ANALYST
·
2023
·Vol. 148
·期 8
·1877-1886
·
IF 4.2
Jiahe Huang,Zhengjin Zhou,Chunhong Zhang,Chao Wang,Yanli Zhou,Lijia Liu,Junqing Li,Toshifumi Satoh,Yoshio Okamoto
A novel one-handed helical copoly(phenylacetylene) (CPA) bearing L-proline tripeptide pendants and a few triethoxysilyl residues was synthesized and hybridized into SiO2 porous microspheres (PMSs) during microsphere growth through the hydrolytic polycondensation of ethoxysilyl groups. Nuclear magnetic resonance and Fourier transform infrared spectroscopy results verified the successful preparation of CPA and its hybrid product using SiO2 PMSs. The chiral recognition ability of the resulting CPA with a hybridized-type chiral stationary phase (HCSP) for high-performance liquid chromatography (HPLC) was investigated, revealing its high recognition ability for selected racemates. Moreover, the HCSP showed good solvent tolerability, thus broadening the selection of suitable eluents. The separation effect of the HCSP for the racemate N,N-diphenylcyclohexane-1,2-dicarboxamide (7) improved significantly after introducing CHCl3 in the eluent, resulting in separation factors equivalent or superior to common commercially available polysaccharide-based chiral stationary phases. The proposed preparation strategy provides a new and valuable method for obtaining poly(phenylacetylene)-based HCSPs suitable for a wide range of applications and eluent conditions.
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JOURNAL OF MEMBRANE SCIENCE
·
2022
·
IF 10.53
Yunji Xie,Su Li,Jinhui Pang,Zhenhua Jiang
The piperidinium cation exhibited a substantial impact on the improvement of alkaline stability of anion exchange membranes (AEMs), yet the research regarding the micro-block polymer AEMs modified with it has not been conducted. Herein, we report two series of micro-block poly(arylene ether sulfone)s containing densely benzyl- N -methylpiperidinium (TTP- n -PIPPES) and benzyl-trimethyl-ammonium (TTP- n -QAPES) functionalized units for AMEs, respectively, where the n represents the molar ratio of monomer containing tri-tetraphenyl to the employed bisphenol monomers. The content and arrangement of the two types of cations in both polymer backbones were the same. The hydrophilic phases of TTP- n -PIPPES membranes exhibited isolated island states, wrapped with coherent hydrophobic phases. While the TTP- n -QAPES membranes formed continuous hydrophilic channels but fragmented hydrophobic phases. The discrepancy in the microscopic morphology of membranes and the intrinsic nature of cations thus rendered two types of AEMs with different advantages in macroscopic properties. The TTP- n -PIPPES membranes performed better dimensional stability and alkaline stability (low temperature). In contrast, the preferable capabilities of TTP- n -QAPES membranes were water affinity, hydroxide conductivity, and alkaline stability (high temperature). For instance, the TTP-18.2-PIPPES membrane was 11.7%, 11.4%, and 27.4% lower than the TTP-18.2-QAPES membrane at 80 °C in terms of dimensional change, water uptake, and hydroxide conductivity, respectively.
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ELECTROCHIMICA ACTA
·
2019
·
IF 5.383
Xiaomei Ning,Xiaosong Zhou,Jin Luo,Lin Ma,Xuyao Xu,Liang Zhan
The effects of catalyst support and synthesis process on the interaction between Pt nanoparticles (NPs) and S-doped carbon nanotubes (SCNTs), and the resultant electro-oxidation catalytic performance of glycerol, formic acid and CO were systematically researched. Pt NPs on SCNTs had better electro-oxidation catalytic performances than that of Pt NPs on CNTs. The doped S in thiophene-like structure (C-S-C) activated the neighboring C atoms to interact with Pt NPs, improving the catalytic performance with stronger ability to remove poisonous intermediates. The formed C-S-C had a synergistic effect with the neighboring Pt-C, promoting the adsorption and activation of reactants. The improved metal-support interaction resulted in Pt with smaller nanoparticle size and more exposed active sites. In different synthesis process, Pt NPs were more likely to interact with activated C neighboring S in ethylene glycol reduction method. However, defects containing doped S preferred to interact with Pt NPs in impregnation method. The research results indicated that rationally regulating the surface properties of carbon support and choosing an appropriate catalyst synthesis strategy to intensify the required metal-support interaction can greatly improve the catalytic performance.
