CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Hui Liu,Haoyuan Li,Siyuan Xia,Shanshan Yu,Yujie Duan,Lei Wang,Hongxiang Zhu,Hui He
The monitoring of intracellular pH value is beneficial for the early diagnosis and treatment of some diseases. Here, a cellulose nanocrystal (CNC)-based upconversion ratiometric fluorescent nanoprobe for pH monitoring and imaging was constructed by chemicaliy bonding the upconversion nanoparticles donor and fluorescein isothiocyanate and rhodamine B acceptors using CNC as a bridge. The CNC bridge could improve stability and solve the problems of aggregation-caused quenching of dye on the donor surface, long donor-to-acceptor distance, and poor water dispersibility of the probe. The probe with a double internal reference of donor and rhodamine B acceptor exhibited excellent selectivity, sensitivity and visualization for intracellular pH of 5.0–7.4 with 980 nm excitation. Interestingly, the chameleon-inspired biocompatible probe based on the luminescent resonance energy transfer platform enhanced the depth of penetration and demonstrated excellent pH monitoring and imaging in living cells and in vivo . Therefore, it has promising application for the early diagnosis and treatment of some diseases.
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COLLOIDS AND SURFACES B-BIOINTERFACES
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2022
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IF 5.999
Kaijun Gou,Wei Xin,Jinying Lv,Zihao Ma,Juqin Yang,Lin Zhao,Ying Cheng,Xuchun Chen,Rui Zeng,Heran Li
The purpose of this study was to develop a nano-drug delivery system with intelligent stimuli-responsive drug delivery in tumor microenvironment (TME). Based on chiral mesoporous silica nanoparticles (CMSN) with a chiral recognition function in our previous research, a pH-responsive CMSN (CS-CMSN) was successfully prepared by chemical modification of chitosan (CS), and the related physicochemical properties, drug release performance, potential anti-tumor effect, and biological safety were studied. The results showed that the CS-CMSN were successfully modified by CS. Moreover, CS-CMSN displayed superior encapsulation ability for doxorubicin (DOX) and exhibited controllable pH-responsive drug release properties. In particular, in a physiological environment (pH 7.4/6.5), CS shielded the nanopores , prevented DOX release, and minimized side effects on normal cells. Once the CS-CMSN was exposed to the TME (pH 5.0), the pH-sensitive moiety of CS was cleaved in an acidic environment, along with the rapid release of DOX. In vitro cell experiments further proved that [email protected] was more strongly taken up by 4T1 cells and could enhance the toxicity to 4T1 tumor cells as well as promote cell apoptosis. More importantly, CS-CMSN were shown to have good biosafety in vitro and in vivo . Overall, the delivery of DOX by CS-CMSN nanocarriers is a promising strategy for tumor-targeted therapy.
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OPTICS EXPRESS
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2022
·Vol. 30
·期 24
·42801-42809
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IF 3.833
Guolu Yin,Guolu Yin,Hu Xiao,Hang Zhou,Tao Zhu,Tao Zhu
We propose a distributed pH sensor based on an optical frequency domain reflectometry using a PEGDA-based pH-sensitive hydrogel coated on a single mode fiber. The volume of hydrogel increased as pH value of the surrounding fluid decreased, which converts the pH value to the axial strain in the fiber. Taking capacity of distributed strain measurement with high spatial resolution in optical frequency domain reflectometry, the pH value of the external medium is distributed measured by the wavelength shifts of the local Rayleigh backscattering spectra. The basic hydrogel with different molecular weight was optimized to balance the sensitivity, the response time and also the stability. In the experiment, the range of the pH value from 2 to 6 was measured with a sampling resolution of 1.7 mm, a sensitivity of -199 pm/pH and a response time of 14 min when the hydrogel coating diameter is 2 mm. Such a distributed pH sensing system has a potential to detect and locate some chemical or biological substances in a large-scale environment.
