FOOD CHEMISTRY
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2021
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IF 7.514
Zhenpeng Li,Quanquan Lin,David Julian McClements,Yuying Fu,Hujun Xie,Teng Li,Guowen Chen
In this study, core-shell biopolymer nanoparticles were fabricated for the encapsulation and delivery of curcumin using a pH-driven method. The influences of the coating composition on the physicochemical properties and curcumin release characteristics of the core-shell nanoparticles were studied. Fourier transform infrared spectroscopy and X-ray diffraction analyses indicated that curcumin was encapsulated in an amorphous state inside the nanoparticles. Particle size and ζ-potential measurements indicated that the biopolymer nanoparticles were relatively stable under different environmental conditions: long term storage, heating, pH changes and salt. The DPPH radical scavenging activity of the curcumin was increased after encapsulation within the nanoparticles, whereas the gastrointestinal release of curcumin was prolonged. These results were attributed to the ability of alginate and NaCas to form a thick layer around the nanoparticles, which increased the steric and electrostatic repulsion between them, as well as inhibiting the release of curcumin.
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ACS Biomaterials Science & Engineering
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2021
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IF 4.749
Zhenjie Zhang,Xiaoyan Niu,Xiaoyue Feng,Xiaohui Wang,Licheng Yu,Wei Wang,Zhi Yuan
The method of tumor microenvironment (TME)-responsive aggregation has become a promising approach to enhance treatment effect by improving the accumulation of nanoparticles in tumors. The enzymatic cross-linking strategy has widely attracted attention owing to its good aggregation stability and biocompatibility. However, the enzymes in nontumor tissue can also catalyze the cross-linking reaction and reduce accumulation of nanoparticles in tumor. In this work, a “dual key”-responsive strategy is utilized to construct a transglutaminase (TGase)/pH-responsive radiosensitizer (Au@TAcoGal) with specific aggregation behavior in hepatic tumor cells. Au@TAcoGal can retain its stability in blood circulation (pH 7.4) even in the presence of TGase in plasma. On reaching tumor sites, it can be endocytosed by hepatoma cells by the active targeting of phenylboronic acid (PBA) and aggregated under acidity and overexpression of TGase in cells. Due to its specific accumulation in hepatoma cells, radiotherapy can be operated under a lower dose of X-ray. The results show that the cellular accumulation of Au@TAcoGal increases by 30–70%, and the cell survival rate is less than 25% under X-ray irradiation. The antineoplastic results show that Au@TAcoGal exhibits a higher therapeutic effect, and the tumor inhibition rate can reach 84.21%.
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SCIENCE OF THE TOTAL ENVIRONMENT
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2021
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IF 7.963
Fuwei Sun,Tianhu Chen,Haibo Liu,Xuehua Zou,Peixun Zhai,Ziyang Chu,Daobing Shu,Hanlin Wang,Dong Chen
Occurring naturally siderite (FeCO 3 ) was used as the heterogeneous catalyst to activate peroxodisulfate (PDS) for the degradation of sulfadiazine under different initial pH values. The findings of this system exhibited various ROS (e.g. 1 O 2 , SO 4 − and OH) present during a wide range of pH values. Among them, 1 O 2 could significantly facilitate the initial degradation rate, and the increased pH enhanced the role of 1 O 2 . The factors including initial pH values, siderite dosage, PDS concentration, initial contaminants concentration, and water matrix were discussed. The role of each ROS was investigated through quenching test and electron paramagnetic resonance (EPR). Furthermore, the comprehensive degradation process was proposed based on the LC-MS results. And the cycle test demonstrates the reusability of siderite at a pH of 3. Accordingly, this study is of great significance for understanding the degradation of such sulfonamide pollutants in the siderite/PDS system.
