PHYSICAL CHEMISTRY CHEMICAL PHYSICS
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2019
·Vol. 21
·期 44
·24572-24583
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IF 3.567
Jiying Liang,Wenting Wei,Huiqin Yao,Keren Shi,Hongyun Liu
In this work, poly(N,N′-dimethylaminoethylmethacrylate-co-N-isopropylacrylamide) copolymer films were polymerized on the surface of Au electrodes with a facile one-step method, and Au nanoclusters (AuNCs) and tetraphenylethene (TPE) were synchronously embedded in the films, designated as P(DMA-co-NIPA)/AuNCs/TPE. Ferrocene dicarboxylic acid (FDA), an electroactive probe in solution displayed inverse pH- and SO42−-sensitive on–off cyclic voltammetric (CV) behaviors at the film electrodes. The electrocatalytic oxidation of nicotinamide adenine dinucleotide (NADH) mediated by FDA in solution could substantially amplify the CV response difference between the on and off states. Moreover, the two fluorescence emission (FL) signals from the TPE constituent at 450 nm and AuNCs component at 660 nm in the films also demonstrated SO42−- and pH-sensitive behaviors. Based on the aforementioned results, a 4-input/9-output biomolecular logic circuit was constructed with pH, Na2SO4, FDA and NADH as the inputs, and the CV signals and the FL responses at 450 and 660 nm at different levels as the outputs. Additionally, some functional non-Boolean devices were elaborately designed on an identical platform, including a 1-to-2 decoder, a 2-to-1 encoder, a 1-to-2 demultiplexer and different types of keypad locks. This work combines copolymer films, bioelectrocatalysis, and fluorescence together so that more complicated biocomputing systems could be established. This work may pave a new way to develop advanced and sophisticated biocomputing logic circuits and functional devices in the future.
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JOURNAL OF CHROMATOGRAPHY A
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2019
·
IF 3.858
Mingxian Li,Congcong Gu,Lan Luo,Jie Zhou,Jing Liu,Feng Zheng
The selective and sensitive determination of potential genotoxic methanesulfonate impurities in drug substances is highly challenging. A new method is reported for testing of methyl methanesulfonate (MMS), ethyl methanesulfonate (EMS) and isopropyl methanesulfonate (IPMS) in active pharmaceutical ingredients (APIs). Headspace single drop microextraction (HS-SDME) with room-temperature ionic liquid (RTIL) as extractant was employed to preconcentrate analytes and eliminate the drug matrix simultaneously. In order to increase volatilities for HS extraction and to improve their reactivity of the further derivatization at the same time, sodium iodide (NaI) was added to the sample to derivatize methanesulfonates to the corresponding iodoalkanes. The iodoalkanes in the extract were derivatized with N , N -diethyldithiocarbamate (DDTC) after HS-SDME, followed by separation and detection with high-performance liquid chromatography with ultraviolet detection (HPLC-UV). Several important parameters, including reaction temperature, reaction time and concentration of NaI, sample volume, microdrop volume, stirring rate, salt addition, extraction time, concentration, reaction time and reaction temperature of DDTC were investigated. Under the optimal conditions, LODs and LOQs of all methanesulfonates were 15 ng mL −1 and 40 ng mL −1 , respectively. Linearity (correlation coefficient values r > 0.999) and precision (the relative standard deviations were 1.0–4.6%) of six repeated injections were obtained. The recoveries at three spiked concentration levels were all in the range of 86.2–107.5% with the relative standard deviations <3.5%. The method reported here avoids interference of drug substances efficiently and detects methanesulfonate impurities in high sensitivity by HPLC-UV in Imatinib Mesylate and Levofloxacin Mesylate.
