Nanomaterials
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2022
·Vol. 12
·期 12
·2094
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IF 5.719
Hongming Liu,Qin Zhou,Yongfu Lian
Individual single–walled carbon nanotubes (SWNTs) with distinct electronic types are crucial for the fabrication of SWNTs–based electronic and magnetic devices. Herein, the water–soluble polymethyl(1–butyric acidyl)silane (BA–PMS) was synthesized via the hydrosilylation reaction between 3–butenoic acid and polymethylsilane catalyzed by 2,2′–azodibutyronitrile. As a new dispersant, BA–PMS displayed a quite good dispersing capacity to arc–discharged SWNTs and moderate selectivity for metallic species. The application of sucrose–DGU, the density gradient ultracentrifugation with sucrose as the gradient medium, to the co–surfactants (BA–PMS and sodium dodecyl sulfonate) individually dispersed SWNTs yielded metallic SWNTs of 85.6% purity and semiconducting SWNTs of 99% purity, respectively. This work paves a path to the DGU separation of the SWNTs dispersed by polymer–based dispersants with hydrophobic alkyl chains.Keywords:polymethyl(1–butyric acidyl)silane;dispersion;density gradient ultracentrifugation
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IMMUNOPHARMACOLOGY AND IMMUNOTOXICOLOGY
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2022
·
IF 3.712
Sa-sa Zhang,Yi-jin Wu,Shu Pan,Qi-hai Wang,Wen-gang Chen,Zhong-fang Wang,Jin-ying Xu,Jian Zuo,Qin Yin
Background The first-line anti-rheumatic drug methotrexate (MTX) is used in the combination. Because of the unpredictable adverse reactions, optimization of relevant regimens is necessary and meaningful. This study aimed to study the possible interaction between Securidaca inappendiculate Hassk. Derived xanthones and MTX.Methods We established adjuvant-induced arthritis (AIA) model, which was treated with MTX and MTX + xanthone-rich fraction (XRF). The clinical efficacy was evaluated by histopathological examination, and LC-MS was used to monitor the blood concentration of MTX. Western blotting and immunohistochemistry were used to detect protein expression. In vitro, we assessed the activity of related transporters by cellular uptake assay based on HEK-293T cells.Results Compared with MTX-treated rats, inflammation in the immunized rats in the MTX + XRF group was obvious, indicating that XRF antagonized the anti-rheumatic effect of MTX. Meanwhile, XRF reduced liver and kidney injuries caused by MTX in addition to MTX. Results from immunohistochemical and nappendiculat assays suggested that XRF may reduce uptake of MTX by down-regulating reduced folate carrier 1 (RFC1).Conclusion This study indicated that XRF could reduce the plasma concentration of MTX by inhibiting the expression of RFC1, antagonize the therapeutic effect of MTX on AIA rats, and reduce its oral bioavailability. The combination of S. inappendiculate and MTX should be further optimized to achieve the goal of increasing efficiency and reducing toxicity.
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GENE
·
2022
·
IF 3.913
Xiaohong Chen,Yueya Zhang,Haifeng Yan,Meiyun Niu,Yuping Xiong,Xinhua Zhang,Yuan Li,Jaime A. Teixeira da Silva,Guohua Ma
The commercial value of Santalum album L. lies in its aromatic heartwood and essential oil. Sesquiterpenes are the main components of sandal essential oil, and these are synthesized through the plant’s mevalonate (MVA) and methylerythritol phosphate (MEP) pathways. In this study, the first key rate-limiting enzyme, 1-deoxy- d -xylulose-5-phosphate synthase (SaDXS), was investigated to provide a theoretical molecular basis for the sandalwood MEP sesquiterpene biosynthetic pathway. The biofunctions of SaDXS were also analyzed. SaDXS promoters were successfully cloned from a seven-year-old S. album tree. SaDXS1A/1B promoter activity was verified by a β-glucuronidase (GUS) assay and by analyzing cis -acting elements of the promoters, which carried light- and methyl jasmonate (MeJA)-responsive signals. In an experiment involving yellow S. album seedlings, exposure to light upregulated SaDXS1A/1B expression and increased chlorophyll and carotenoid contents when overexpressed in Arabidopsis thaliana . Analysis of the expression of SaDXS1A/1B and SaSSy , key genes of santalol biosynthesis, revealed SaDXS1A expression in all tissues whereas SaDXS1B was expressed in tissues that contained photosynthetic pigments, such as stems, leaves and flowers. Sandal seedlings exogenously treated with two hormones, MeJA and ethylene, revealed similar expression patterns for SaDXS1A/1B and SaSSy . Sandal seedlings were treated with an inhibitor of DXS, clomazone, but showed no significant changes in the contents of α-santalene, β-santalene and α-santalol between treatment and control groups. These results suggest that SaDXS1A/1B play a role in the synthesis of sandalwood sesquiterpenes, providing carbon for downstream secondary metabolites. SaDXS1A/1B also play a role in the biosynthesis of chlorophyll, carotenoids, and primary metabolites.
