LANGMUIR
·
2020
·
IF 3.557
Xiaojiang Li,Peiyao Zhu,Xin Lv,Guijiang Yan,Hongsheng Lu
In this work, a novel Pickering emulsion is stabilized by silica nanoparticles functioned with a redox and pH-responsive surfactant FA-DMDA-Ox that is prepared simply by direct neutralization of ferrocenecarboxylic acid (FA) and N,N-dimethyldodecylamine (DMDA) and exhibits redox and doubly pH-switchable behavior. Here, the Pickering emulsion can be stabilized easily by combining hydrophilic silica nanoparticles with less than 0.1 wt % FA-DMDA-Ox. After adding Na2SO3 and H2O2 alternately, the demulsification and emulsification of this Pickering emulsion are controlled reversibly. Moreover, the emulsion is switched “off” upon the addition of HCl and switched “on” upon the addition of NaOH and is also switched off upon the addition of NaOH and switched on upon the addition of HCl, which demonstrate the doubly pH-switchable behavior. Based on the analysis of ζ-potential, contact angle, and adsorbed amount of silica nanoparticles, the pH and redox-switchable mechanism of the Pickering emulsion are analyzed. Here, the redox-switchable behavior is induced by the reversible adsorption and desorption of FA-DMDA-Ox on the surface of silica nanoparticles. The pH-switchable behavior is driven by the controllable dispersion systems of silica nanoparticles and FA-DMDA-Ox because of the doubly pH switchability of FA-DMDA-Ox. More importantly, upon adding fresh oil after removing the original oil, the Pickering emulsion is recycled three times. Hence, the multiswitchable Pickering emulsion can be expected to be treated as a multifunctional material in practical applications, such as oil or wax removal in the petroleum industry.
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高影响因子
JOURNAL OF MATERIALS SCIENCE
·
2023
·Vol. 58
·期 46
·17711-17725
·
IF 4.5
Jia Tianshuo,Kuang Dajiang,Qi Zhenzhen,Tan Guohongfang,Yang Xiaojing,Kundu Subhas C.,Lu Shenzhou
Silk fibroin is a widely used biocompatible medical material with tunable mechanical, degradability and environmental non-toxicity. This paper prepared the silk fibroin/chitosan hydrogel microneedle with pH sensitivity by blending silk fibroin with chitosan to induce graft cross-linking. The cross-linked silk fibroin/chitosan microneedles network is expanded by hydrogen ions and water molecules, forming a more significant swelling. In vitro, the transdermal drug release showed that insulin loaded in microneedles exhibited pH-sensitive drug release behavior and was released faster under acidic conditions than under neutral conditions. By changing the pH of the solution, microneedles can achieve a stimulating response to the environment, thereby intelligently regulating the transdermal release of insulin.
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ACS Applied Bio Materials
·
2018
·
IF 0
Xiaojuan Wei,Jian Shen,Zheng Gu,Yazhi Zhu,Feng Chen,Mingqiang Zhong,Li Yin,Yao Xie,Zhenjie Liu,Wei Jin,Mehdi Nouri,Lingqian Chang
Polydimethylsiloxane (PDMS) is a common biomaterial with excellent properties. However, its inherent hydrophobicity impedes cell growth and differentiation. PDMS is an intrinsically inert material, which limits its applications to specific scenarios where responsive materials are needed. Dopamine can easily adhere to various substrate surfaces through noncovalent and covalent interactions. In this work, a bioinert PDMS surface was modified into a bioactive surface by biocompatible and pH-sensitive polydopamine (PDA). The binding of PDA and PDMS in different forms was verified by the typical scanning electron microscopy (SEM) and atomic force microscope (AFM). By PDA film modification, the contact angle of PDMS was significantly reduced. Hydrophobicity was achieved by PDA nanosphere (PDA NS) modification. PDA-modified PDMS was also found to be pH-sensitive, as validated by contact angle measurement, macroscopic friction test, and protein adsorption. Compared to an unmodified surface, the PDA significantly improved cell adhesion, proliferation and spreading. We came to a conclusion that the surface roughness of PDA-modified PDMS had little effect on cell growth and the cytocompatibility of the materials was mainly determined by the surface chemical properties. Our results further validated that PDA/PDMS is pH-sensitive and can effectively promote cell growth and proliferation.