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ACS Biomaterials Science & Engineering
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2019
·
IF 4.511
Yin-Jia Cheng,Si-Yong Qin,Yi-Han Ma,Xiao-Sui Chen,Ai-Qing Zhang,Xian-Zheng Zhang
A multifunctional nanoplatform based on mesoporous silica nanoparticles (MSNs) was developed for combinational tumor therapy. Doxorubicin (DOX) was chosen as an antitumor drug and loaded into mesopores of MSNs via physical absorption. Then, a tumor-targeted fusion peptide conjugated with 2,3-dimethylmaleic anhydride (DTCPP) and a therapeutic peptide conjugated with 2,3-dimethylmaleic anhydride (DTPP) were introduced to the surface of MSNs as super-pH-sensitive nanovalves through disulfide linkages. The BSA adsorption assay confirmed the charge-reversal property of MSN-ss-DTPP&DTCPP nanoparticles at slightly acidic condition (pH 6.8) and superior stability in physiological environment (pH 7.4). According to the drug release research, both glutathione (GSH) and acidic condition are required for the accelerated drug release from DOX@MSN-ss-DTPP&DTCPP nanoparticles. Moreover, in vitro studies demonstrated the significantly reinforced tumor cellular uptake efficiency and mitochondrial disruption ability of DOX@MSN-ss-DTPP&DTCPP nanoparticles in tumor environment, in which DOX@MSN-ss-DTPP&DTCPP nanoparticles exhibited the preferred cytotoxicity toward αvβ3-positive human cervical carcinoma (HeLa) cells. We believe that the multifunctional dual-stimuli-sensitive MSN could provide an effective strategy for combinational tumor therapy.
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JOURNAL OF APPLIED POLYMER SCIENCE
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2019
·Vol. 136
·期 25
·47683
·
IF 2.188
Bin Guo,Huimin Wang,Danan Lan,Xiaomin Pang,Yiming Li,Haiyan Liu,Hongyuan Yan,Ligai Bai
Three temperature-sensitive monolithic columns were prepared by atom transfer radical polymerization and oxidation–reduction method using the initiator systems of CCl 4 /FeCl 2 , BPO/DMA, and APS/TEMED, respectively. The three monoliths were characterized by scanning electron microscopy, nitrogen adsorption, and thermogravimetric analysis. The obtained monolithic columns were used as on-line solid phase extraction sorbent coupled with high-performance liquid chromatography for the enrichment of β-sitosterol. By comparing some influencing factors on the adsorption, the optimum temperature-sensitive monolithic column which was initiated by CCl 4 /FeCl 2 was selected for enrichment of β-sitosterol from plant oil. The maximum adsorption capacity of the monolith for β-sitosterol was 10.0031 mg/g. The limit of detection and limit of quantitation were 0.039 and 0.13 mg/mL, respectively. The recovery was in the range of 90.21–98.26%. The results showed that the monolith had better selectivity for β-sitosterol and could be used for enrichment of β-sitosterol in food samples. © 2019 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2019 , 136 , 47683.
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POLYMER
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2018
·
IF 3.483
Qijing Chen,Fei Han,Chao Lin,Xuejun Wen,Peng Zhao
The aim of this study is to synthesize well-defined bioreducible core crosslinked star (CCS) polymers via heterogeneous reversible addition-fragmentation transfer (RAFT) polymerization in aqueous ethanol solutions. To this end, water-soluble linear arm polymers, poly (poly (ethylene glycol) methyl ether methacrylate) (PPEGMA), poly (2-(dimethylamino)ethyl methacrylate) (PDMAEMA) and poly ( N , N -dimethylacrylamide) (PDMA), were prepared respectively. Next, heterogenous RAFT polymerization of the polymers with N , N ′-bis(acryloyl)cystamine (BAC) as a crosslinker was systemically investigated in an aqueous ethanol solvent. It was found that these bioreducible CCS polymers with crosslinked BAC core could be prepared successfully depending on polymerization parameters. The formation of PPEGMA-based CCS polymers was affected by water volume fraction ( V w ) of water-ethanol solution, reaction time, arm polymer concentration, and spacing monomer . Besides, at an optimal V w of 80% ( i . e . the molar concentration of water is 44.44 M) and arm polymer concentration of 10% (w/v), PPEGMA-based CCS polymers at >90% yield could be achieved within 1 h. By the same V w and reaction time, PDMAEMA- and PDMA-based CCS polymers could also be prepared with high yield (>75%). The mechanism underlying the formation of the CCS polymers was ascribed to enhanced driving force of polymerization-induced self-assembly at an optimal V w . These CCS polymers were degradable in thiol-containing dithiothreitol, suggesting their potential application for drug release in a reductive intracellular environment.
