles as template and Fe source. The as-prepared NPCA calcined at 900 °C (NPCA-900) exhibits excellent electrocatalytic performance with high diffusion-limiting current density and stability comparable to those of commercial Pt/C catalysts in alkaline environment . The remarkable ORR performance of NPCA could be ascribed to the abundant porosity, large specific surface area (1060 m 2  g −1 ), as well as the doping of Fe-N (especially pyridinic N). The NPCA derived from cheap petroleum asphalt has good application future in the field of catalysis, while it may pave a new way to realize the clean and high value utilization of heavy oils.

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RSC Advances · 2016 ·Vol. 6 ·期 95 ·92739-92747 · IF 3.289

N-, Fe-Doped carbon sphere/oriented carbon nanofiber nanocomposite with synergistically enhanced electrochemical activities

Li Zhang,Wei Wan,Qiang Wang,Wen-Chao Lu,Bei-Hua Hou,Ping Chen

Catalysts for the oxygen reduction reaction (ORR) are crucial in metal–air batteries, fuel cells and other electrochemical devices. Developing heteroatom-doped carbon catalysts with high performance and stability in alkaline media for practical application of metal–air batteries or in acidic media for practical application of proton exchange membrane fuel cells is still difficult and challenging. Here, we report the N-, Fe-doped carbon sphere/oriented carbon nanofiber nanocomposite (NFe-CS/CNF). N-, Fe-doped carbon spheres (NFe-CS) were derived from p-phenylenediamine and oriented N-, Fe-doped carbon nanofibers (NFe-CNF) were derived from o-phenylenediamine. 3.89 at% of N and 0.38 at% of Fe were doped in a typical product, which has high surface area. The typical product exhibits a high ORR activity and stability in acidic media and reveals superior stability and tolerance to methanol than Pt/C. In alkaline media, the typical product shows superior activity to Pt/C. The performance of a zinc–air full cell under real battery operation conditions indicates that the typical product is a competitive alternative to commercial PtC. The unique structure of NFe-CS/CNF could create strong interactions between the nanospheres and oriented nanofibers, promote charger transfer at the interface and improve the conductivity. This work provides a new fundamental understanding and design strategy for excellent carbon-based ORR catalysts.

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JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY · 2016 · IF 2.857

Mass Spectrometric Analysis of N-Glycoforms of Soybean Allergenic Glycoproteins Separated by SDS-PAGE

Lingmei Li,Chengjian Wang,Shan Qiang,Jixiang Zhao,Shuang Song,Wanjun Jin,Bo Wang,Ying Zhang,Linjuan Huang,Zhongfu Wang

Glycosylation of many proteins has been revealed to be closely related with food allergies, and screening and structural analysis of related glycoproteins and glycoallergens are essential for studies in this field. Herein, we describe detailed N-glycoform analysis of all glycoprotein fractions of soybean protein isolate (SPI) separated by sodium dodecyl sulfate polyacrylamide gel electrophoresis (SDS-PAGE) to disclose structural features of the glycan moieties of more soybean glycoproteins. SPI was fractionated by SDS-PAGE, and the generated protein bands were recovered and subjected to in-gel N-glycan release and labeling using a one-pot method newly developed by our group, followed by detailed analysis by electrospray ionization mass spectrometry (ESI-MS) and online hydrophilic interaction liquid chromatography coupled with electrospray ionization tandem mass spectrometry (HILIC-ESI-MS/MS). As a result, we found seven bands mainly containing oligomannose-type glycans; two mainly contain core α1,3-fucosylated glycans, and six have no glycans. This study is the first report that discovers core α1,3-fucosylated N-glycans in bands 1, 2, and 6 and discloses bands 3, 4, 5, and 7 as glycoproteins and their N-glycoforms. Therefore, it can expand our knowledge about soybean protein glycosylation and provide significant structural reference for research of soybean allergens.

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