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SCIENCE OF THE TOTAL ENVIRONMENT
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2021
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IF 7.963
Yunfei Zhang,Qiang Zhao,Baoliang Chen
In materials science, “green” synthesis has gotten a lot of interest as a reliable, long-lasting, and ecofriendly way to make a variety of materials/nanomaterials, including metal/metal oxide nanomaterials . To accommodate various biological materials, green synthesis of metallic nanoparticles has been used (e.g., bacteria, fungi, algae, and plant extracts). In this work, Shewanella oneidensis MR-1 was used to biosynthesize palladium nanoparticles (bio Pd) under aerobic conditions for the Cr(VI) bio-reduction. The size and distribution of bio-Pd are controlled by adjusting the ratio of microbial biomass and palladium precursors. The high cell: Pd ratio has the smallest average particle size of 6.33 ± 1.69 nm. And it has the lowest electrocatalytic potential (−0.132 V) for the oxidation of formic acid , which is 0.158 V lower than commercial Pd/C (5%). Our results revealed that the small size and uniformly distributed extracellular bio-Pd could achieve completely catalytic reduction of 200 mg/L Cr(VI) solution within 10 min, while the commercial Pd/C (5%) need at least 45 min. The bio-Pd materials maintain a high reduction during five cycles. Microorganisms play an important role in the whole process, which can fully disperse palladium nanoparticles, completely reduce Cr(VI), and effectively adsorb Cr(III). This work expands our understanding and provides a reference for the design and development of efficient and green bio-Pd catalysts for environmental pollution control under simple and mild conditions.
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RSC Advances
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2021
·Vol. 11
·期 46
·28711-28715
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IF 3.361
Lin Bai,Shenglong Ding,Xiaofang Ma
An efficient methodology for the synthesis of symmetrical methylene diesters was developed through direct reaction of various aromatic carboxylates with 1,n-dihaloalkanes under solvent-free conditions. This strategy offers a high product yield, facile work-up and purification, and an environmentally friendly approach to obtain long-chain methylene carboxylate scaffolds with increased diversity.
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JOURNAL OF HAZARDOUS MATERIALS
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2021
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IF 10.588
Xiaoyan Ma,Lei Wang,Hong Wang,Jing Deng,Yali Song,Qingsong Li,Xueyan Li,Andrea M. Dietrich
Natural organic matter (NOM) has rich halogenation reactive sites, therefore acts as the main precursor of disinfection byproducts (DBPs) in the chlorine disinfection process during drinking water treatment . In this research, high-quality metal-organic framework HKUST-1 is rapidly synthesized by a solvothermal method, and we are the first to report adsorption of aqueous humic acid (HA), representing NOM, and its adsorption behavior, influencing factors, and recycling capability. The crystalline HKUST-1 possessed a microporous framework with a high 1385 m 2 /g specific surface area, and three-dimensional structure as characterized by Fourier transform infrared spectroscopy (FTIR), X-ray diffraction (XRD), scanning electron microscope (SEM). 99% removal of 5 mg/L HA was observed at pH 5.8, room temperature, and 0.6 g/L HKUST-1. The maximum capacity was 14.42 mg HA/g HKUST-1 at room temperature. The Langmuir adsorption isotherm , quasi-second-order kinetic model, and thermodynamic parameters accurately describe the spontaneous and disorderly endothermic adsorption of HA by HKUST-1. The desorption regeneration process was accomplished by washing HKUST-1 with NaOH and calcination ; it showed that HKUST-1 was viable in three regeneration cycles. The mechanism of HA adsorption by HKUST-1 is electrostatic and synergistic interaction between π-π bonding, and hydrogen bonding. HKUST-1 is a potential treatment strategy to remove NOM.
