Water
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2022
·Vol. 14
·期 8
·1190
·
IF 3.53
Hao Li,Jin Wang,Yu Luo,Bo Bai,Fangli Cao
For improving the mechanical strength of controlled release fertilizer (CRF) hydrogels, a novel material ofChlorellawas employed as a bio-based filler to prepare chitosan–chlorella hydrogel beads with physical crosslink method. Here, the synthesis mechanism was investigated, and the chitosan–chlorella hydrogel beads exhibited enhanced mechanical stability under centrifugation and sonication than pure chitosan hydrogel beads.Chlorellabrought more abundant functional groups to original chitosan hydrogel, hence, chitosan–chlorella hydrogel beads represented greater sensitivity and controllable response to external factors including pH, salt solution, temperature. In distilled water, the hydrogel beads with 40 wt%Chlorellareached the largest water absorption ratio of 42.92 g/g. Moreover, the mechanism and kinetics process of swelling behavior of the chitosan–chlorella hydrogel beads were evaluated, and the loading and releasing of humic acid by the hydrogel beads as a carrier material were pH-dependent and adjustable, which exhibit the potential of chitosan–chlorella hydrogel beads in the field of controlled release carrier biomaterials.Keywords:hydrogel;controlled release;swelling;Chlorella;pH sensitivity
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ANALYTICAL CHEMISTRY
·
2022
·
IF 8.008
Lijuan Chen,Fan Chen,Gang Liu,Haoliang Lin,Yu Bao,Dongxue Han,Wei Wang,Yingming Ma,Baohua Zhang,Li Niu
Sweat pH is a critical indicator for evaluating human health. With the extensive attention on the wearable and flexible biosensing devices, the technology for the monitoring of human sweat can be realized. In this study, a sensitive, miniaturized, and flexible electrochemical sweat pH sensor was developed for the continuous and real-time monitoring of the hydrogen-ion concentration in human sweat. A flexible electrode was fabricated on the poly(ethylene terephthalate) (PET) substrate by a simple and low-cost screen-printing technology, which was based on the integration of fluoroalkyl silane-functionalized Ti3C2Tx (F–Ti3C2Tx) and the polyaniline (PANI) membrane technology instead of the traditional ion-sensitive membrane. The surface functionalization strategy for Ti3C2Tx with perfluorodecyltrichlorosilane can provide environmental stability. Functionalized Ti3C2Tx (F–Ti3C2Tx) was doped with PANI to obtain improved responsiveness, sensitivity, and reversibility. The constructed microsize, portable, and wearable F–Ti3C2Tx/PANI pH sensor aimed to real-time monitor the pH value of human sweat during exercise. On-body sweat pH monitoring for females and males, respectively, exhibited high accuracy and continuous stability compared with ex situ analyses. This study thus offers a facile and practical solution for developing a highly reliable MXene-based mini-type pH sensor to realize the online monitoring of human sweat pH.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2022
·
IF 11.357
Lin-Fang Li,Zhe Chen,Pai Liu,Yun-Hong Zhang
Accurately measuring the pH of atmospheric aerosols is a prerequisite for understanding the multiphase chemistry that profoundly affects the environment and climate systems. Despite the advancements of experimental techniques for in situ pH measurements in aerosols, current studies are limited to measuring the static pH of aerosol microdroplets with an unperturbed composition. This steady-state scenario, however, deviates from the real-world aerosols undergoing atmospheric aging reactions, specifically, those characterized with a spontaneous displacement of strong bases (or acids) with high volatility. Here, we introduce a continuous and in situ measurement of aerosol pH by using a 4-mercaptopyridine-functionalized silver nanoparticle probe and surface-enhanced Raman spectroscopy. We find that the ammonium depletion─a spontaneous displacement of ammonium by dicarboxylic acid salts─continuously acidifies aerosol water over time. The decaying trends of pH in the aerosols under various humidity conditions can be unified with a universal exponential function. Such an exponentially decaying function further indicates that the ammonium depletion reaction is a self-limiting process. Our technique can be applied to study the dynamic change of aerosol acidity during the complex atmospheric aging processes, toward elucidating their implications on atmospheric chloride, nitrate, and ammonium cycles.
