MICROCHIMICA ACTA
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2021
·Vol. 188
·期 1
·1-12
·
IF 5.833
Wang Qin,Shi Yupeng,Chen Wandi,Yang Mo,Yi Changqing
A novel dual-functional nanoprobe was designed and synthesized by facile assembly of quinoline derivative (PEIQ) and meso-tetra (4-carboxyphenyl) porphine (TCPP) via electrostatic interaction for simultaneous sensing of fluorescence of Zn 2+ and pH. Under the single-wavelength excitation at 400 nm, this nanoprobe not only exhibits “OFF-ON” green fluorescence at 512 nm by specific PEIQ-Zn 2+ chelation, but also presents red fluorescence enhancement at 654 nm by H + -triggered TCPP release. The nanoprobe demonstrated excellent sensing performance with a good linear range (Zn 2+ , 1–40 μM; pH, 5.0–8.0), low detection limit (Zn 2+ , 0.88 μM), and simultaneous response towards Zn 2+ and pH in pure aqueous solution within 2 min. More importantly, this dual-functional nanoprobe demonstrates the capability of discerning cancerous cells from normal cells, as evidenced by the fact that cancerous HepG2 cells in tumor microenvironment exhibit substantially higher red fluorescence and significantly lower green fluorescence than normal HL-7702 cells. The simultaneous, real-time fluorescence imaging of multiple analytes in a living system could be significant for cell analysis and tracking, cancer diagnosis, and even fluorescence-guided surgery of tumors. Graphical abstract
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RSC Advances
·
2020
·Vol. 10
·期 69
·42423-42431
·
IF 3.119
Ruidong Luo,Jinfeng Dong,Yunbai Luo
We first synthesized a diblock copolymer poly[tert-butyl methacrylate]-b-poly[3-(trimethoxysilyl)propyl methacrylate] (PtBMA-b-PTMSPMA) through reversible addition–fragmentation chain transfer (RAFT) living radical polymerization and grafted it onto fumed silica by converting the PTMSPMA segment to silanol and the PtBMA segment to polymethylacrylic acid (PMAA) in the presence of trifluoroacetic acid in order to obtain PMAA brush-coated silica nanoaggregates P-Si. TEM, DLS, FTIR, and TGA results confirmed the successful modification of the starting materials. The nanoaggregates flocculated and stabilized a toluene-in-water Pickering emulsion at low pH, while the nanoaggregates were well dispersed in water and broke the emulsion under both neutral and basic conditions. Alternatively, the addition of acid/base induced emulsification/demulsification cycles that were sustained for several cycles. Moreover, when the P-Si was mixed with Rh-loaded silica, Rh-Si, the mixture had the same pH-responsive Pickering emulsion behavior as the single P-Si. This Pickering emulsion system can be used in the biphasic interfacial catalytic hydrogenation of olefins and had excellent yields under a hydrogen atmosphere. The yield of Pickering emulsion catalysis rapidly reached more than 99% in 3 h, while that of the demulsified mixture failed to reach 20% in 4 h, which verified the promotion of catalysis by the Pickering emulsion. Base-induced demulsification can be used to separate the products and recycle the catalyst. This pH-responsive Pickering emulsion catalytic system was capable of several cycles of reuse, and there was no significant decrease in catalytic efficiency even after eight cycles.