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FIBERS AND POLYMERS
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2018
·Vol. 19
·期 5
·977-986
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IF 1.353
Li Xiaolei,Chen Jun,Yang Chaofen
Highly selective polyether sulfone (PES) blend imprinted membranes for template p -hydroxybenzonic ( p -HB) were synthesized by phase inversion imprinting technique using polybenzimidazoles (PBI) as a functional polymer and nanosized Al 2 O 3 as the additives. The SEM analysis showed that cross-sectional morphology of membranes were strongly influenced by the content of nano-sized Al 2 O 3 . Compared with PES 1 -MIM, PES 2 -MIM and PES 4 -MIM, the PES 3 -MIM containing 2.0 wt.% nano-sized Al 2 O 3 exhibited higher membrane flux, kinetic equilibrium adsorption value, binding capacity and better selectivity for p -HB. The experimental data of adsorption kinetic were well fitted to the pseudo-secondorder kinetic model using multiple regression analysis. Static adsorption isotherm experiments exhibited that the PES 3 -MIM had the maximum adsorption capacity for p -HB. Moreover, selective experiment showed that the selectivity coefficients of PES 3 -MIM for p -HB relative to salicylic acid (SA) was 3.670, showing that PES 3 -MIM had excellent binding affinity and selectivity for separating p -HB form p -HB-contained aqueous solution.
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International Journal of Nanomedicine
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2018
·
IF 4.37
Yanqiu Zhang,Lianjun Peng,Jiahui Chu,Ming Zhang,Lizhu Sun,Bin Zhong,Qiyong Wu
Background Co-delivery all-trans-retinoic acid (ATRA) and paclitaxel (PTX) is an effective strategy for cancer therapy. However, in many previous reported ATRA conjugated co-delivery systems, the ATRA was released slower than PTX, and the total drug release of ATRA far lower than that of PTX.Purpose We designed and prepared a pH and redox dual responsive drug delivery system (DA-ss-NPs) co-delivery ATRA and PTX for cancer therapy. The surface charge of DA-ss-NPs could change from negative to positive under tumor slightly acidic microenvironment, and both drugs could be quickly released from DA-ss-NPs under intracellular high concentration of glutathione (GSH).Methods The DA-ss-NPs were constructed by encapsulating PTX into the hydrophobic core of the polymer micelles, in which the polymer was synthesized by conjugating ATRA and 2,3-Dimethylmalefic anhydride (DMA) on side chains of Cystamine dihydrochloride (Cys) modified PEG-b-PAsp (named DA-ss-NPs). The surface charge of DA-ss-NPs under different pH conditions were detected. And the drug release was also measured under different concentration of GSH. The therapeutic effect of DA-ss-NPs were investigated in Human lung cancer A549 cells and A549 tumor-bearing mice.Results The zeta potential of DA-ss-NPs was -16.3 mV at pH 7.4, and which changed to 16 mV at pH 6.5. Cell uptake experiment showed that more DA-ss-NPs were internalized by A549 cells at pH 6.5 than that at pH 7.4. In addition, in presence of 10 mM GSH at pH 7.4, about 75%-85% ATRA was released from DA-ss-NPs within 48 h; but less than 20% ATRA was released without GSH. In vivo antitumor efficiency showed that the DA-ss-NPs could affectively inhibite the tumor in compared with control groups.Conclusion The charge-reversal and GSH-responsive DA-ss-NPs provide an excellent platform for potential tumor therapy.
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ADVANCED FUNCTIONAL MATERIALS
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2018
·Vol. 28
·期 47
·1804609
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IF 13.325
Xinxin Dai,Kai Han,Zhaoyu Ma,Heyou Han
The precise recognition of tumor tissue is the key challenge that hinders successful clinical translation of drug delivery systems. Herein, a tumor extracellular matrix orthogonal stimuli-responsive chimeric peptide is developed for logic gate controlled tumor recognition and photodynamic therapy. In vitro studies show that the negatively charged chimeric peptide is sensitive to two typical tumor hallmarks, i.e., mild acidity and matrix metalloproteinase 2 (MMP-2) simultaneously. Consequently, the chimeric peptide can undergo charge reversal from negative charge to positive charge in tumor, accelerating the cellular uptake. Specifically, the enhanced cellular uptake of chimeric peptide can be activated efficiently only in the presence of both acidity and MMP-2, endowing chimeric peptide with highly specific tumor therapy both in vitro and in vivo. This chimeric peptide based “AND” logic gate should show great potential in precise tumor therapy.