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Acta Biomaterialia
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2022
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IF 10.633
Linzhu Su,Yuanfeng Li,Shuang Tian,Fan Huang,Yijin Ren,Cuihong Yang,Henny C. van der Mei,Henk J. Busscher,Linqi Shi
Antibiotic-loaded PEG/PAE-based micelles are frequently considered for eradicating infectious biofilms. At physiological pH, PEG facilitates transport through blood. Near an acidic infection-site, PAE becomes protonated causing micellar targeting to a biofilm. However, micellar penetration and accumulation is confined to the surface region of a biofilm. Especially matured biofilms also possess hypoxic regions. We here designed dual-responsive PEG/PAE- b -P(Lys-NBCF) micelles, responding to both acidity and low oxygen-saturation level in matured biofilms. Dual, pH- and hypoxia-responsive micelles targeted and accumulated evenly over the depth of 7- to 14-days old biofilms. Delineation demonstrated that pH-responsiveness was responsible for targeting of the infection-site and accumulation of micelles in the surface region of the biofilm. Hypoxia-responsiveness caused deep penetration in the biofilm. Dual, pH- and hypoxia-responsive micelles loaded with ciprofloxacin yielded more effective, synergistic eradication of 10-days old, matured Staphylococcus aureus biofilms underneath an abdominal imaging-window in living mice than achieved by ciprofloxacin in solution or single, pH- or hypoxia responsive micelles loaded with ciprofloxacin. Also, wound-healing after removal of window and its frame proceeded fastest after tail-vein injection of ciprofloxacin-loaded, dual, pH- and hypoxia-responsive micelles. Concluding, pH- and hypoxia-responsiveness are both required for eradicating mature biofilms and advancing responsive antibiotic nanocarriers to clinical application. Statement of significance pH-responsive antibiotic nanocarriers have emerged as a possible new strategy to prevent antimicrobial-resistant bacterial infections from becoming the leading cause of death. In this paper, we show that commonly studied, pH-responsive micellar nanocarriers merely allow self-targeting to an infectious biofilm, but do not penetrate deeply into the biofilm. The dual-responsive (acidic pH- and hypoxia) antibiotic-loaded micelles designed here not only self-target to an infectious biofilm, but also penetrate deeply. The in vitro and in vivo advantages of dual-responsive nanocarriers are most obvious when studied in infectious biofilms grown for 10 viz a viz the 2 days, usually applied in the literature. Significantly, clinical treatment of bacterial infection usually starts more than 2 days after appearance of the first symptoms.
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FOOD HYDROCOLLOIDS
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2022
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IF 11.504
Ya-Ru Wang,Qin Yang,Ya-Nan Du,Han-Qing Chen
Food protein fibrils display superior mechanical and interfacial properties compared to the native protein. During processing, protein fibrils are stored for a long time and undergo pH shifts, which accelerate their degradation. In this study, the effects of chitosan on the morphology, structural and rheological properties of ovalbumin (OVA) fibrils after storage at pH higher than isoelectric point were studied. The results showed that OVA fibrils prepared at pH 2.0 remained stable after 7 days of storage. However, after storage at pH 8.0 for 7 days, the turbidity of OVA fibrils increased, the contour length and ThT fluorescence intensity decreased. Furthermore, OVA fibrils became stable again by interacting with chitosan via electrostatic interaction, which was confirmed by zeta potential . In addition, based on the results of Fourier transform infrared spectroscopy , sodium dodecyl sulfide polyacrylamide gel electrophoresis , and fluorescence spectra, it could be concluded that chitosan could interact with OVA fibrils at pH 8.0 during storage. Transmission electron microscope images indicated that the structure of OVA fibrils was maintained by the addition of positively charged chitosan. Finally, the viscosity and storage modulus of OVA fibrils after storage at pH 8.0 increased with the addition of chitosan. These findings implied that OVA fibrils were degraded when stored at pH above isoelectric point, but this degradation could be ameliorated by the addition of chitosan.
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Gels
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2022
·Vol. 8
·期 10
·683
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IF 4.432
Xiangbin Liu,Suling Wang,Weiguang Shi,He Liu
Smart hydrogels, owing to their exceptional viscoelastic and deformable capacity in response to environmental stimulation involving temperature and pH, have been successfully applied in oilfields for purposes such as water and/or gas shutoff treatments. However, the CO2breakthrough problem in low permeability reservoirs has not been well solved. In this work, a rheological method-based Avrami dynamics model and Dickinson dynamics model were employed to investigate the dynamic gelation process of thermo-/pH-dual-sensitive PEG/PAMAM nanogels to further our understanding of the microstructure of their gelation and pertinence plugging application. Plugging experiments were performed by alternating injections of CO2and hydrogel solution in a slug type on three fractured low permeability cores with a backpressure of 13 MPa. The nanogels presented a secondary growth pattern from three to one dimension from micrometer to nanometer size with a morphological transformation from a sphere to an irregular ellipsoid or disk shape. The phase transition temperature was 50 °C, and the phase transition pH was 10. If both or either were below these values, the hydrogel swelled; otherwise, it shrank. Plugging results show that the plugging efficiency was higher than 99%. The maximum breakthrough pressure was 19.93 MPa, and the corresponding residual pressure remained 17.64 MPa for a 10 mD core, exhibiting great plugging performance and high residual resistance after being broken through by CO2.Keywords:smart nanogel;PEG;PAMAM;reaction dynamics;CO2channeling plugging