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Marine Drugs
·
2022
·Vol. 20
·期 5
·278
·
IF 6.085
Yingqi Mi,Jingjing Zhang,Wenqiang Tan,Qin Miao,Qing Li,Zhanyong Guo
In this study, chitosan nanoparticles (HF-CD NPs) were synthesized by an ionic gelation method using negatively charged carboxymethyl-β-cyclodextrin and positively charged 2-hydroxypropyltrimethyl ammonium chloride chitosan bearing folic acid. The surface morphology of HF-CD NPs was spherical or oval, and they possessed relatively small particle size (192 ± 8 nm) and positive zeta potential (+20 ± 2 mV). Meanwhile, doxorubicin (Dox) was selected as model drug to investigate the prepared nanoparticles’ potential to serve as a drug delivery carrier. The drug loading efficiency of drug-loaded nanoparticles (HF-Dox-CD NPs) was 31.25%. In vitro release profiles showed that Dox release of nanoparticles represented a pH-sensitive sustained and controlled release characteristic. At the same time, the antioxidant activity of nanoparticles was measured, and chitosan nanoparticles possessed good antioxidant activity and could inhibit the lipid peroxidation inside the cell and avoid material infection. Notably, CCK-8 assay testified that the nanoparticles were safe drug carriers and significantly enhanced the antitumor activity of Dox. The nanoparticles possessed good antioxidant activity, pH-sensitive sustained controlled release, enhanced antitumor activity, and could be expected to serve as a drug carrier in future with broad application prospects.Keywords:chitosan nanoparticles;cyclodextrin;antioxidant activity;antitumor activity;drug release
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CHINESE JOURNAL OF ANALYTICAL CHEMISTRY
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2022
·
IF 1.193
Yan-Yan XING,Mei-Ling CHEN,Xin-Ai SHEN,Ning LIANG,Xiao-Hong HOU
In consideration of the promising application of peroxidase (POD)-like nanozymes in biomedical analysis, the development of POD mimics with good catalytic performance under neutral conditions remains significant. As a new catalyst, metal-organic frameworks have been explored as candidate nanozymes owing to their high catalytic activity, good stability, flexible and simple synthesis methods, diverse types, and properties. Herein, rod-like Fe-MIL-88A was successfully synthesized via a simple hydrothermal method. Fe-MIL-88A exhibited POD-like properties under neutral conditions and a stronger affinity for substrate 3,3 ' ,5,5 ' -tetramethylbenzidine and H 2 O 2 than natural horseradish POD. This result was primarily due to the additional exposed (100) facets of rod-like Fe-MIL-88A, which can catalyze the decomposition of H 2 O 2 to •OH more easily. Based on the POD-like properties of Fe-MIL-88A under neutral conditions, combined with glucose oxidase, a one-pot colorimetric analysis method for glucose detection was established. The proposed measurement had a linear range of 1–100 µM and a limit of detection of 0.45 µM. The colorimetric method was accurate, reliable, highly selective, convenient, and time-saving. Furthermore, the one-pot method was successfully applied to detect the concentration of glucose in human blood samples, and the measured results were consistent with those of commercial glucose meters, indicating that the proposed method can be a potential candidate for glucose detection.
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Applied Nanoscience
·
2022
·Vol. 12
·期 5
·1545-1556
·
IF 3.869
Yan Jia,Xie Shujie,Xia Qin,Li Xiang,Chen Shuhuai,Shen Jia
Combination cancer therapy may be facilitated using a nanoparticle-based drug delivery system. However, the therapeutic efficiency of cancer nanomedicines is reduced due to poor drug release into the cancer cells. To the treatment of liver malignancy, a PEGylated poly( α -lipoic acid) copolymer with mPEG- α PLA was constructed and exploited as a dual reduction/pH response nanocarrier to delivery of capsaicin (CAP) and doxorubicin (DOX). Due to their self-assembly in an aqueous solution, the mPEG- α PLA amphiphilic polymers could be effectively encapsulated on CAP and DOX to synthesize CAP and DOX co-loaded nanomaterials (CAP/DOX@NPs). After being prepared, the CAP/DOX@NPs released more CAP and DOX in response to reduction and acid stimuli than those left undamaged. According to the results of flow cytometry and confocal laser scanning microscopy, the HepG2 liver cancer cells rapidly absorbed the dual-drug-loaded nanoparticles and released drugs intracellularly. As a result, in HepG2 cells, CAP/DOX@NPs promoted increased cell death and had synergistic therapeutic effects. In biochemical models such as acridine orange and ethidium bromide (AO/EB and nuclear DAPI staining), results were demonstrating the nanoparticles effectively induce apoptosis in HepG2 liver cancer cells. Moreover, in vivo systemic toxicity outcomes shown that the CAP/DOX@NPs could be quickly excreted from the body with no apparent toxicity signs. Overall, these findings demonstrate that the suggested technique for treating liver cancer with a dual-response nanocarrier based on mPEG- α PLA copolymer is promising.