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BIOSENSORS & BIOELECTRONICS
·
2019
·
IF 9.518
Jia Li,Junlin He,Chengli Zhang,Jun Chen,Weiran Mao,Chao Yu
In this study, a dual-type responsive electrochemical biosensor was developed for the quantitative detection of α2,6-sialylated glycans (α2,6-sial-Gs), a potential biomarker of tumors. The gold nanorods (AuNRs), which exhibited great specific surface area, as well as good biocompatibility , was synthesized by the way of seed growth method. Furthermore, a biotin-streptavidin (biotin-SA) system was introduced to improve the immunoreaction efficiency. Accordingly, a label-free biosensor was fabricated based on AuNRs-SA for the quick detection of α2,6-sial-Gs by recording the signal of differential pulse voltammetry (DPV). Furthermore, to expand the ultrasensitive detection of α2,6-sial-Gs, a carboxylated single-walled carbon nanohorns/sulfur-doped platinum nanocluster (c-SWCNHs/S-PtNC) was synthesized for the first time as a novel signal label, which showed an excellent catalytic performance. The usage of c-SWCNHs/S-PtNC could significantly amplify the electrochemical signal recorded by the amperometric i-t curve. Herein, a sandwich type biosensor was constructed by combining the AuNRs-SA on the electrode and c-SWCNHs/S-PtNC (signal amplifier). The label-free biosensor possessed a linear range from 5 ng mL −1 to 5 μg mL −1 with a detection limit of 0.50 ng mL −1 , and the sandwich-type biosensor possessed a wide linear range from 1 fg mL −1 to 100 ng mL −1 with a detection limit of 0.69 fg mL −1 . Furthermore, the biosensor exhibited excellent recovery and stability, indicating its potential for use in actual samples.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2018
·
IF 3.779
Xiaolan Chen,Tian Wang,Wanzheng Lu,Tianxiang Cao,Mingzhe Xue,Bing Li,Cunman Zhang
A modified solution method was applied to synthesize cubic garnet solid-state electrolyte Li 7 La 3 Zr 2 O 12 (LLZO) and Li 6.45 Ca 0.05 La 2.95 Ta 0.6 Zr 1.4 O 12 (LCLTZO). The synergetic doping of Ca and Ta is found to induce the formation of cubic LCLZTO with high ionic conductivity of 4.03 × 10 −4 S cm −1 while LLZO without substitution exhibits tetragonal phase with low conductivity. A Li-S cell with sulfur cathode and as-prepared LCLTZO solid electrolyte “separator” was conducted to deliver large initial discharge capacity of 1090 mAh g −1 with high initial Coulombic efficiency up to 92%. Cell with LCLTZO also exhibited better cycling performance at 0.2 C and extremely high Coulombic efficiency (close to 100%) than the cell without solid electrolyte. Better rate performance was also achieved at lower rate (0.2 C, 0.5 C and 1 C) by cell with LCLTZO although it lost advantages at higher rate of 2 C and 5 C due to the limitation of ionic conductivity of LCLTZO. Energy dispersive X-ray spectroscopy (EDS) provided direct evidence that LCLTZO solid electrolyte greatly suppressed the shuttle effect generated by polysulfides . The electrochemical impedance spectroscopy was applied to discuss the difference between cells with and without LCLTZO during the discharge process. Charge transfer reaction referred to soluble polysulfides was found to be slower in cell with LCLTZO than that in cell without solid electrolyte.
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POLYMER
·
2018
·
IF 3.483
Yang Tang,Song-Qing Zhao,Na Liu,Zong-Quan Wu
Living polymerization of achiral phenyl isocyanide using a simply prepared chiral π-allylnickel complex as initiator was found to proceed in helix-sense-selective manner. The polymerization of achiral phenyl isocyanide, 4-isocyanobenzoyl-2-aminoisobutyric acid hexyl ester ( 1a ) produced optically active helical poly- 1a m (L or D) whose chirality totally come from the helical conformation without containing any other chiral atoms. The monomer-structural effect on the helix-sense-selectivity was examined and indicated the long alkyl group in the monomer is not essential for the helix-sense-selective polymerization. The effect of chiral phosphine ligand was also investigated. The success of the helix-sense-selective polymerizations indicated the high activity of π-allylnickel complexes. Finally, polymerization of 2,5-dibromo-3-hexylthiophene (3HT) and subsequent addition of 1a in the presence of chiral π-allylnickel complex as a single catalyst afforded P3HT m - b -poly- 1a n with nonhelical P3HT and helical poly(phenyl isocyanide) (PPI) segments, which may be used as unique chiral organic materials in the future.
