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Polymers · 2019 ·Vol. 11 ·期 2 ·302 · IF 3.164

Regenerated Antheraea pernyi Silk Fibroin/Poly(N-isopropylacrylamide) Thermosensitive Composite Hydrogel with Improved Mechanical Strength

Boxiang Wang,Song Zhang,Yifan Wang,Bo Si,Dehong Cheng,Li Liu,Yanhua Lu

At present,Antheraea pernyisilk fibroin (ASF) has attracted research efforts to investigate it as a raw material for fabrication of biomedical devices because of its superior cytocompatibility. Nevertheless, native ASF is not easily processed into a hydrogel without any crosslinking agent, and a single hydrogel shows poor mechanical properties. In this paper, a series of ASF/poly (N-isopropylacrylamide) (PNIPAAm) composite hydrogels with different ASF contents were manufactured by a simple in situ polymerization method without any crosslinking agent. Meanwhile, the structures, morphologies and thermal properties of composite hydrogels were investigated by XRD, FTIR, SEM, DSC and TGA, respectively. The results indicate that the secondary structure of silk in the composite hydrogel can be controlled by changing the ASF content and the thermal stability of composite hydrogels is enhanced with an increase in crystalline structure. The composite hydrogels showed similar lower critical solution temperatures (LCST) at about 32 °C, which matched well with the LCST of PNIPAAm. Finally, the obtained thermosensitive composite hydrogels exhibited enhanced mechanical properties, which can be tuned by varying the content of ASF. This strategy to prepare an ASF-based responsive composite hydrogel with enhanced mechanical properties represents a valuable route for developing the fields of ASF, and, furthermore, their attractive applications can meet the needs of different biomaterial fields.Keywords:Antheraea pernyi;silk fibroin;hydrogel;thermosensitive;mechanical properties

CAS / MDL: 2210-25-5
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ACS Sustainable Chemistry & Engineering · 2019 · IF 6.97

One-Step Preparation of Zwitterionic-Rich Hydrophilic Hydrothermal Carbonaceous Materials for Enrichment of N-Glycopeptides

Xiaowei Li,Haiyang Zhang,Na Zhang,Shujuan Ma,Junjie Ou,Mingliang Ye

Two kinds of novel zwitterionic hydrophilic interaction liquid chromatography (ZIC-HILIC) materials decorated with phosphorylcholine or sulfobetaine type zwitterionic groups were facilely synthesized employing hydrothermal carbonization (HTC) reaction, in which sustainable carbohydrate (glucose) could be converted into functionalized carbonaceous materials with strong hydrophilicity using a one-step and environmentally mild process. The properties of obtained materials were characterized by helium ion microscopy (HIM), N2 adsorption/desorption measurement, static water contact angle measurement, elemental analysis, Fourier transform infrared spectroscopy (FT-IR), X-ray photoelectron spectroscopy (XPS), and ζ-potential. As a result, 26 N-glycopeptides with S/N above 20 could be detected from 150 fmol IgG digests after hydrophilic interaction chromatography (HILIC) enrichment by using as-synthesized material HTC-Glc-10%MPC. The limit of detection in matrix assisted laser desorption ionization-time of flight-mass spectrometry (MALDI-TOF MS) analysis was as low as 5 fmol and enrichment selectivity reached 100:1. Furthermore, 175 N-glycosylation sites in 285 N-glycopeptides from 92 glycoproteins were identified from 2 μL of human serum. This work provided a new, simple, and green way to synthesize an N-glycopeptide enrichment material for liquid chromatography–mass spectrometry/mass spectrometry (LC-MS/MS) analysis of glycoproteomes.

CAS / MDL: 50-99-7
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH · 2019 · IF 3.375

Strong Synergy between Ti3C2 and N-Doped Co Nanoparticles Boosts the Selective Hydrogenation of Propyne

Jianian Chen,Mingyu Chu,Fenglei Lyu,Jin Gong,Linzhong Wu,Lijia Liu,Yong Xu,Qiao Zhang