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POLYMERS FOR ADVANCED TECHNOLOGIES
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2022
·Vol. 33
·期 6
·1867-1880
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IF 3.348
Lin Quan,Jianfei Tie,Yamei Wang,Zhiping Mao,Linping Zhang,Yi Zhong,Xiaofeng Sui,Xueling Feng,Hong Xu
Conductive hydrogels with adhesion, toughness and self-healing properties have attracted more and more attention due to their wide application in wearable devices and health monitoring. However, integrating adhesion, toughness and self-healing properties into a hydrogel remains a serious challenge. Herein, we prepared an ionic conductive hydrogel using Fe 3+ ion, tert-butyl acetoacetate-modified polyvinyl alcohol (PVAA) and catechol-modified chitosan (CCS) based on mussel inspired catechol chemistry. The adhesion, toughness and self-healing properties of the hydrogel could be easily regulated. The prepared hydrogel had excellent adhesion properties (102 kPa), rapid self-healing properties (5 min at room temperature), pH responsiveness and toughness up to 1386 kJ/m 3 . Therefore, the hydrogel could be used as a wearable sensor to detect human movement, and it could also be used as a bioelectrode to collect electrocardiographic signal (ECG). It might not only show great potential in applications such as wearable devices and health monitoring, but also promote the development of next-generation adhesive hydrogel bioelectronic devices.
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Sustainable Energy & Fuels
·
2022
·Vol. 6
·期 4
·1084-1093
·
IF 6.813
Meilian Gao,Pingping Gao,Ting Lei,Chun Ouyang,Xiaobo Wu,Anru Wu
A novel porous iron phosphide (p-FeP) loading on nitrogen-doped carbon fiber/carbon paper (p-FeP/NCF/CP) as highly effective self-supporting catalysts for the hydrogen evolution reaction (HER) is synthesized by a three-step approach, including N-doped carbon fiber network preparation, porous FeOOH/NCF/CP precursor by selectively etching, and subsequent phosphorization process. The as-obtained p-FeP/NCF/CP composite exhibits a higher specific surface area and larger porosity in comparison to FeP/CP composite due to the rich porous structure and 3D network of the N-doped carbon fiber matrix (NCF). Electrochemical measurements demonstrate that p-FeP/NCF/CP composite exhibits an excellent electrocatalytic activity for HER with small overpotentials of 63 mV and 96 mV at 10 mA cm−2 current density in 0.5 M H2SO4 and 1.0 M KOH, respectively. The p-FeP/NCF/CP material also exhibits a small Tafel slope and charge transfer resistance as well as good stability and durability in pH 7 and pH 14.
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LANGMUIR
·
2023
·
IF 3.9
Na Li,Ximing Huang,Huibo Shao
Insights into the chemical essence of weak interactions on the surface of biomacromolecules may help to regulate biological processes. In this work, the pH sensitivity of ion-pair interactions occurring on a cysteine self-assembled monolayer (Cys SAM) that simulates the local surface of a protein was probed by scanning electrochemical microscopy (SECM). Cys SAM and the ion-pair interactions subsequently formed with the introduced aspartic acid (Asp) were both pH-sensitive, as confirmed by the tip current changes in the feedback mode. After continuous pH measurements, the most significant negative feedback was observed at pH 5.50, indicating the most robust ion-pair interactions, which were simultaneously identified by voltammetry. In this case, the extra addition of the inorganic cation (i.e., Ca2+) did not disrupt the existing ion-pair interactions, and the binding constant (K) and Gibbs free energy (ΔGo) of the ion pair were finally determined to be 6.44 × 105 M–1 and −33.14 kJ mol–1, respectively. Overall, the pH sensitivity of ion-pair interactions was found to be mainly attributable to pH-induced changes in the deprotonated/protonated states of the α-amino acid moieties, which may provide insights into the artificial manipulation of complex binding events at the molecular level on the biological surface.