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DYES AND PIGMENTS
·
2018
·
IF 3.767
Shenghong Yang,Wenjing Guo,Xiaohan Sun
A ratiometric fluorescence probe for robust and rapid Cu 2+ detection was established based on an electrostatic association complex of polyallylamine capped CdTe(S) quantum dots (CdTe(S)@PAI QDs) and a small molecule dye 5-oxo-3,5-dihydro-2H-thiazolo[3,2-a]pyridine-7-carboxylic acid (TPCA). Both of the components are easy to make. Strongly fluorescent CdTe(S)@PAI QDs could be simply prepared through a one-step UV irradiation while TPCA could be obtained directly through the hydrothermal method . The ratiometric probe was built through mixing of both components, neither organic solvent nor other harsh conditions is involved. The as-prepared probe shows dual-emission at 525 nm and 420 nm under excitation wavelength of 350 nm. The fluorescence ratio ( I 525nm /I 420nm ) remains constant with concentration changes of the complex up to ± 20% and a temperature variation from 20 to 50 °C, but shows significant change in the presence of Cu 2+ . The proposed probe exhibits excellent selectivity and sensitivity for Cu 2+ . The fluorescence ratio ( I 525nm /I 420nm ) show good linear relationship with the Cu 2+ concentration range from 0.05 to 1.6 μM and the limit of detection (S/N = 3) can reach 24 nM . Its applicability was demonstrated by detecting Cu 2+ ions in certified reference materials and real samples with recoveries in a range of 91.0–107.3%.
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Energy Technology
·
2018
·Vol. 7
·期 5
·1800757
·
IF 3.175
Shuolin Li,Hongmei Li,Shaowei Huang,Qian He,Linxi Hou
Tailoring cobalt phosphide electrocatalysts with a tunable phase and morphology is of great importance for the advancement of hydrogen evolution reaction (HER). The synthesis of phase- and morphology-modulated hollow cobalt phosphide nanoparticles coupled with N, P, S co-doped carbon (Co-P@NPS-C) polyhedrons through a facile three-step method is reported. Benefiting from the cooperation of structural features, heteroatoms doping, and catalytic components (Co x P, a mixture of CoP and Co 2 P), the hollow Co x P@NPS-C polyhedrons exhibit superior HER performance and long-term stability in 1.0 m KOH solution, with a low onset potential value (18 mV), an overpotential of 80 mV at 10 mA cm −2 , and a small Tafel slope of 57.6 mV dec −1 . In addition, the Co x P@NPS-C electrodes exhibit good electrochemical properties and stability in 0.5 m H 2 SO 4 solution. These results suggest a novel and promising coating approach with poly(cyclotriphosphazene- co -4,4′-sulfonyldiphenol (PZS) to fabricate other heterogeneous catalysts for various applications.
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Journal of Materials Chemistry A
·
2018
·Vol. 6
·期 23
·10856-10867
·
IF 9.931
Xiangzhong Ren,Moujie Huang,Shan Luo,Yongliang Li,Libo Deng,Hongwei Mi,Lingna Sun,Peixin Zhang
A novel free-standing and binder-free air electrode with excellent electrochemical performance was designed for highly reversible Li–O2 batteries. The 3D hierarchically N, S co-doped macro–mesoporous carbon (NSMmC) was deposited on carbon paper (CP) via a template method, and then uniformly decorated with PdNi nanoparticles. The macropores of the porous carbon can provide enough space to accommodate discharge products, while the interconnected pores and channels efficiently facilitate oxygen and electrolyte diffusion. The introduction of PdNi nanoparticles greatly reduce the charge transfer resistance, resulting in the improvement of electron mobility of the whole cathode. Compared with Pd–NSMmC/CP and NSMmC/CP cathodes, the PdNi–NSMmC/CP cathode shows considerable enhancement of Li–O2 battery performance. The ultrafine and evenly distributed PdNi nanoparticles can not only provide enough catalytic sites, but can also tailor the discharge products into a cage-like morphology, which provides enough channels for electron and lithium ion transport. Moreover, the smaller size of the cage-like Li2O2 makes it decompose more easily, resulting in lower charge overpotential. This study provides a promising strategy to design 3D structured air cathodes for Li–O2 batteries with high electrocatalytic performance.
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DALTON TRANSACTIONS
·
2018
·Vol. 47
·期 43
·15538-15544
·
IF 4.099
Ruijiao Chen,Xiaowen Wu,Zhi Su
A series of quaternary chalcogenides, Na3ZnMIIIQ4 (MIII = In, Ga; Q = S, Se), were successfully synthesized for the first time through a high temperature solid-state reaction method. All of them exhibit similar structures and crystallize in the I41/acd space group of the tetragonal system. In their structures, typical super-tetrahedron (T2-type) clusters composed of four vertex-sharing (Zn/MIII)S4 tetrahedra are discovered and these T2-clusters further link together to form interesting wavelike chains. Adjacent T2 clusters present a torsion angle of 24.6° with each other when viewed along the c-axis, which has rarely been found among all the reported T2-containing chalcogenides. Moreover, we have systematically investigated the connection modes of NaSn (n = 4–6) in all the known Na-contained quaternary sulfides, and the result shows that the connection modes (corner-, edge-, and face-sharing) of NaS6 ligands in the title sulfides are also rarely (only 3%) found. Besides, the optical properties including diffuse-reflection and Raman spectra are systematically characterized. Theoretical calculations based on the first principles theory were also used to analyze their structure–performance relationships.