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WATER RESEARCH
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2021
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IF 11.236
Lifa Ge,Yamei Yue,Wei Wang,Fatang Tan,Shenghua Zhang,Xinyun Wang,Xueliang Qiao,Po Keung Wong
Currently existing Fenton-like catalysts were limited in wastewater treatment owing to their potential transition-metal poisoning, narrow applicable pH range and high dependence on external energy excitation. In this work, the MgNCN/MgO nanocomposites were firstly synthesized by a facile one-pot calcination of melamine and basic magnesium carbonate, and used as novel H 2 O 2 activator for antibiotic removal. It was found that the MgNCN/MgO composite calcined at 550°C with the mass ratio of melamine to basic magnesium carbonate at 2:1, exhibited an excellent catalytic ability to tetracycline (TC) degradation in a wide pH range of 4-10 without any external energy input. More than 90% of TC (100 mL, 50 mg/L) could be degraded within 30 min by 10 mg of the nanocomposite in the presence of 0.2 mL of 30 wt% H 2 O 2 . Based on the experimental results, it was concluded that the Mg-N coordination between MgNCN and MgO in MgNCN/MgO nanocomposites activated H 2 O 2 to produce primary singlet oxygen ( 1 O 2 ) and minor hydroxyl radicals (·OH), responding for TC degradation. In addition, the degradation pathways of TC were deduced by determining the generated intermediates during the degradation process. This work provided a novel idea for designing transition-metal-free catalysts for nonradical activation of H 2 O 2 in the absence of external energy excitation.
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ACS Omega
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2021
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IF 3.512
Yinghua Tao,Dan Zheng,Jingyang Zhao,Kefeng Liu,Jing Liu,Jiandu Lei,Luying Wang
Pharmaceutical science based on biological nanotechnology is developing rapidly in parallel with the development of nanomaterials and nanotechnology in general. Pectin is a natural polysaccharide obtainable from a wide range of sources. Here, we show that doxorubicin (DOX)-conjugated hydrophilic pectin (PET) comprising an amphiphilic polymer loaded with hydrophobic dihydroartemisinin (DHA) self-assemble into nanoparticles. Importantly, conjugated DOX and DHA could be released quickly in a weakly acidic environment by cleavage of the acid-sensitive acyl hydrazone bond. Confocal microscopy and flow cytometry confirmed that these PET-DOX/DHA nanoparticles efficiently delivered DOX into the nuclei of MCF-7 cells. Significant tumor growth reduction was monitored in a female C57BL/6 mouse model, showing that the PET-DOX/DHA nanoparticle-mediated drug delivery system inhibited tumor growth and may improve therapy. Thus, we have demonstrated that pectin may be useful in the design of materials for biomedical applications.
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ANALYTICAL CHEMISTRY
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2021
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IF 6.986
Juan Qiao,Yuying Song,Chuanfang Chen,Li Qi
Sialic acid (SA) is an important monosaccharide that is involved in incurable cancer immunotherapy. However, it is difficult to detect SA in situ using the existing strategy based on the SA-terminated glycopeptide extraction from the cell lysate. The countermeasures of the bottleneck caused by cell disruption and peptide extraction should be designed based on a “cell-surface attachment and controlled enzymolysis” protocol. Herein, a poly(styrene-co-maleic anhydride-acrylic acid-concanavalin A) (PSM-PAA-ConA) was synthesized and developed as a pH-regulated enzyme nanoreactor after being loaded with sialidase and myoglobin. The nanoreactor showed controllable biocatalysis induced by a cascade enzyme reaction and applied for the in situ detection of SA on a living cell surface. The addition of an acidic solution resulted in a decrease in the size of the nanoreactor and enhancement of its permeability, triggering an “on” state of the SA catalysis. Subsequent pH increase led to increased hydrophilicity of the nanoreactor, increasing its size and resulting in the catalytic “off” state. ConA assisted the cell-surface attachment of the enzyme reactor. Furthermore, SA on the surface of living cancer cells was successfully monitored by the pH-regulated enzyme nanoreactor, demonstrating the feasibility of high specificity in situ analysis for SA. This pH-induced catalytic efficiency control by the enzyme nanoreactor provides a potential platform for functional stimuli-responsive catalytic systems as well as a strategy for in situ analysis of biomolecules on the cell surface.