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Environmental Science-Processes & Impacts
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2022
·Vol. 24
·期 7
·1071-1081
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IF 5.334
Qiqi Wei,Qiang Zhang,Yihan Jin,Usman Farooq,Weifeng Chen,Taotao Lu,Deliang Li,Zhichong Qi
To date, there is still very little knowledge about the combined effects of typical inorganic ligands and solution pH values on mobility characteristics of tetracycline (TC) through saturated aquifer media. In this work, three typical inorganic ligands (i.e., phosphate, silicate, and iodate) were employed in the transport experiments. Generally, all the ligands promoted TC mobility over the pH range of 5.0–9.0 owing to the enhanced electrostatic repulsion between sand grains and TC anionic forms (i.e., TC− and TC2−) as well as the competitive deposition between ligands and antibiotic molecules for attachment sites. Furthermore, the transport-enhancement effects of ligands on TC intensively depended on ligand type and followed the sequence of phosphate > silicate > iodate. This phenomenon was ascribed to their different molecular sizes and binding abilities to sand grains. Interestingly, the differences in extents of enhanced effects of various inorganic ligands on TC transport varied with background solution pH due to pH-induced different extents of deposition site competition effects. Moreover, the two-site nonequilibrium model (which accounts for an equilibrium site and a kinetic site) as well as adsorption and kinetic studies were performed to help interpret the controlling mechanisms for the synergistic effects of inorganic ligands and solution pH on TC transport in saturated quartz sand. The findings of our study clearly demonstrate that inorganic ligands may be critical factors in assessing the fate and transport of antibiotics in groundwater systems.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2022
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IF 8.025
Yumin Wu,Ying Ma,Yiliang Gao,Yuetao Liu,Chuanhui Gao
A poly (lactic acid) (PLA) -based functional partition composite membrane (PLA/CA) containing chitosan (CS) and alizarin (AL) was designed by solution casting method. The PLA/CA membrane contains the antibacterial zone of the edge part (PLA/CS) and the pH response detection zone of the central part (PLA/AL). At the same time, the environmentally friendly plasticizer tributyl citrate (TBC) was added to make the prepared PLA/CA composite membrane have good flexibility and high transparency. The results of FE-SEM and FTIR showed that CS and AL were uniformly dispersed in PLA matrix and had good compatibility with PLA. The antioxidant activities of PLA/CS and PLA/AL composite films were 43.3 % and 72.8 %, respectively. At the same time, the inhibitory rates of PLA/CS membrane against Escherichia coli and Staphylococcus aureus were as high as 87.91 % and 75.17 %, respectively. PLA/AL films exhibit excellent UV barrier properties. When the environmental pH (ammonia and acetic acid vapor) changed repeatedly, the PLA/AL membrane showed reversible color change of yellow under acidic condition and purple under alkaline condition. During the packaging and storage of chicken breast meat, the freshness of chicken breast meat can be detected by the color change of functional PLA/CA composite membrane.
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INTERNATIONAL JOURNAL OF PHARMACEUTICS
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2022
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IF 6.51
Tingting Du,Yuchi Wang,Zhiyong Luan,Chaoyue Zhao,Kangjuan Yang
The low immunogenicity and tumor immunosuppressive microenvironment (TIM) are two major obstacles for cancer immunotherapy . Synergistically immunogenic cell death induction and tumor-associated macrophages depletion could perfectly overcome this limitation. Herein, a tumor-associated macrophage (TAMs) membrane-camouflaged pH-responsive doxorubicin (DOX) loaded hyaluronic acid (HA)-g-poly (histidine) polymeric micelles ( [email protected] ) was fabricated for the first time. [email protected] could effectively accumulated into tumor regions via TAMs membrane mediated immune camouflage. In acidic tumor microenvironment , particle size of DHP was enlarged due to decrease hydrophobic interaction of inner core, which caused a “membrane escape effect” to expose inner HA residue. Together high expression of α4β1 integrin , [email protected] could reach CD44/VCAM-1 dual-targetability to facilitate intracellular DOX accumulation for efficient ICD induction. Meanwhile, TAMs membrane could absorb colony stimulating factor 1(CSF1) through high expression of its receptor (CSF1R) on TAMs membrane to deplete TAMs in tumor tissues and relieved TIM. This strategy could efficiently induce cytotoxic T lymphocyte (CTLs) infiltration for antitumor immune response and inhibit tumor progression in 4T1 tumor bearing Balb/c mice. Therefore, [email protected] is suitable for cancer chemotherapy-sensitized immunotherapy.