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CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2021
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IF 3.171
Yueqing Wang,Hongxing Wang,Hongmei Chen,Hantao Liu
Converting polyethylene terephthalate (PET) wastes to its monomer and valuable chemicals via eco-friendly chemical method is still a challenge task. Previously, phase transfer catalysts used for alkaline hydrolysis were soluble in reaction media and hardly separated after reaction. Here, we reported several pH-responsive catalysts combined alkyl quaternary ammonium units with heteropolyacid anion for achieving stepwise product/catalyst separation and catalyst recycling. The properties of homogeneous/heterogeneous transfer behavior allow catalyst to be easily separated from reaction media by adjusting of pH value. Among them, [C 16 H 33 N(CH 3 ) 3 ] 3 PW 12 O 40 (abbreviated as [CTA] 3 PW) exhibits the highest activity and the most suitable pH responsive values. Such a pH triggered switchable catalytic system not only shows good performance for depolymerization of pure PET, but also some real PET wastes such as coloured trays and PE/PET complex films could be completely degraded into terephthalic acid. Additionally, the reaction kinetics and activation energy of PET alkaline hydrolysis also studied with and without pH-responsive [CTA] 3 PW.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2021
·
IF 5.316
Jinghua Li,Jianbo Zhang,Xibin Jiao,Jiahua Shi,Jiangxue Ye,Kena Song,Jianfeng Bao,Guangda Li,Kun Lei
In this work, near-infrared (NIR) light driven concave octopod PtCu alloy nanocages (OPtCu-NCs) were fabricated and first developed as photothermal synergetic Fenton catalyst for degradation of pollutant dyes. Moreover, by irradiating with NIR laser (808 nm), the obtained OPtCu-NCs exhibit excellent NIR absorption capacity and thus produce hyperpyrexia over 50 °C. Concomitantly, by the photothermal effect, the OPtCu-NCs nanocatalysts was used for elimination of organic dyes such as Methylene blue (MB) and Rhodamine B (RhB). The NIR-driven photothermal degradation mechanism under NIR irradiation can be attributed to the Fenton-like catalytic performance of Cu ions , then -N C- and/or C-C bonds in the molecular skeleton were fractured and electrons were donated intensively. As confirmed by a typical radical trapping experiment, electrons trigger the formation of miscellaneous reactive species (O 2 - , HO 2 , especially •OH) subsequently . Moreover, the photothermal Fenton-catalytic activity of the as-prepared OPtCu-NCs had maintained at 93.15% (for MB) and 91.87% (for RhB) after ten circulating degradation processes. All acquired results reveal that the OPtCu-NCs have the potential applied value in dyestuff-wastewater treatment under neutral pH.
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Journal of Environmental Chemical Engineering
·
2021
·
IF 5.909
Yue Gao,Fang Yang,Hongxian Jian,Kai Zhen,Peng Zhang,Xuejiao Tang,Zhen Fu,Wei Xu,Cuiping Wang,Hongwen Sun
To explore an effective liquid material for the degradation of polycyclic aromatic hydrocarbons (PAHs), sodium citrate (SC) was selected from four kinds of chelating agents for persulfate (PS) activation by transition metals to degrade pyrene in an aqueous system. PS activated by SC chelated ferrous ion (PS/Fe 2+ /SC) can catalyze pyrene degradation under neutral pH, and when the molar ratio of PS, SC, Fe 2+ and pyrene was 2000/2000/2000/1, the maximum degradation percentage reached 94.4% in 720 min through enhancing the PS consumption and oxidative capacity of the system. Furthermore, the pyrene degradation catalyzed by PS/Fe 2+ /SC was not influenced by pH in the range from 3.0 to 11.0, PS/Fe 2+ /SC system could effectively catalyze the pyrene degradation over a wide pH range. Additionally, the presence of 0.1 M of SO 4 2- and H 2 PO 4 - decreased the pyrene degradation using the PS/Fe 2+ /SC system, while 0.1 M of Cl - and NO 3 - had little effect on the pyrene degradation when PS/Fe 2+ /SC was used under neutral pH. Furthermore, pyrene degradation was attributed to the sulfate and hydroxyl radicals produced from PS/Fe 2+ /SC system, and these radicals were detected with strong signals of DMPO-SO 4 and DMPO-OH through electron paramagnetic resonance (EPR) spectroscopy. Finally, seven pyrene degradation products were identified by gas chromatography-mass spectrometer (GC-MS), and a possible pathway of pyrene degradation was proposed.
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