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JOURNAL OF MATERIALS SCIENCE
·
2019
·Vol. 54
·期 13
·9983-9994
·
IF 3.442
Yang Meng,Wang Linlin,Cheng Yongbin,Ma Ke,Wei Xinran,Jia Pengxiang,Gong Yongkuan,Zhang Yang,Yang Jingfa,Zhao Jiang
A self-healing hydrogel was synthesized via the multi-component reaction of azobenzene-methacrylamide, β-CD and 3-methacrylamido phenylboronic acid. The orthogonal method was applied to analyze the influence of host–guest inclusion complexation, cross-linker and phenylboronic acid monomers content on mechanical properties and healing efficiency of the hydrogel. The results indicated that hydrogel showed autonomic self-healing behavior. The hydrogel demonstrated light-switchable self-healing ability and pH-sensitive swelling ratio. It was found that hydrogel showed high elongation, excellent resilience and low elastic hysteresis. The design of the combined host–guest interactions and boronate esters on the hydrogel showed advantage for improving the mechanical, self-healing and recovery properties simultaneously.
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CHEMISTRY-A EUROPEAN JOURNAL
·
2017
·Vol. 24
·期 1
·212-221
·
IF 5.317
Jun Song,Yanlong Wei,Jiwen Hu,Guojun Liu,Zhengzhu Huang,Shudong Lin,Feng Liu,Yangmiao Mo,Yuanyuan Tu,Ming Ou
Graphical Gated delivery : pH-Responsive porous nanocapsules have been prepared from ternary graft copolymers and used as potential vehicles for controlled release of drugs, food, and bioactive compounds (see figure). In this work pH-responsive porous nanocapsules have been successfully prepared from a ternary graft copolymer, poly(glycidyl methacrylate)- g -[poly(2-cinnamoyloxyethyl methacrylate)- r -poly(ethylene glycol) methyl ether- r -poly(2-diethylaminoethyl methacrylate)] or PGMA- g -(PCEMA- r -MPEG- r -PDEAEMA). The graft copolymers were fabricated by grafting three types of polymer chains onto the backbone polymer by using click chemistry. These ternary copolymers underwent self-assembly to form vesicles in a DMF/water solvent mixture. While the MPEG chains served as the corona and stabilized the vesicles, the vesicle wall was composed of a dominant PCEMA continuous phase that was interspersed by PDEAEMA domains. After photo-cross-linking, the PDEAEMA domains were embedded in the structurally locked PCEMA wall. By decreasing the pH of the external solution, we were able to trigger the release of encapsulated pyrene due to the capsule wall becoming porous as a result of the PDEAEMA chains bearing positively charged amine groups stretching into the water. While these pH-responsive porous nanocapsules exhibited potential applications in drug delivery, detection and catalysis, the strategy reported in this contribution also represented a new paradigm for the design and preparation of other novel stimuli-responsive porous nanocapsules.
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BIOMACROMOLECULES
·
2014
·
IF 5.788
Feng Liu,Shudong Lin,Zuoquan Zhang,Jiwen Hu,Guojun Liu,Yuanyuan Tu,Yang Yang,Hailiang Zou,Yangmiao Mo,Lei Miao
Three ternary graft copolymers bearing polystyrene (PS), poly(ethylene glycol) methyl ether (MPEG), and poly(acrylic acid) (PAA) side chains were synthesized and characterized. At pH = 7.4, these copolymers stabilized doxorubicin (DOX)-containing benzyl benzoate (BBZ) nanoemulsion droplets in water and formed a compact polymer layer to inhibit DOX release. Upon lowering the solution pH to 5.0, the AA groups dissociated less and became less soluble. Moreover, the neutralized AA groups formed presumably H-bonded complexes with the EG units, reducing the solubility of the EG units. This dual action drastically shifted the hydrophilic and hydrophobic balance of the copolymer and caused the original stabilizing polymer layer to rupture and the nanoemulsion droplets to aggregate, releasing DOX. The rate and extent of DOX release could be increased by matching the numbers of PAA and MPEG chains per graft copolymer. In addition, these nanoemulsions were not toxic and entered human carcinoma cells, releasing DOX there. Thus, these nanoemulsions have potential as drug delivery vehicles.