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COLLOIDS AND SURFACES B-BIOINTERFACES
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2022
·
IF 5.999
Xinjing Du,Yuanyuan Peng,Chunyue Zhao,Jinfeng Xing
Tumor microenvironment-responsive nanogels loading antitumor drugs can improve the chemotherapy efficiency due to their suitable size, great hydrophilicity , excellent biocompatibility, and sensitivity to specific stimulation. Herein, a simple and effective strategy of one-pot laser-induced emulsion polymerization at 532 nm was developed to prepare carmofur-loaded nanogels based on biocompatible and temperature/pH-sensitive monomers including polyethylene glycol diacrylate (PEGDA), N-vinylcaprolactam (NVCL), and 2-(dimethylamino) ethyl methacrylate (DMAEMA). The nanogels loading carmofur with dual-stimuli responsive drug release properties were rapidly obtained under laser irradiation (beam diameter 2.5 mm, laser power 60 mW) for only 100 s. These nanogels exhibited an average hydrodynamic diameter of 195.9 nm and a low polydispersity index of 0.115. The effect of monomer ratio on the size, morphology, double-bond conversion, and thermo/pH-sensitivity of nanogels was investigated. The cumulative carmofur release from nanogels at pH 5.0 within 48 h was nearly three times that at pH 7.4, while the release amount at 42 °C was twice that at 25 °C, showing the controlled and sustainable release with the change of pH and temperature. The in vitro release kinetics of carmofur was in accord with first-order release model.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2022
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IF 5.518
Xianliang Li,Yuyang Di,Zhihao Chen,Wenzhong Yang
In this study, novel pH-sensitive bimetallic Ce-ZIF-8 nanocontainers are loaded with benzotriazole (BTA) corrosion inhibitors and then decorated with a polydopamine (PDA) shell. The applied PDA layer acts as an acid-responsive gatekeeper, controlling the intelligent release of the encapsulated inhibitors and also preventing their self-leakage. UV–vis and ICP-OES tests indicate that the BTA and cerium inhibitors release slowly in the neutral 3.5 wt% NaCl solution. Afterward, the designed pH-responsive Ce-ZIF-8-BTA-PDA nanocontainers are dispersed uniformly in the epoxy matrix as a novel intelligent filler. EIS results demonstrate that the incorporation of Ce-ZIF-8-BTA-PDA nanocontainers significantly improves the corrosion resistance of epoxy coatings, in which the low-frequency impedance is about three orders of magnitude higher than that of the pure epoxy coating after 60 days of immersion. Furthermore, the low-frequency value of the scratched Epoxy-Ce-ZIF-8-BTA-PDA coating increases from 5.05 × 10 5 Ω cm 2 to 8.83 × 10 5 Ω cm 2 after 8 h of exposure to the 3.5 wt% NaCl solution, confirming their outstanding self-healing performance. The excellent corrosion protection and self-healing ability are due to the incorporation of the Ce-ZIF-8-BTA-PDA nanocontainers, improving the surface compactness and therefore enhancing the physical barrier effect. Moreover, the intelligent release of the encapsulated corrosion inhibitors provides active corrosion protection performance by forming a dense protective film on the Al alloy surface when the coating is damaged. Meanwhile, the highly dispersed nanocontainers lengthen the diffusion path of corrosive ions and therefore extend the service life of the epoxy coatings in aggressive environments. This new type of acid-responsive smart coating based on the bimetallic Ce-ZIF-8 nanocontainers has the potential to broaden the future applications of active corrosion protection of metals.
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EUROPEAN JOURNAL OF MEDICINAL CHEMISTRY
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2022
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IF 7.088
Yi Zhao,Yao Peng,Zhongzhen Yang,Jiaqi Lu,Ru Li,Yuesen Shi,Yaxin Du,Ze Zhao,Li Hai,Yong Wu
To synergistically treat glioma with a combination chemotherapy, we design and prepare novel cascade-targeted liposomes (Lip-TPGS) using glucose and triphenylphosphonium (TPP) as targeting moieties, which could intelligently deliver redox-sensitive doxorubicin (DOX) prodrugs (SDOX) and chemotherapeutic sensitizer lonidamine (LND). The pH-responsive ligand Chol-TPG modified by PEGylated glucose can overcome the blood-brain barrier and reach tumor cells. Combined with the modification of mitochondria targeting ligand (Chol-TPP), Lip-TPGS are endowed with pH-responsive charge regulation function and multi-stage targeting abilities. After triggered by the excessive glutathione in tumor cells, Lip-TPGS could sufficiently release the parent drugs DOX, which would significantly reduce side effects without compromising anti-glioma efficacy. Therefore, Lip-TPGS possess these characteristics: good pharmacokinetic behavior, superior brain targeting ability, specific tumor recognition and internalization capability, and strong endo/lysosome escaping and mitochondria targeting potential. Furthermore, Lip-TPGS exhibit significant advantages on anti-glioma by inhibiting proliferation, promoting apoptosis , inducing mitochondria dysfunction, inhibiting migration and invasion, prolonging the survival time, narrowing tumor areas, limiting lung metastasis , and reducing toxicity to normal organs. In summary, Lip-TPGS, with cascade targeting abilities from tissue/cell to organelle levels and highly controlled drug release properties, would become a promising drug delivery system for glioma treatment.
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