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RSC Advances
·
2020
·Vol. 10
·期 56
·33635-33641
·
IF 3.119
Meihua Lin,Xin Ma,Shijun Lin,Xiaojin Zhang,Yu Dai,Fan Xia
Carbon dots (CDs) as fluorescent probes have been widely exploited to detect biomarkers, however, tedious surface modification of CDs is generally required to achieve a relatively good detection ability. Here, we synthesized N-doped carbon dots (N-CDs) from triethylenetetramine (TETA) and m-phenylenediamine (m-PD) using a one-step hydrothermal method. When the pH increases from 3 to 11, the fluorescence intensity of the N-CDs gradually decreases. Furthermore, it displays a linear response to the physiological pH range of 5–8. Au3+ is reduced by amino groups on the surface of N-CDs to generate gold nanoparticles (AuNPs), causing fluorescence quenching of the N-CDs. If glutathione (GSH) is then added, the fluorescence of the N-CDs is recovered. The fluorescence intensity of the N-CDs is linearly correlated with the GSH concentration in the range of 50–400 μM with a limit of detection (LOD) of 7.83 μM. The fluorescence probe was used to distinguish cancer cells from normal cells using pH and to evaluate intracellular GSH. This work expands the application of CDs in multicomponent detection and provides a facile fluorescent probe for the detection of intracellular pH and GSH.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2020
·
IF 16.683
Sijin Zuo,Xuming Jin,Xinwei Wang,Yunhao Lu,Qi Zhu,Jiangwei Wang,Weiping Liu,Yonghua Du,Juan Wang
ABSTRACT Atomically dispersed heterogeneous metal catalysts are promising in dealing with the ever-growing environment and energy issues. However, the practical uses of such catalysts are challenged by the concerns of low reliability and reusability of current compositions under changeable conditions. Here we demonstrate a strategy to stabilize the atomically dispersed Fe catalysts through anchoring the Fe atoms in between a C 3 N 4 -rGO double-layered support. The layered structure is found to significantly prohibit acid leaching and agglomeration of Fe atoms while maintaining activity of the reaction sites, even under extreme pH conditions (pH < 3 or> 11). This allows us to realize high performance Fenton-like reaction via activation of persulfate with unforeseen reactive and recycling abilities over all pH values (0 to 14). This work offers opportunities for understanding the Fenton-like system at extreme reaction conditions, while providing keen insights into the development of stable atomic metal catalysts for practical use.
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AAPS PHARMSCITECH
·
2020
·Vol. 21
·期 7
·1-11
·
IF 2.401
Ma Qun,Luo Rui,Zhang Huimin,Dai Manman,Bai Luyu,Fei Qingsong,Lei Fang,He Ning
We developed a pH-triggered in situ gel (ISG) for ocular delivery of vinpocetine to achieve systemic absorption and a brain-targeting effect in rats. Carbopol acted as a gelling agent combined with hydroxypropyl methylcellulose (HPMC) as a viscosity-enhancing agent. The concentration of Carbopol (0.2%, w/v) and HPMC (1.5%, w/v) was optimized for the ISG system. The optimized formulation was evaluated for studies on release in vitro , rheology, differential scanning calorimetry, ocular irritation, residence time, and in vivo pharmacokinetics. The vinpocetine ISG stayed longer in rabbit eyes than vinpocetine ointment. In vivo pharmacokinetics showed that compared with vinpocetine ointment, vinpocetine ISG attained a peak plasma concentration and area under the curve that was 1–2 folds greater in rat plasma. The Drug Targeting Index (DTI) was 1.06 and 1.26 for vinpocetine ointment and vinpocetine ISG, respectively, after ocular administration, showing that vinpocetine ISG had better distribution in rat brain. These results revealed that a pH-triggered ISG system via ocular administration could be an alternative approach compared with traditional ophthalmic formulations.
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JOURNAL OF MOLECULAR LIQUIDS
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2020
·
IF 5.065
Xinyu Zheng,Huaili Zheng,Rui Zhao,Zikang Xiong,Yili Wang,Yongjun Sun,Wei Ding
In order to deal with the increasingly serious water pollution caused by dye wastewater, a novel sulfonic acid-modified polyacrylamide magnetic composite (Fe 3 O 4 @SiO 2 /P(AM-AMPS)) was facilely prepared by crosslink reaction. The physicochemical properties and adsorption performances of Fe 3 O 4 @SiO 2 /P(AM-AMPS) were systematically studied by different characterization techniques and a series of batch experiments, respectively. It was found that the adsorption capacities of Fe 3 O 4 @SiO 2 /P(AM-AMPS) towards cationic dyes crystal violet (CV) and methylene blue (MB) were largely enhanced than those of silica-coated Fe 3 O 4 (Fe 3 O 4 @SiO 2 ) and maintained at relatively high levels in a wide pH range, due to the three-dimensional network structure and abundant functional groups of modified polyacrylamide. Besides, owing to the introduction of Fe 3 O 4 @SiO 2 , Fe 3 O 4 @SiO 2 /P(AM-AMPS) presented a unique magnetic property that helped it to be rapidly separated from water in a magnetic field. The maximum adsorption capacities of Fe 3 O 4 @SiO 2 /P(AM-AMPS) were 2106.37 mg g −1 for CV removal and 1462.34 mg g −1 for MB removal at 298.15 K, much higher than those of other reported magnetic composites. Furthermore, Fe 3 O 4 @SiO 2 /P(AM-AMPS) was effectively regenerated with HCl solution and the regeneration rates were higher than 97% and 80% for CV and MB removal after five adsorption-desorption cycles, respectively. With its excellent adsorption capacity, wide pH applicability, high separation speed, and satisfactory regeneration ability, Fe 3 O 4 @SiO 2 /P(AM-AMPS) was expected to become a promising adsorbent in the purification of cationic dye wastewater.