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CELLULOSE
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2018
·Vol. 25
·期 3
·1705-1714
·
IF 3.809
Liu Ting,Ding Enyong,Xue Feng
Polymer grafting is an efficient way to obtain functional cellulose nanocrystals. In this work, we used a “macro-RAFT (macromolecular reversible addition–fragmentation chain transfer) agent-assisted” strategy, which adds extra amount of amphiphilic macro-RAFT agent with low molecular weight to graft poly(N,N-dimethylacrylamide) (PDMA) from cellulose nanocrystals. Successful grafting was evidenced by different characterization methods, and a high weight ratio of grafted PDMA was obtained (77.6%). The grafting process was studied through the weight ratio of grafted PDMA, monomer conversion, and the molecular weight of free and grafted PDMA at different reaction time. As a result, we have suggested that there were three types of grafted polymer chains on cellulose nanocrystals in this reaction system and discussed their evolution during the grafting reaction. Finally, we summarized several key factors for successful grafting in this macro-RAFT agent-assisted strategy.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2017
·
IF 3.671
Ting Liu,Enyong Ding,Feng Xue
Natural polymer flocculants for wastewater treatment have received close attention in recent years. Here we used two flocculants, polyacrylamide and poly( N , N -dimethylacrylamide) grafted cellulose nanocrystals synthesized by a “macro-RAFT assisted” strategy, for the flocculation of kaolin suspension. The flocculation performance of these two flocculants, including flocculants dosage, settling time and floc size, was carefully studied and compared. Results suggested that poly( N , N -dimethylacrylamide) grafted cellulose nanocrstyals showed better flocculation performance than polyacrylamide grafted ones. Meanwhile, their flocculation behavior was also compared with other cellulose-based flocculants in literature and we suggested polymer modified cellulose nanocrstals as flocculants might have higher flocculation performance, but this needs further verification.
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ECOTOXICOLOGY
·
2017
·Vol. 26
·期 2
·202-210
·
IF 1.951
Ding Tengda,Zhang Jianying,Ni Wanmin,Li Juying
The toxicity and bioavailability of single arsenic species have been widely investigated, however, the biological effects of mixed arsenic species co-existing in natural waters still remain unknown. The objective of this work was to discern the adverse effects of combined arsenite (As(III)) and dimethylarsenic acid (DMA) on diatom Nitzschia palea . The combined ecotoxicity of As(III) and DMA on N. palea was observed to be time-dependent and showed dose-effect relation. The toxicity of DMA and As(III) mixture was higher than individual DMA or As(III) when the As(III) concentration was in the range of 0.085–0.316 mg L −1 . As the As(III) concentration increased from 0.487 to 0.858 mg L −1 , the antagonistic effect was found, which could be due to the higher thiols contents in the thiol-containing proteins (e.g., frustulins, silaffins and other glycoproteins). The content of malondialdehyde (MDA) in the treatment of mixed arsenic species was found to be at the same level compared to the As-free control after 72 h of exposure, indicating that the co-toxicity of As(III) and DMA on diatom frustules was not significant. Furthermore, the increase of frustule formation rate in the mixture of EC 50 As(III)-EC 10 DMA at 72 h exposure time indicated that the damaged diatom cell walls was likely repaired gradually. The results from this study suggested that the effects of co-existed arsenic species were concentration-specific and should be considered in the risk assessment of arsenic and development of water quality criteria for the protection of aquatic ecosystems.
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MICROCHIMICA ACTA
·
2017
·Vol. 184
·期 4
·1185-1190
·
IF 4.58
Gong Lingling,Du Bibai,Pan Long,Liu Qingju,Yang Kunhao,Wang Wei,Zhao Hong,Wu Li,He Yujian
The authors describe a colorimetric assay for the determination of As(III) in aqueous solution using citrate capped gold nanoparticles (AuNPs) which, in the presence of As(III), undergo aggregation due to the interaction of citrate ion with As(III). This results in an easily detectable color change from wine-red to blue. The ratio of the absorbances at 661 and 519 nm is linearly related to the As(III) concentration in the 4 to 100 ppb range, with a detection limit as low as 1.8 ppb (at 3σ) which is below the guideline value of 10 ppb. The method is rather simple in that it does not require the surface of the AuNPs to be modified. It was successfully applied to the determination of As(III) in spiked drinking water where it gave adequate recoveries.
The ratio of the absorbances at 661 and 519 nm is linearly related to the As(III) concentration in the 4 to 100 ppb range, with a detection limit as low as 1.8 ppb (at 3σ) which is below the guideline value of 10 ppb.
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