Two-dimensional (2D) metal carbides, carbonitrides, and nitrides (MXenes) have recently emerged as promising candidates in catalysis due to their unique properties. In this work, we composited Ti3C2 with Co-embedded N-doped carbon nanotubes (CNTs) via the pyrolysis of zeolitic imidazolate frameworks (ZIF-67) for propyne selective hydrogenation. Detailed characterizations show that strong synergistic effects are observed between the Ti3C2 and Co-embedded N-doped CNTs in the composite catalysts. This work provides an efficient strategy to achieve N-doping on Co nanoparticles, which play a vital role in the propyne selective hydrogenation. The optimized catalyst gives a high propyne conversion (∼99%) and high propene selectivity (∼96%) on propyne selective hydrogenation at 150 °C, which surpasses the reported non-noble metal catalysts in literature works. This work may not only open an avenue for obtaining active and selective catalysts for propyne selective hydrogenation but also promote research on the role of MXenes in catalysis.

CAS / MDL: 693-98-1
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RSC Advances · 2019 ·Vol. 9 ·期 58 ·33997-34003 · IF 3.049

Boosting the hydrogen evolution activity of a Co–N–C electrocatalyst by codoping with Al

Xiao Zhou,Haoran Yu,Yang Liu,Yong Kong,Yongxin Tao,Yong Qin

Co, Al and N tri-doped graphene (CANG) was successfully fabricated via annealing N-doped graphene with Co and Al precursors. The material was characterized by scaning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray diffraction (XRD), Raman spectroscopy, physical adsorption, and X-ray photoelectron spectroscopy (XPS). It was found that the as-prepared CANG features a robust three-dimensional hierarchically porous structure. The contents of Co and Al can achieve the maximum value of 2.18 at% and 0.51 at% at the annealing temperature of 950 °C. Upon using the electrocatalyst for the hydrogen evolution reaction (HER), the CANG exhibited remarkable electrocatalytic performance in both acidic (η10 = 105 mV) and alkaline media (η10 = 270 mV), and outperforms Co,N-codoped graphene and Al,N-codoped graphene, respectively. In combination with the density functional theory (DFT) calculations, it was revealed that the introduction of the Al heteroatom can decrease the absolute value of hydrogen adsorption free energy (ΔG(H*)) of Co–N–C catalysts, thus greatly enhancing the HER activity. This discovery will provide new guidance to the design of advanced and inexpensive carbon materials for fuel cell, water-splitting and other electrochemical devices.

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JOURNAL OF ELECTROANALYTICAL CHEMISTRY · 2019 · IF 3.218

New application of p-n junction in electrochemical detection: The detection of heavy metal ions

Jinghua Shang,Minggang Zhao,Huiyan Qu,Hui Li,Rongjie Gao,Shougang Chen

The 3D Ni/NiO/MoO 3 /chitosan foam was fabricated and the interfacial barrier of p-n junction was proposed as a driving factor for electrochemical detection of Cu 2+ . The electrochemical response resulted from the decreased barrier height caused by the absorbed Cu 2+ . The liner range (0–25 μM) and the lower detection limit (5.69 nM) were obtained. The direct electrochemical detection of Cu 2+ in real water sample with excellent stability and recovery was achieved. It affords a new approach to achieve the direct electrochemical detection of metal ions with depressed interference by employing the interfacial effects of p-n junction.

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ANALYTICA CHIMICA ACTA · 2019 · IF 5.256

Carbon dots as fluorescent nanoprobe for the determination of N-acetyl-β-d-glucosaminidase activity

Jimei Ma,Heng Zhang,Fangfang Peng,Xiaoqing Yang,Zi-Long Li,Linhao Sun,Hong Jiang

Carbon dots (CDs) were synthesized from p -aminophenol and ethylenediamine via one-step under mild condition and used as a sensitive fluorescent nanoprobe for the activity determination of N -acetyl-β- d -glucosaminidase (NAG). In this assay, p -nitrophenol was in situ produced from p -nitrophenyl-β-D- N -acetyl-glucosaminide, which was exclusively hydrolyzed by NAG. The UV absorption peak of p -nitrophenol (maximum at 400 nm) overlapped the excitation peak of CDs with maximum wavelength at 415 nm, which caused the fluorescence decline of CDs based on inner filter effect. The activity of NAG was determined by the fluorescence changes. The assay is highly sensitive to NAG with a low detection limit of 0.75 U L −1  (K = 3) and showed a good linear relationship in the range from 1 to 45 U L −1 . This CDs nanoprobe was successfully applied for the determination of NAG activity in human serum and urine samples.