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CHEMICAL ENGINEERING SCIENCE
·
2020
·
IF 3.871
Wei Zhu,Wenquan Huang,Liping Ye,Yuehua Deng,Qiuling Xie,Yanbin Jiang
Zein nanoparticles have good prospects as a pharmaceutical carrier but limited in further application by its poor stability and re-dispersibility. To obtain high stability and pH-responsive drug delivery, succinylated-zein (Suc-zein) was synthesized by nucleophilic substitution reaction, the material obtained was used to prepare Suc-zein nanoparticles (SZs). The SZs prepared not only had good dispersibility but showed better stability than zein particles on pH, storage and salinity. After loading indomethacin (Indo) into zeolitic imidazolate framework-8 (ZIF-8), the core-shelled Indo-Suc-zein-ZIF-8 (Indo-SZZs) were fabricated by coating Suc-zein onto the surface of ZIF-8 with better stability and high drug loading. Indo-SZZs were pH-responsive and sustained a drug release profile in a simulated environment. Also SZZs presented as being non-toxic, having good biocompatibility and good cellular up-take performance, and the cytotoxicity of Indo-SZZs was significantly higher than that of Indo. This provides a new insight into the preparation of a zein-based oral drug delivery system.
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Nanoscale
·
2020
·Vol. 12
·期 24
·13010-13016
·
IF 6.895
Qiaoling Liu,Xiuyun Niu,Yan Zhang,Ying Zhao,Kaixin Xie,Boru Yang,Qing He,Shiyou Lv,Lin Li
The abnormal concentrations of both biothiols and pH in lysosomes are seriously related to many major diseases, such as Parkinson's and Alzheimer's diseases. Up to now, there are few reports that clearly illustrate the relationship between lysosomal pH and biothiols via fluorescence assay. Herein, novel carbon dots (Scy-CDs) are prepared with good water dispersibility and excellent photostability, and a large Stokes shift of 106 nm is exhibited under an excitation wavelength of 450 nm. The remarkable pH-dependent behavior of Scy-CDs is presented with the fluorescence quenching based on the donor-excited photoinduced electron transfer (d-PET) process. The pKa value is 5.30, which is in good agreement with the range of the normal and abnormal lysosomal pH. Upon the addition of cysteine (Cys) or homocysteine (Hcy), the d-PET process is effectively inhibited with fluorescence recovery totally. The significant co-localization of Scy-CDs with Lyso-Tracker Deep Red in HEp-2 cells and the Pearson correlation coefficient 0.88 strongly suggest that the Scy-CDs can target lysosomal pH and Cys/Hcy in living cells.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2020
·
IF 7.489
Lei Tang,Gang Wang,Zhixiang Zeng,Luli Shen,Lijing Zhu,Yingxin Zhang,Qunji Xue
With the development of research on superwettability materials, superhydrophobic and superoleophilic materials show superior separation ability in oil-water separation due to their excellent oil-water selectivity. However, due to the super wetting ability of the oil to the material, it is difficult to clean and reuse after adsorbing the oil spill. Therefore, how to realize the complete regeneration of superhydrophobic and superoleophilic materials is still a worldwide problem. In this paper, the controlled adsorption-desorption process of oil and the complete regeneration of materials are realized by pH induced superwettability transformation. We fabricate a pH-responsive oil-water separation sponge by a method of simply impregnating the carboxyl and alkyl group modified SiO 2 nanoparticles on the surface of melamine sponge (MS) skeleton, which can change the wettability from superhydrophobicity and superhydrophilicity through protonation and deprotonation in different pH solutions. The experiment results indicate that the sponge is superhydrophobic and superoleophilic in acid and neutral solution, and can adsorb oil in water. While in basic solution, it becomes superhydrophilic and underwater superoleophobic, which can release the adsorbed oil. With the help of a vacuum pump, we can use this wettability transition to achieve a continuous oil adsorption and desorption process. These findings offer a new preparation method of regenerative 3D adsorption materials like MS in oil-water separation.
