Nanomaterials
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2020
·Vol. 10
·期 10
·2000
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IF 4.324
Yongpan Shan,Chunli Xu,Hongjun Zhang,Huiping Chen,Muhammad Bilal,Shujun Niu,Lidong Cao,Qiliang Huang
Recently, metal–organic frameworks (MOFs) have become a dazzling star among porous materials used in many fields. Considering their intriguing features, MOFs have great prospects for application in the field of sustainable agriculture, especially as versatile pesticide-delivery vehicles. However, the study of MOF-based platforms for controlled pesticide release has just begun. Controlled pesticide release responsive to environmental stimuli is highly desirable for decreased agrochemical input, improved control efficacy and diminished adverse effects. In this work, simple, octahedral, iron-based MOFs (NH2-Fe-MIL-101) were synthesized through a microwave-assisted solvothermal method using Fe3+as the node and 2-aminoterephthalic acid as the organic ligand. Diniconazole (Dini), as a model fungicide, was loaded into NH2-Fe-MIL-101 to afford Dini@NH2-Fe-MIL-101 with a satisfactory loading content of 28.1%. The subsequent polydopamine (PDA) modification could endow Dini with pH-sensitive release patterns. The release of Dini from PDA@Dini@NH2-Fe-MIL-101 was much faster in an acidic medium compared to that in neutral and basic media. Moreover, Dini@NH2-Fe-MIL-101 and PDA@Dini@NH2-Fe-MIL-101 displayed good bioactivities against the pathogenic fungus causing wheat head scab (Fusarium graminearum). This research sought to reveal the feasibility of versatile MOFs as a pesticide-delivery platform in sustainable crop protection.Keywords:metal–organic framework;polydopamine;pesticide;pH-sensitive release;fungicidal activity
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PROCESS BIOCHEMISTRY
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2020
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IF 2.952
Yan Zhang,Hongzhou Zhang,Dong He,Xuejun Cao,Junfen Wan
Aqueous two-phase systems have been widely studied for the separation and recovery of bioproducts. In this study, the thermosensitive polymer EO 30 PO 70 and pH-responsive polymers (P ADB4.66 and P ADB6.26 ) were used to develop a recyclable aqueous two-phase system suitable for spiramycin partitioning. EO 30 PO 70 represents poly-(ethylene oxide-propylene oxide), where 30 and 70 indicate the proportions of ethylene oxide and propylene oxide, respectively. P ADB4.66 and P ADB6.26 represent poly-(acrylic acid-dimethylamine ethyl methacrylate-butyl methacrylate), where the numbers (4.66 and 6.26) in the subscripts indicate the isoelectric point of the polymers. The phase separation mechanism of ATPS was studied through low-field nuclear magnetic resonance (LF-NMR) and surface tension. Moreover, the parameters affecting spiramycin partitioning, such as system components and composition, pH, temperature, and type and concentration of additive salt, were investigated. The best partitioning conditions were determined using 4.70% P ADB6.26 and 31.67% EO 30 PO 70 in the presence of 0.05 mol/L NaSCN at 35 °C and pH = 9.2. The highest partition coefficient of spiramycin from fermentation broth was 11.92, with an extraction recovery of 97.69%. In addition, phase-forming polymers P ADB6.26 and EO 30 PO 70 could be recovered by regulating the pH or temperature, and their recoveries reached 92.39% and 98.76%, respectively.
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ACS Omega
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2021
·
IF 3.512
Shuhua Chang,Dawei Qin,Rongjun Yan,Mengli Zhang,Binglin Sui,Hui Xu,Zhaomin Zheng,Xiaoli Hou,Yonggang Wang,Chenggang Qi
pH- and temperature-sensitive nanogels (NGs) were prepared from sodium alginate (SA) and N-isopropylacrylamide (NIPAM), as the sensitivity at pH 5.5 and 31 °C. SA was pH-modified with glutamic acid (Glu) and ethylenediamine (EDA). The products Glu-SA (Glu-modified SA) and EGSA (EDA- and Glu-modified SA) were characterized by ninhydrin color reaction, infrared spectroscopy, and zeta potential, and the best reactant ratio was selected. Moreover, temperature-sensitive, pH-sensitive EGSA-NGs possessing a semi-interpenetrating network structure were prepared by radical polymerization using N-isopropylacrylamide. The morphology of EGSA-NGs was characterized by transmission electron microscopy (TEM), scanning electron microscopy (SEM), and atomic force microscopy (AFM). The cytotoxicity test shows the low cytotoxicity and high biocompatibility of the NGs. The newly prepared NGs were also subjected to pH-sensitive temperature-sensitive in vitro drug-loading and drug-release experiments. The pH-sensitive and temperature-sensitive experiments showed that the particle size of EGSA-NGs was reduced at pH 5.5 and above 31 °C. The drug-loading and drug-release experiments also confirmed this finding, indicating that the newly synthesized NGs could release the drug according to the environmental changes. Therefore, the material has potential application value in solid tumor targeted therapy.