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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2019 · IF 4.084

Non-noble-metal Ni nanoparticles modified N-doped g-C3N4 for efficient photocatalytic hydrogen evolution

Puhui Deng,Mengxiang Gan,Xue Zhang,Zhuzhu Li,Yu Hou

The use of non-noble-metal to replace precious metal as co-catalyst in solar-driven hydrogen evolution reaction (HER) is important for lowering hydrogen production cost. In this work, nickel metal nanoparticles loaded nitrogen-doped graphite carbon nitride (NiNCN3) was prepared, which significantly enhanced the HER activity of nitrogen-doped graphite carbon nitride. The hydrogen evolution rate of NiNCN3 can reach to 1507 μmol g −1  h −1 , much higher than that of 3 wt % Pt/NCN (1055 μmol g −1  h −1 ). The distinguished photocatalytic performance is due to the accelerated electron transfer efficiency and inhibited photogenerated electron-hole recombination. Our study offers an alternative method to achieve the low-cost and effective noble-metal-free photocatalyst for HER.

CAS / MDL: 102-71-6
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COMBUSTION AND FLAME · 2019 · IF 4.12

Probing the low-temperature chemistry of di-n-butyl ether: Detection of previously unobserved intermediates

Luc-Sy Tran,Julia Wullenkord,Yuyang Li,Olivier Herbinet,Meirong Zeng,Fei Qi,Katharina Kohse-Höinghaus,Frédérique Battin-Leclerc

Di- n -butyl ether (DBE, C 8 H 18 O) has been proposed as a promising biofuel for diesel engines , but details of its low-temperature (LT) oxidation chemistry are not well understood. This paper reports new speciation data obtained in the temperature range of 400–1100 K at ϕ=1 and nearly-atmospheric pressure, using a plug flow reactor combined with electron ionization molecular-beam mass spectrometry (MBMS) and two different jet-stirred reactors coupled with either online gas chromatography or tunable synchrotron vacuum ultraviolet photoionization-MBMS. The experimental results confirm that DBE is very reactive and exhibits two negative-temperature coefficient (NTC) zones around 500–550 K and 650–750 K. Speciation data with about 40 C 0 -C 8 species are presented, including about 20 LT species not reported previously. Among those, fuel-specific C 8 H 16 O 2 cyclic ethers were quantified. Also, butanoic acid , which is present in highest amounts among the detected LT intermediates, and C 8 H 14 O 3 diones, were found to peak already near 500 K, suggesting their importance in the LT chemistry of DBE. Signals of several highly oxygenated peroxides ( e.g. , C 8 H 14 O 5 and C 8 H 16 O 6 ) were detected, indicating third O 2 addition steps. Respective reaction pathways are suggested and discussed based on these experimental results. To better understand the LT chemistry of DBE, the present data were compared to two recent DBE models (Cai et al., 2014; Thion et al., 2017). Significant discrepancies between the experimental data and both models were found for important LT intermediates, of which many were not included in the respective mechanisms. The results reported in the present study thus provide new opportunities for refining DBE kinetic models .

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JOURNAL OF NANOSCIENCE AND NANOTECHNOLOGY · 2018 ·Vol. 18 ·期 6 ·4196-4203 · IF 1.354

High Quality Nitrogen and Silicon Co-Doped Carbon Dots (N/Si-CDs) for Fe3+ Sensing

Wu Jinzhu,Feng Yaxiu,Shao Yanbin,Sun Yanchun

Nitrogen and silicon co-doped carbon nanodots (N/Si-CDs) were synthesized by one-step hydrothermal carbonization of folic acid and 3-aminopropyl trimethoxy silane with the assistance of glycerol. The resultant N/Si-CDs present intense excitation-independent photoluminescence (PL) emission owing to their monodisperse sizes and specific surface states. In comparison to nitrogen single doped CDs (N-CDs), the co-doped N/Si-CDs possess better PL properties following different emission manner due to the synergistic effects of the nitrogen and silicon dopants. Besides, the functionalized surfaces of N/Si-CDs endow them with superior solubility and stability. The as-synthesized N/Si-CDs demonstrate selective and sensitive fluorescence response to Fe3+, which could be explained by the PL quenching effects of Fe3+ on N/Si-CDs. Based on this finding, the quantitative analysis of aqueous Fe3+ by N/Si-CDs was established, showing good linearity in a range of 10 nM~45 μM and good sensitivity with a detection limit of 3.8 nM, so did for the detection of Fe3+ in fetal bovine serum (FBS) spiked samples. Therefore, the N/Si-CDs as a novel fluorescence probe hold promising for monitoring environmental and clinical Fe3+.