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ACS Biomaterials Science & Engineering
·
2020
·
IF 4.152
Zhongyin Chen,Lihui Wan,Ye Yuan,Ying Kuang,Xiangyu Xu,Tao Liao,Jia Liu,Zi-Qiang Xu,Bingbing Jiang,Cao Li
The purpose of developing novel anticancer drug delivery systems (DDSs) is to efficiently carry and release drugs into cancer cells and minimize side effects. In this work, based on hollow mesoporous silica nanoparticle (HMSN) and the charge-reversal property, a pH/GSH-dual-sensitive DDS named DOX@HMSN–SS-PLL(cit) was reported. HMSN encapsulated DOX with high efficacy and was then covered by the “gatekeeper” β-cyclodextrin (β-CD) through the glutathione (GSH)-sensitive disulfide bond. Thereafter, adamantine-blocked citraconic-anhydride-functionalized poly-l-lysine (PLL(cit)-Ad) was decorated on the surface of the particles via host–guest interaction. The negatively charged carriers were stable in the neutral environment in vivo and could be effectively transported to the tumor site. The surface charge of the nanoparticles could be reversed in the weakly acidic environment, which increased the cellular uptake ability of the carriers by the cancer cells. After cellular internalization, β-CD can be removed by breakage of the disulfide bond in the presence of a high concentration of GSH, leading to DOX release. The preparation process of the carriers was monitored. The charge-reversal capability and the controlled drug-release behavior of the carriers were also investigated. In vitro and in vivo experiments demonstrated the excellent cancer therapy effect with low side effects of the carriers. It is expected that dual-sensitive DOX@HMSN–SS-PLL(cit) could play an important role in cancer therapy.
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JOURNAL OF APPLIED POLYMER SCIENCE
·
2020
·Vol. 137
·期 41
·49250
·
IF 2.52
Ya Li,Cui Cheng,Xiaoran Gao,Siyuan Wang,Hanhui Ye,Xiao Han
Despite aminoglycosides (AGs) have superior antibacterial ability, all approved AGs by FDA are associated with adverse effects such as ototoxicity and nephrotoxicity. To solve these problems, AGs hydrogels based on dynamic covalent bond cross-linking were quickly prepared within 25 s by using AGs, aldehyde hyaluronic acid (A-HA), and adipic acid dihydrazide graft hyaluronic acid (HA-ADH) as materials. FT-IR, thermal analysis, and SEM results exhibited that A-HA/HA-ADH/AGs hydrogels were successfully synthesized with highly porous and interconnected network structure. The water absorption ratio of the hydrogels increased with the decreasing pH and temperature, indicating the hydrogels were pH- and temp-responsive. The pH-dependent degradation also demonstrated pH sensitivity of the hydrogels. Rheology and self-healing analysis assessment displayed that AGs hydrogels had good mechanical property, self-healing ability, and injectability. The hydrogels had no cytotoxicity to L929 cells and their hemolysis ratios were between 0.7% and 1.3%, which reached a nontoxic level. Most importantly, inhibition zones results demonstrated that the hydrogels had excellent and sustained antibacterial performance against Escherichia coli and Staphylococcus aureus . Therefore, A-HA/HA-ADH/AGs hydrogels are potential dressings for wound healing. Further plans including antibacterial and in vivo wound healing assays will be shown in the next work.
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ACS Applied Materials & Interfaces
·
2020
·
IF 8.758
Wei Li Peng,Ze Ping Zhang,Min Zhi Rong,Ming Qiu Zhang
A novel strategy for developing homogeneous reversibly interlocking polymer networks (RILNs) with enhanced mechanical properties and underwater self-healing ability is proposed. The RILNs are prepared by the topological reorganization of two preformed cross-linked polymers containing reversible catechol–Fe3+ coordinate bonds and imine bonds and exhibit enhanced mechanical properties, superior underwater self-healing effect within a wide pH range, and water-assisted recycling ability through synergetic action between the reversible catechol–Fe3+ and imine bonds. At higher pH values, the catechol–Fe3+ coordinate bonds are responsible for self-healing, while the imine bonds maintain the stability of the materials. In neutral water, the imine bonds mainly account for self-healing, and hydrogen bonds and entanglements between the two networks prevent the material from collapsing. Under a lower pH value, intermolecular hydrogen bonds and entanglements contribute to self-healing. The outcomes of this work provide a new idea for developing robust multifunctional underwater self-healing materials.
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