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JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
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2020
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IF 4.192
Yu Xu,Xiang Li,Wei Gong,Hai-Bo Huang,Bei-Wei Zhu,Jiang-Ning Hu
The aim of this study is to construct a pH- and reduction-responsive nanodrug delivery system to effectively deliver a ginsenoside (Rh2) and enhance its cytotoxicity against human hepatocarcinoma cells (HepG2). Here, pullulan polysaccharide was grafted by urocanic acid and α-lipoic acid (α-LA) to obtain a copolymer, α-LA-conjugated N-urocanyl pullulan (LA-URPA), which was expected to have pH and redox dual response. Then, the copolymer LA-URPA was used to encapsulate ginsenoside Rh2 to form Rh2 nanoparticles (Rh2 NPs). The results showed that Rh2 NPs exhibited an average size of 119.87 nm with a uniform spherical morphology. Of note, Rh2 NPs showed a high encapsulation efficiency of 86.00%. Moreover, Rh2 NPs possessed excellent pH/reduction dual-responsive drug release under acidic conditions (pH 5.5) and glutathione (GSH) stimulation with a low drug leakage of 14.8% within 96 h. Furthermore, Rh2 NPs with pH/reduction dual response had higher cytotoxicity than Rh2 after incubation with HepG2 cells for 72 h, indicating that Rh2 NPs had a longer circulation time. After the treatment with Rh2 NPs, the excessive increase of reactive oxygen species and the decrease of superoxide dismutase, glutathione (GSH), and mitochondrial membrane potential suggested that the mitochondrial pathway mediated by oxidative stress played a role in this Rh2 NP-induced apoptosis. In conclusion, this study provides a new strategy for improving the application of ginsenoside Rh2 in the food and pharmaceutical fields.
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RSC Advances
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2020
·Vol. 10
·期 40
·23532-23542
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IF 3.119
He Guo,Xiaomeng Cheng,Hongping Li,Jun Li,Jinjin Wei,Chongyang Feng
A new nanoprobe, the luminescent diblock copolymer PNIPAM(MAh-4)-b-P4VP (PN4P), with pH- and thermo-responsive deprotonation-driven emission decay (DDED) and aggregation-induced emission (AIE) features was designed and synthesized. The nanoprobe PN4P can form micellar structures in water with reversible dual-responsive fluorescence (FL) behavior within a wide pH range of 2–11. The critical solution temperature was found at about 32, 30 and 27 °C as the pH switched from 2, 7 to 11. The critical pH value of the probe was about 4.0, and the micelles showed a core–shell inversion in response to pH and thermal stimuli, accompanied by a desirable emission tunability. P4VP as the micellar shell at pH = 2 was more easily dehydrated with the increase in temperature as compared to PNIPAM as the micellar shell at pH > 4. The strongest dehydration of the P4VP shell would make PN4P the most strongly aggregated and the most AIE-active, which supports the 2.10-fold most distinguished thermal-responsive emission enhancement at pH = 2. Moreover, a dramatic acidochromic redshift of the emission band from 450 (pH > 4) to 490 nm (pH = 2) was observed, and the maximum emission at pH = 2 was enhanced by about 2.07-fold as compared with that at pH = 7. Therefore, the probe displays the desired dual responses and good reversibility. AIE and DDED are the two major mechanisms responsible for the dual-responsive emission change, with AIE playing a more important role than DDED. This work offers a promising approach to interpreting temperature (range from 28 to 40 °C) and pH changes (range from 2 to 7) in water.