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ACS Omega
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2021
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IF 3.512
Guodong Zheng,Jiahui Zheng,Le Xiao,Tongyi Shang,Yanjun Cai,Yuwei Li,Yiming Xu,Xiaoming Chen,Yun Liu,Bin Yang
In this study, a pH-responsive nano-prodrug was fabricated by conjugating emodin to the PEGylated polyethyleneimine (mPEG-PEI) with acid-sensitive boronate ester bonds. 1H NMR spectra results showed that emodin was effectively bonded to mPEG-PEI, and acid-sensitive assay further confirmed the formation of boronate ester bonds. The size and morphology of the nano-prodrug were ascertained through transmission electron microscopy (TEM) and dynamic light scattering (DLS), which showed that the prodrug has a sphere-like shape with hydrodynamic size around 102 nm at pH 7.4. Subsequently, a drug-release behavior assay was carried out to carefully investigate the acid-sensitive drug-delivery property of the prodrug. Moreover, in vitro cell viability assay confirmed the superior cytotoxic effect of the nano-prodrug against HeLa cells compared to free emodin. Furthermore, the antibacterial study showed that the nano-prodrug could inhibit the bacterial (both Gram-positive and Gram-negative) growth more effectively than free emodin. Overall, this study provides a promising paradigm of the multifunctional nano-prodrug for pH-responsive tumor therapy and antibacterial activity.
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ENVIRONMENTAL POLLUTION
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2021
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IF 8.071
Huan-Qin Li,Ying-Jia Shen,Wen-Lei Wang,Hong-Tao Wang,Hu Li,Jian-Qiang Su
Microplastic (MP) pollution is widespread in various ecosystems and is colonized by microbes that form biofilms with compositions and functions. However, compared with aquatic environments, the soil environment has been poorly studied in terms of the taxonomic composition of microbial communities and the factors influencing the community structure of microbes in the plastisphere. In the present study, a microcosm experiment was conducted to investigate the plastisphere bacterial communities of MP (polyvinyl chloride, PVC) in soils with different pH (4.62, 6.5, and 7.46) and arsenic (As) contents (13 and 74 mg kg −1 ). Bacterial communities in the plastisphere were dominated by Proteobacteria and Firmicutes, with distinct compositions and structures compared with soil bacterial communities. Soil pH and As content significantly affected the plastisphere bacterial communities. Constrained analysis of principal coordinates and a structural equation model demonstrated that soil pH had a stronger influence on the dissimilarity and diversity of bacterial communities than did soil As content. Soil pH affected As speciation in soil and on MP. The concentration of dimethylarsinic acid (DMA) was significantly higher on MP than that in soil, indicating that As methylation occurred on MP. These results suggest that environmental fluctuations govern plastisphere bacterial communities with cascading effects on biogeochemical cycling of As in the soil ecosystems.
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BIOMACROMOLECULES
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2021
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IF 6.988
Panpan Song,Nannan Song,Li Li,Minghao Wu,Zhongxia Lu,Xia Zhao
Glioblastoma (GBM) is a fatal brain tumor with poor prognosis. Blood–brain barrier (BBB) prevents the effective delivery of chemotherapeutic agents to GBM. Herein, we developed a pH/reduction-sensitive carboxymethyl chitosan nanogel (CMCSN) modified by targeting peptide angiopep-2 (ANG) and loaded with doxorubicin (DOX). The multifunctional nanogel (DOX-ANG-CMCSN) exhibited good pH and reduction sensitivity, ideal stability, and biocompatibility. Its hydrodynamic diameter was 190 nm, drug loading was 12.7%, and the cumulative release rate of 24 h was 82.3% under the simulated tumor microenvironment. More importantly, the modification of ANG significantly enhanced BBB penetration and tumor targeting ability both in vivo and in vitro. DOX-ANG-CMCSN achieved 2–3-fold higher uptake and an enhanced antitumor activity compared with nontargeted DOX-CMCSN. Therefore, the targeted nanogels with the pH/reduction dual-stimuli response may provide a promising platform for GBM-targeted chemotherapy.