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
·
2026
·
IF 4.8
Huiping Wang,Zhaoyu Ma,Zhouxu Liu,Yaojie Zhang,Yumin Hao,Chenxing Li,Zhanpeng Tao,Shaomin Shuang,Chuan Dong,Xiaojuan Gong
Fluorescent sensors are pivotal in environmental and bioanalysis owing to their high sensitivity and rapid response. Among them, carbon dots (Cdots) stand out as ideal platforms for multifunctional sensing. Their tunable fluorescence and excellent biocompatibility facilitate the integration of multiple detection modalities, enabling versatile analyte detection. This capability can be further enhanced through heteroatom doping. Notably, boron doping introduces defect sites and active functional groups, providing a powerful strategy for developing advanced sensors suited for challenging applications in complex media. In this work, boron-doped yellow fluorescent carbon dots (BCdots) were synthesized via a green, facile approach to construct a dual-mode fluorescence/colorimetric sensing system for pH and vitamin B12 (VB12) detection. The fluorescence-based pH sensing operates on a protonation-induced enhancement mechanism, enabling ultrasensitive dynamic monitoring within a linear range of pH 2.5–6.0. For VB12 sensing, fluorescence quenching occurs via an inner filter effect (IFE) between VB12 and BCdots, yielding a wide linear range of 0.47–359.12 μM and a low detection limit of 80.15 nM. The colorimetric mode also displayed excellent sensitivity, with a linear range of 0.70–219.64 μM and a detection limit of 0.12 μM. Real sample analyses validated accuracy and reproducibility of the dual-mode fluorescence/colorimetric sensing platform, achieving recoveries of 95.74%–108.85% and RSDs below 3.33%. This study presents a carbon-based dual-mode sensor for the simultaneous detection of pH and vitamin B12, leveraging a synergistic integration of fluorescence and colorimetric detection. The developed platform demonstrates high precision, strong selectivity, and reliable performance in complex sample matrices. This work provides a crucial methodology for advancing multifunctional sensing tools in environmental monitoring and biomedical diagnostics.
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FOOD CHEMISTRY
·
2022
·
IF 9.231
Haihua Jiang,Junhui Pan,Xing Hu,Miao Zhu,Deming Gong,Guowen Zhang
Glutenin has limited applicability in food industry due to poor water solubility and emulsifying properties. In this study, the physicochemical properties of glutenin were improved by combined treatments of alkaline pH-shifting or acidic pH with heating. The surface morphology, structure and physicochemical properties were measured during the modification process of glutenin. Results showed that the smaller square clusters and regular tubular fibrils were observed in modified glutenin and the α-helix proportion of the treated glutenin was finally increased to 59.90 ± 0.01%. Compared with untreated glutenin, the combined treatments of pH-shifting with heating as well as fibrillation process increased the solubility of glutenin by 21.3 and 3.5 times, respectively. Moreover, the treated glutenin showed excellent emulsifying stability (EAI: 50.84 ± 0.51 m 2 g −1 ) and thermal stability (peak temperature increased from 109.58 to 149.05 °C). This study provides an informative basis for improving the physicochemical and functional properties of glutenin.
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Food Structure-Netherlands
·
2025
·
IF 5.9
Xin Qi,Yulin Li,Jinzhou Xiao,Liting Shen,Zhonghua He,Jianhua Xie
This study aimed to investigate the effects of pH-shifting on the aggregation behavior of pea protein isolate (PPI) and gellan gum (GG), as well as the gel properties and formation mechanism of PPI-GG composite gels. With the pH shifted from 3 to 11, the solubility of PPI decreased at first and then increased, reaching minimum value at pH 5 . PPI-GG allowed for the fastest sol-gel transition at pH 5. In this case, PPI-GG composite gel exhibited the highest dynamic modulus, gel strength (189.00 ± 24.06 g), hardness (631.92 ± 95.14 g), water holding capacity (94.3 ± 3.2 %), and thermal stability. However, steady shear tests revealed structural instability under high shear rates. In contrast, PPI-GG composite gel formed at pH 7 exhibited higher yield stress and lower tan δ, indicating its more stable and homogeneous network structure. Fourier transform infrared spectroscopy revealed that the β-sheet content reached its maximum at pH 5 and progressively decreased as the pH moved away from the isoelectric point. Measurements of sulfhydryl groups and intermolecular interactions indicated that disulfide bonds contributed to gel formation at both pH 5 and pH 7, with a more pronounced effect observed at pH 5. This study provides the first comprehensive analysis of pH-mediated transitions in the physicochemical, structural, and gel properties of PPI–GG composite gels, elucidating the underlying gelation mechanisms across different pH levels and contributing to the rational design and development of gel-based foods with tailored functionalities.