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CERAMICS INTERNATIONAL
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2020
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IF 3.83
Jinyue Zhang,Mingshi Jin,Yong Il Park,Longyi Jin,Bo Quan
Manganese silicate nanoparticles have recently attracted great attention due to the effectiveness of T 1 -weighted magnetic resonance imaging (MRI) contrast agents (CAs) in the mildly acidic and high glutathione (GSH) conditions of the tumor microenvironment. Herein, ultra-small hollow manganese silicate (UHMS) nanoparticles were prepared via a facile, economical, and eco-friendly method based on a hydrothermal process using small silica nanoparticles as both the silicon source and templates. The nanoparticles showed remarkable biocompatibility and dispersion stability after modification with polyethylene glycol (PEG). Owing to their ultra-high longitudinal relaxation rate (r 1 ) at low pH values and high GSH levels, the [email protected] nanoparticles have performed an excellent pH/GSH-responsive T 1 -weighted MRI. Meanwhile, the nanoparticles showed insignificant cytotoxicity in vitro and in vivo. Therefore, the [email protected] nanoparticles show promise as T 1 -MRI CAs in the tumor microenvironment and may be used to assist in clinical cancer diagnosis.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2020
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IF 5.162
Bahaaldin Rashidzadeh,Ebrahim Shokri,Gholam Reza Mahdavinia,Reza Moradi,Sarvin Mohamadi-Aghdam,Shadi Abdi
This work reports the synthesis of novel antibacterial magnetic-/pH-sensitive hydrogel beads based on ionotropic-gelation of alginate biopolymer . Using pomegranate peels extract, green-Ag nanoparticles were synthesized inside a mixture of alginate and Fe 3 O 4 , via in situ method. The alginate beads were investigated by VSM, TEM , XRD, and FE-SEM techniques. The introducing Ag and Fe 3 O 4 nanoparticles in hydrogel beads caused a reduction in the swelling capacity of hydrogel beads. Besides, a pH-dependent swelling behavior was observed for hydrogel beads with a maximum swelling capacity at pH = 7.4. Diclofenac sodium (DS) as a model drug was loaded in hydrogel beads and its release showed a pH-dependent behavior. Drug release studies exhibited significant behaviors on the subject of physiological simulated pHs with a high release rate at pH = 7.4. The alginate beads have shown a prolonged and successive controlled drug release nearly 83% at pH = 7.4 and time 200 min. In addition to the pH, the release of DS from magnetic beads was affected by the external-magnetic-fields. Also, the Ag-incorporated alginate beads showed strong antibacterial activity against S. aureus and E. coli . These results indicated that the hydrogel beads have potentially applicable in drug delivery systems.
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JOURNAL OF MOLECULAR LIQUIDS
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2020
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IF 5.065
Wei Long,Hui Ouyang,Chaoqun Zhou,Weimin Wan,Shengxian Yu,Kai Qian,Meiying Liu,Xiaoyong Zhang,Yulin Feng,Yen Wei
Molybdenum disulfide (MoS 2 ) is one of the most promising two-dimensional (2D) materials after graphene oxide . Its excellent properties make it promising for various applications, especially in the field of biomedicine owing to its small size, unique 2D morphology and photothermal conversion capacity. However, the lack of specific surface functional groups has still largely impeded their surface modification and for drug loading and controlled release. In this paper, the surface of MoS 2 sheets was modified by hydrazine groups, which could form dynamic hydrazone bonds with CHO-PEG and doxorubicin hydrochloride (DOX) to construct the PEGylated MoS 2 based drug delivery systems. The structure, thermal stability, surface morphology and particle size of MoS 2 related materials were characterized by different equipment. The characterization results confirm that these functionalized MoS 2 (MS-CO-NH) composites have been successfully prepared through the formation of dynamic bonds. On the other hand, the release of MS-P-D composites loaded with CHO-PEG and DOX showed that pH responsive behavior, and had a good sustained-release effect. More importantly, cell viability and internalization results showed that MS-CO-NH material had excellent biocompatibility. MS-P-D composite has good cancer treatment effect, and can transport DOX into HepG2 cells and slowly release DOX into the nucleus to kill cancer cells. In view of the results, we believe that this new MoS 2 -based vector is expected to be a candidate for controlling intracellular drug delivery and cancer treatment.
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SENSORS AND ACTUATORS B-CHEMICAL
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2020
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IF 7.1
Kun Zhou,Zhida Zhao,Pengbo Yu,Zheyao Wang
This paper presents a method of achieving high sensitivity for silicon nanowire (SiNW) field-effect transistor (FET) pH sensor by operating the FETs in both capacitive amplification mode and differential amplification mode. The capacitive amplification is implemented by employing an inversed double-gate configuration that uses the electrode immersed in a solution well etched from the backside of the sensor chip as the top gate and the SiNW metal gate as the back gate. This enables the threshold voltages of the FETs to be amplified through the ratio of the top gate capacitance to the back gate capacitance. The differential amplification is achieved by a readout circuit chip that is vertically integrated with the sensor chip using flip-chip bonding. This allows the back gate to be controlled independently by the circuits, such that the differential amplification that is originally applicable to single-gate FETs can be applied to double-gate FETs. By operating the dual amplifications simultaneously, a sensitivity of 720.7 mV/pH has been achieved in the pH range of 4−10. Small deviations between the SiNW pH sensor and a commercial pH meter in measuring phosphate buffer saline, bovine serum, and tap water demonstrate the capability of the SiNW pH sensor in measuring practical samples.