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Acta Biomaterialia
·
2017
·
IF 6.319
Yanan Kang,Lu Lu,Jinshuai Lan,Yue Ding,Jing Yang,Yong Zhang,Yuan Zhao,Tong Zhang,Rodney J.Y. Ho
A novel redox-sensitive system for co-delivering hydrophobic drugs and hydrophilic siRNA or shRNA was developed by conjugating gambogic acid (GA) with poly(amido amine)s (PAAs) through amide bonds, which is called GA-conjugated PAAs (PAG). PAG can self-assemble into micelles as amphiphilic block copolymers , which exhibits an excellent loading ability for the co-delivery of docetaxel (DTX) and MMP-9 shRNA with adjustable dosing ratios. In addition, confocal microscopy , flow cytometry and in vitro transfection analyses demonstrated more efficient cellular internalization of DTX and MMP-9 shRNA after incubation with PAG/DTX- MMP-9 shRNA micelles (PAG/DTX-shRNA) than with free drugs. Unlike traditional amphiphilic copolymer micelles, GA conjugated in PAG possesses an intrinsic anticancer efficacy. The presence of disulfide bonds in PAAs enables rapid disassembly of PAG micelles in response to reducing agents, inducing the release of loaded drugs (DTX, GA and MMP-9 shRNA). In vitro cellular assays revealed that PAG/DTX-shRNA micelles inhibited MCF-7 cell proliferation more efficiently than the single drug or single drug-loaded micelles. In vivo biodistribution and anti-tumor effect studies using an MCF-7 breast cancer xenograft mouse model have indicated that PAG/DTX-shRNA micelles can enhance drug accumulation compared with the free drug, thereby sustaining the therapeutic effect on tumors. Additionally, PAG/DTX-shRNA micelles displayed a greater anti-tumor efficacy than Taxotere® and PAG-shRNA micelles. These results suggest that the redox-sensitive PAG platform is a promising co-delivery system for combining drugs and gene therapy for the treatment of cancer. Statement of Significance The PAG micelles were designed by conjugating gambogic acid (GA) with poly(amido amine)s (PAAs), which would serve dual purposes as both gene and drugs co-delivery carrier and an anti-tumor prodrug. Unlike traditional amphiphilic micelles, GA conjugated in PAG could exert its intrinsic efficacy and provide synergistic antiproliferative effects with docetaxel (DTX) on MCF-7 cells. Disulfide bonds in PAG enables a rapid disassembly of PAG micelles in response to reducing agents and to release all loaded drugs (DTX, GA and MMP-9 shRNA) at tumor sites. PAG/DTX-shRNA micelles displayed greater anti-tumor efficacy than that of Taxotere®, indicating the design concept for PAG works well. And the strategy for PAG could be used to develop a series of similar co-delivery systems through conjugations of other small-molecule drugs with PAAs, such as doxorubicin , methotrexate and other drugs with carboxy groups in their structure.
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ECOTOXICOLOGY AND ENVIRONMENTAL SAFETY
·
2024
·
IF 6.2
Jin-Yang Chen,Ying-Xin Weng,Yong-He Han,Rui-Hong Ye,Di-Hui Huang
Bisphenol A (BPA) and its substitute bisphenol S (BPS) are desirable materials widely used in manufacturing plastic products but can pose carcinogenic risks to humans. A new conductive iron-based metal-organic framework (Fe-HHTP)-modified pencil graphite electrode (PGE) for electrochemically sensing BPA and BPS was prepared and fully characterized by SEM, TEM, FT-IR, XRD, and XPS. Results showed that the optimal conditions for preparing Fe-HHTP/PGE were a pH of 6.5, a Fe-HHTP concentration of 2 mg·mL −1 , a deposition potential of 0 V, and a deposition time of 100 s. The Fe-HHTP/PGE prepared under such conditions harbored a significant electrocatalytic activity with a detection limit of 0.8 nM for BPA and 1.7 nM for BPS ( S / N = 3). Correspondingly, the electrochemical response current was linearly correlated to BPA and BPS, ranging from 0.01 to 100 μM. Fe-HHTP/PGE also obtained satisfactory recoveries by 93.8–102.1% and 96.0–101.3% for detecting BPA and BPS in plastic food packaging samples. Our work has provided a novel electrochemical tool to simultaneously detect BPA and BPS in food packaging samples and environmental matrixes.
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危险品化学品经营许可证（带存储）