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mAbs · 2018 · IF 5.165

N-terminal α-amino group modification of antibodies using a site-selective click chemistry method

De-zhi Li,Bing-nan Han,Rui Wei,Gui-yang Yao,Zhizhen Chen,Jie Liu,Terence C.W. Poon,Wu Su,Zhongyu Zhu,Dimiter S. Dimitrov,Qi Zhao

Site-specific conjugation of small molecules to antibody molecules is a promising strategy for generation of antibody-drug conjugates. In this report, we describe the successful synthesis of a novel bifunctional molecule, 6-(azidomethyl)-2-pyridinecarboxyaldehyde (6-AM-2-PCA), which was used for conjugation of small molecules to peptides and antibodies. We demonstrated that 6-AM-2-PCA selectively reacted with N-terminal amino groups of peptides and antibodies. In addition, the azide group of 6-AM-2-PCA enabled copper-free click chemistry coupling with dibenzocyclooctyne-containing reagents. Bifunctional 6-AM-2-PCA mediated site-specific conjugation without requiring genetic engineering of peptides or antibodies. A key advantage of 6-AM-2-PCA as a conjugation reagent is its ability to modify proteins in a single step under physiological conditions that are sufficiently moderate to retain protein function. Therefore, this new click chemistry-based method could be a useful complement to other conjugation methods.

CAS / MDL: 76-05-1
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ELECTROCHIMICA ACTA · 2018 · IF 5.116

Structural engineering of N/S co-doped carbon material as high-performance electrode for supercapacitors

Mingquan Liu,Silu Huo,Min Xu,Linlin Wu,Mingjie Liu,Yifei Xue,Yi-Ming Yan

Nitrogen and sulfur co-doped carbon (NSC) is considered as a promising electrode material for supercapacitors (SCs). However, the specific capacitance and the rate performance of NSC are not satisfied for practical applications due to its inappropriate structural properties. Herein, we report the structural engineering of NSC by optimizing pore structure to obtain an ordered hierarchical pore network. The as-prepared NSC possesses a high gravimetric capacitance of 322 F g -1  at the current density of 1.0 A g −1 and retains 206 F g −1 (64% of its capacitance at 1.0 A g −1 ) at the high current density of 100 A g −1 . Moreover, it reveals an excellent cycling performance with ∼93.4% capacitance retention after 10000 cycles at the current density of 20 A g −1 . An assembled symmetric supercapacitor (SC) shows a remarkable energy density of 11.4 Wh kg −1 and a high power density of 12.9 kW kg −1 . The outstanding performances of NSC electrodes benefit from the efficient ion diffusion and fast charge transfer. This work paves a way to rationally design and engineer the structure of NSC for achieving both high rate capability and high specific capacitance for SCs applications.

CAS / MDL: 638-16-4
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NEW JOURNAL OF CHEMISTRY · 2018 ·Vol. 42 ·期 14 ·11334-11340 · IF 3.201

One-dimensional controllable crosslinked polymers grafted with N-methyl-D-glucamine for effective boron adsorption

Jingjing Kang,Yakun Tang,Shasha Gao,Lang Liu

In this research, a series of one-dimensional controllable crosslinked polymers with the different mass ratios of 4-vinylbenzychloride (VBC) and divinyl benzene (DVB) was prepared via cationic polymerization, and the polymers were grafted with the functional group N-methyl-D-glucamine (NMDG) for boron removal. The optimum polymeric mass ratio and a series of boron adsorption performances were studied. The maximum adsorption capacity was 18.15 mg g−1, of which 94% was retained after 4 cycles. Meanwhile, different pH values had negligible effect on the boron adsorption capacity, which was favorable for the removal of boron from its aqueous solution in a wide pH window. In addition, a magnetic adsorbent was prepared by the combination of Fe3O4 nanoparticles and the polymer, which provided an effective way to collect and recover adsorbents from their aqueous solutions.

CAS / MDL: 109-63-7 1321-74-0
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