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Journal of Environmental Chemical Engineering
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2020
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IF 4.3
Lilan Huang,Leitao Zhang,Deyuan Li,Qingping Xin,Rui Jiao,Xiaoyang Hou,Yuzhong Zhang,Hong Li
Delicate design of hierarchical and porous nanoarchitectures has become a highly effective strategy to develop novel bimetallic catalyst with improved stability and catalytic performance. Herein, a core-shell hierarchical 4A zeolite/Fe@Cu Fenton-like catalyst with 4A zeolite/Fe as core components and two-dimensional Cu hydroxide nanosheets assemblies as shell structure was fabricated through a simple and scalable approach and used for phenol degradation. The results indicated that 4A zeolite/Fe@Cu bimetallic catalyst had higher catalytic activity and utilization efficiency of H 2 O 2 than that of 4A zeolite/Fe and 4A zeolite@Cu monometallic catalysts at near neutral pH. In the presence of H 2 O 2 , the 4A zeolite/Fe@Cu bimetallic catalyst could remove 95.3 % phenol after 4 h at pH 5, which was much higher than that of monometallic catalyst under the same condition. The enhanced activity of 4A zeolite/Fe@Cu was ascribed to the synergistic effect between the 4A zeolite/Fe (core) and two-dimensional Cu hydroxide nanosheets (shell). More importantly, the copper hydroxide nanosheets with open network structure on the surface of 4A zeolite/Fe@Cu improved the stability of the Fe(III) at acidic conditions, and avoided reduced catalytic efficiency of Fe(III) caused by embedding effect. This strategy provided guidance to the design of high-performance bimetallic Fenton-like catalysts.
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LANGMUIR
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2020
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IF 3.557
Wenwen Liu,Junjie Li,Zhihui Qin,Mengmeng Yao,Xinlu Tian,Zhiming Zhang,Li Zhang,Qin Guo,Linhua Zhang,Dunwan Zhu,Fanglian Yao
Circulation stability in vivo and stimuli-responsiveness under a tumor microenvironment of the polymeric prodrug micellar drug delivery systems are very critical to improve the tumor therapeutic efficiency. In this study, a series of polyamidoamine (PAMAM)-graft-poly(2-(diethylamino) ethyl methacrylate) (PDEAEMA)-block-poly(betaine sulfonate) (PSBMA) (PDS) unimolecular micelles were prepared via atom transfer radical polymerization. PAMAM served as a hydrophobic core to load the drug, the PDMAEMA segment was a middle layer to provide both thermo- and pH-sensitivity, whereas the PSMBA shell layer was used to improve the stability of the unimolecular micelles. The PDS exhibited a spherical structure with the size of 10–20 nm at pH 7.4. PDS micelles had excellent stability to resist the large volume liquid dilution. Moreover, it exhibited excellent stability in a complex biological microenvironment because of a superhigh antiprotein adhesion capacity of the PSBMA shell layer compared with PAMAM micelles. Drug release studies confirmed that the DOX can remain in the PDS micelles at pH 7.4 and 37 °C, whereas it can rapidly be released when the pH decreases to 5.0 and/or the temperature increases to 40 °C. In vitro studies suggested that the PDS drug delivery system can effectivity induce apoptosis and inhibit the proliferation of cancer cells. In vivo studies suggested that the PDS micelles prolonged the circulation time, decreased the side effects, and increased the antitumor efficacy. Therefore, the prepared PDS micelles are a potential anticancer drug delivery carrier for cancer therapy.
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Materials
·
2020
·Vol. 13
·期 6
·1279
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IF 3.057
Yanqin Xu,Liyue Xiao,Yating Chang,Yuan Cao,Changguo Chen,Dan Wang
In order to achieve a controlled release drug delivery system (DDS) for cancer therapy, a pH and redox dual-responsive mesoporous silica nanoparticles (MSN)-sulfur (S)-S- chitosan (CS) DDS was prepared via an amide reaction of dithiodipropionic acid with amino groups on the surface of MSN and amino groups on the surface of CS. Using salicylic acid (SA) as a model drug, SA@MSN-S-S-CS was prepared by an impregnation method. Subsequently, the stability, swelling properties and drug release properties of the DDS were studied by x-ray diffraction, scanning electron microscopy, Fourier transform infrared microspectroscopy, size and zeta potential as well as Brunauer–Emmett–Teller surface area. Pore size and volume of the composites decreased after drug loading but maintained a stable structure. The calculated drug loading rate and encapsulation efficiency were 8.17% and 55.64%, respectively. The in vitro drug release rate was 21.54% in response to glutathione, and the release rate showed a marked increase as the pH decreased. Overall, double response functions of MSN-S-S-CS had unique advantages in controlled drug delivery, and may be a new clinical application of DDS in cancer therapy.Keywords:mesoporous silica nanoparticles;double response;drug delivery;drug release
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