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Soft Matter
·
2022
·Vol. 18
·期 16
·3157-3167
·
IF 4.046
Zhouxuan Xiang,Ting Liu,Huimin Wang,Genxin Chen,Xiongbin Zhu,Tonghui Hao,Jiabing Ran,Changying Yang
Developing customizable pH-responsiveness for supramolecular hydrogels is of great significance and has drawn tremendous attention. Through systematic simulation analysis, we formulated a simple supramolecular hydrogel (i.e., poly(AAm-co-NaSS)/BSA on the basis of electrostatic interaction between the sulfonate groups of poly(AAm-co-NaSS) and the protonated side groups of BSA, and proposed a novel pH-responsive mode for it: changing the internal electric charge composition of the hydrogel through pH-induced ionization/protonation transition of BSA, thereby regulating the structural stability/shrinkage/extension of the supramolecular network. On basis of this theory, the pH-responsiveness of the poly(AAm-co-NaSS)/BSA hydrogel, in principle, could be pre-designed by adjusting the initial BSA/NaSS ratio. In this regard, we fabricated a poly(AAm-co-NaSS)/BSA hydrogel prototype with a BSA/NaSS ratio of 1/57 and investigated its rheological/swelling/disassembling behavior under different pH conditions (1.7, 4.7, 7.7, 10.7, and 13.7). In addition, we also prepared two capecitabine-loaded poly(AAm-co-NaSS)/BSA hydrogel prototypes with BSA/NaSS ratios of 1/57 and 1/102 respectively at pH 4.0, and compared their drug release behavior in SGF and SIF. Finally, the experimental results fitted well with our theoretical expectations, which testified the rationality of our assumption. Thus, we believed that the poly(AAm-co-NaSS)/BSA supramolecular hydrogel could find diverse applications in the future.
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ANALYTICAL CHEMISTRY
·
2020
·
IF 6.785
Lu Shi,Feifei Cao,Limin Zhang,Yang Tian
The development of switches responding to specific pH changes was particularly useful in wide application fields. Owing to flexible switches simulated by pH, i-motif DNAs are widely used as a pH sensor. But its character of structure transition strongly dependent on acidic pH severely hampers the application of i-motif DNA in physiological media. Herein, we report the stable i-motif structure formed at a physiological pH triggered by spatial confinement of silica nanochannels. Three classic DNA chains containing 21-mer i-motif domain base-pairs and a single-stranded multiply (T)n spacer, 5′-COOH-(T)n-CCCTAACCCTAACCCTAACCC-3′, were employed to evaluate the enhanced stability of i-motif structure. Compared to their free states in a dilute solution, the transition pH of all i-motif DNAs decorated in nanochannels remarkably shifts toward a neutral pH. Moreover, the transition midpoint can be tuned sensitively over the physiologically relevant pH range through slightly varying the length of T base spacer. Density functional theory (DFT) calculations validate that the increased proton density in a nanochannel triggers the formation of an i-motif structure under a neutral pH. Finally, this i-motif DNA based nanochannels electrode was successfully employed to monitor pH in brain microdialysates followed by cerebral ischemia. The present approach is not limited by fundamental investigation for DNA conformation but may extend toward the manipulation of i-motif based structures for artificial molecular machines and signaling systems.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2019
·
IF 5.107
Gang Yi,Xinfei Fan,Xie Quan,Haiguang Zhang,Shuo Chen,Hongtao Yu
Nanofiltration offers an effective solution in wastewater treatment by size sieving and particularly electrostatic interaction (Donnan effect). However, its separation performance fluctuates with pH changes because both membrane charge and contaminate ionization are sensitive to pH. Therefore, it is significant to fabricate a nanofiltration membrane with steady separation efficiency over a wide pH range. In this study, a novel pH-responsive reduced graphene oxide membrane intercalated by polyacrylic acid-grafted-carbon nanotube (RGO-gCNT membrane) was designed elaborately. Benefited from the pH-responsive property of polyacrylic acid, the pore size of RGO-gCNT membrane can be narrowed in acid solution and enlarged in basic solution. And the pore sizes at pH 3.0 and pH 8.2 are calculated to be about 0.8 and 1.3 nm, respectively. The results of pH influence on phosphate separation show that phosphate rejection rate of the non-responsive RGO-CNT membrane decreases sharply from 91.6% to 11.1% when the pH changes from 8.2 to 3.0. However, the pH-responsive RGO-gCNT membrane can retain 92.7% and 74.2% of the feed phosphates at pH 8.2 and 3.0, respectively. This novel pH-responsive RGO-gCNT membrane provides reliable separation efficiency over a wide pH range and gives new insight to design smart membranes.
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