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ACS Nano
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2021
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IF 15.881
Jinglin Shen,Qianwen Xiao,Panpan Sun,Jin Feng,Xia Xin,You Yu,Wei Qi
The self-assembly of chiral metal nanoclusters into supramolecular chiral aggregates is of interest for developing advanced materials. Herein, we manipulated the self-assembly of Au nanoclusters modified by l-/d-cysteine (l-/d-AuNCs) into ordered microstructures featuring enhanced phosphorescence and optical activities. The formation of these aggregates was driven by synergistic effect of coordination and electrostatic interactions assisted by Cd2+/H+. Detailed structural characterization and theoretical studies confirmed that the compact aggregation structures are essential for the emission enhancement and the chirality amplification of l-/d-AuNCs. Interestingly, upon the formation of microflowers, the emission lifetime was prolonged to 3.34 ms with a switch from fluorescence to phosphorescence induced by aurophilic Au(I)···Au(I) interactions and intensive ligand-to-metal charge transfer (LMCT). Moreover, both the CD and photoluminescence (PL) signals of the microflowers exhibited pH-responsiveness. This dual-mode sensitive platform could be developed as a pH sensor with improved accuracy. Additionally, the pH-responsive photoluminescence ON/OFF switch of the microflowers could be employed for reliable information encryption and decryption. This study provides useful ideas for regulating the self-assembly of nanoclusters to generate desired photophysical properties with potential applications.
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CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Cong Yang,Wenjie Xu,Xin Meng,Xinlong Shi,Luhua Shao,Xiangliang Zeng,Zhenfei Yang,Sijian Li,Yutang Liu,Xinnian Xia
Giving the coating to exert a powerful active protective effect for metal substrates, such as self-healing property by encapsulating corrosion inhibitor into a pH-responsive release tool, is a crucial way to develop an efficient anticorrosive coating. Here, a pH-responsive hydrophilic controlled release system (BTA@ZIF-8@tannic acid, abbreviated ZBT) based on ZIF-8 for waterborne EP self-healing anticorrosive coating was reported. Encapsulation of BTA into ZIF-8 by a facile one-pot method and the resulting product showed a high loading percentage. The anticorrosion performance of composite coatings was studied by EIS, and the results indicated that ZBT could effectively enhance the protective performance of the coating and endow it with outstanding self-healing performance, in which the |Z| 0.01 Hz was about 2 orders of magnitude higher than that of pure EP coating after 20 days of immersion. The outstanding performance is related to the excellent compatibility of ZBT, the blocking effect of newly produced hydrophobic substances and the corrosion inhibitor and ferric tannate protective films formed on the exposed metal surface. In this work, tannic acid plays a role of killing two birds with one stone in enhancing the corrosion protection performance of the coating. This synergistic strategy opens a new possibility to fabricating excellent anticorrosive coatings with efficient self-healing functionality.
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Journal of Magnesium and Alloys
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2020
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IF 7.115
Yuejun Ouyang,Lin-Xin Li,Zhi-Hui Xie,Lili Tang,Fuhui Wang,Chuan-Jian Zhong
The preparation of pH-responsive nanocontainers by typical silane modification of the mesoporous silica nanoparticle (MSN) surface is usually high-cost, complex, and time-consuming, which remains a great challenge for effective corrosion protection of magnesium alloy. Here, a new strategy to construct pH-responsive nanocontainers (MSN-MBT@LDH) is demonstrated. The nanocontainers consist of corrosion inhibitor (2-mercaptobenzothiazole, MBT) loaded MSN core and layered double hydroxide (LDH) nanosheet shell serving as gatekeepers. The successful loading of MBT and encapsulation by LDH nanosheets were confirmed by a series of characterization such as scanning transmission electron microscopy coupled with energy dispersive X-ray spectroscopy (STEM-EDS) and N 2 adsorption/desorption isotherms. The pH-responsive feature of the nanocontainers was demonstrated by determination of the MBT concentration in buffer solutions with different pH values. A smart corrosion protection system on Mg alloy is obtained by incorporating the synthesized nanocontainers into a self-assembled nanophase particle (SNAP) coating. The electrochemical tests and visual observations show that the hybrid coating has the best barrier properties and robustness in corrosion protection in NaCl corrosive solutions in comparison with the control coatings. The present method simplifies the synthesis processes of nanocontainers and eliminates the potential detrimental effect of excess gatekeepers on the coating. The findings provide new insights into the preparation of scalable nanocontainers. The self-healing coatings are expected to have widespread applications for corrosion protection of Mg alloy and other metals.
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