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MICROPOROUS AND MESOPOROUS MATERIALS
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2021
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IF 5.455
Jun Liang,Yingying Wang,Xiangcheng Li,Ming Xu,Shaochun Shen,Chuang Liu,Wenhua Fu,Weichuan Tao,Zhiqing Yuan,Zhendong Wang,Weimin Yang
A novel quaternary ammonium hydroxide , p-Xylylene-bis(N-methylpiperidinium hydroxide) (XBMPOH), was prepared and used as an organic structure-directing agent (OSDA) for the syntheses of BEC zeolites . Both Si,Ge- BEC and Al incorporated BEC (Al- BEC ) zeolites were successfully synthesized. In comparison with commonly used OSDA (tetraethylammonium hydroxide (TEAOH)), XBMPOH was more suitable for the crystallization of BEC structure, especially in the Al containing system. Al- BEC zeolites were directly synthesized at lower germanium and OSDA content, in a wider (Si + Ge)/Al ratio range (20 to ∞ vs. 50 to ∞) and shorter time (6 h vs. 12 h). For the first time, Al- BEC zeolites were used as a solid acid to catalyze the alkylation of benzene with 1-dodecene, and showed significant catalytic performance. After an acidic treatment procedure, the catalytic performance was further improved due to the removal of non-framework Al with accompanied exposure of framework Al.
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ENVIRONMENTAL TECHNOLOGY
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2021
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IF 3.247
Min Xiaobo,Li Xinyu,Zhao Jie,Hu Xiaoxian,Yang Weichun
Aiming at exploring an effective photocatalytic adsorbent for organic dye removal, a series of heterostructured TiO2@HKUST-1 photocatalysts, by incorporating HKUST-1 with different TiO2 nanoparticles loading, were prepared by single-step hydrothermal method. The morphology and surface characteristics of the as-prepared TiO2@HKUST-1were analyzed using SEM, HRTEM, XRD, FTIR, UV–vis DRS, and Photoluminescence techniques. The adsorption-photocatalytic degradation of the model dye methylene blue (MB) on the catalysts was investigated. It was indicated that the introduction of a certain amount of TiO2 on the surface of HKUST-1 could improve the transfer and separation of the photogenerated charge carriers, resulting in the enhanced photocatalytic activity. The optimal 0.02TiO2@HKUST-1 exhibited the highest MB removal rate with about 4.4 and 19.3 times as high MB removal efficiency as that of HKUST-1 and TiO2, respectively. Heterostructured TiO2@HKUST-1 materials for the removal of MB involved the integrated adsorption and visible light photocatalysis. Meanwhile, the composite exhibited good reusability in the process of cyclic experiments. Therefore, this work provides a potential MOF-based photocatalytic adsorbent for organic dye removal.
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Acta Biomaterialia
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2021
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IF 8.947
Xinran Song,Yuxin Jiang,Weixing Zhang,Gomaa Elfawal,Kaili Wang,Di Jiang,Huoyan Hong,Jinglei Wu,Chuanglong He,Xiumei Mo,Hongsheng Wang
Transcutaneous immunization (TCI) has the advantages of safety, high efficiency, non-invasiveness and convenient use. The key for a TCI system is transdermal targeted delivery of antigen to dendritic cells (DCs), the most powerful antigen presenting cells . DCs also play an important role in tumor immunotherapy, which provides a huge imagination for the application of TCI to tumor treatment. In this study, a transcutaneous tumor vaccine (TTV) delivery system was developed using the electrospun silk fibroin (SF) and polyvinyl alcohol (PVA) composite nanofibrous patch loaded with mannosylated polyethyleneimine (PEI man )-modified ethosome (Eth) (termed Eth-PEI man ). Eth-PEI man showed a good performance in targeting DCs, and the carriers loaded with antigen (encapsulated in Eths) and adjuvant (absorbed in PEI man ) were observed effectively induce DCs maturation in vitro. With the tyrosinase-related protein-2 (TRP2) peptide as antigen and oligodeoxynucleotides containing unmethylated CpG motifs as adjuvant, the TTV-loaded patches (TTVP) significantly inhibited the growth of melanoma in a syngeneic mouse model for melanoma by subcutaneous injection of B16F10 cell lines. Moreover, the combined application of the TTVP and anti-programmed death-1 monoclonal antibody (aPD-1) produced a synergistic antitumor effect, which could be related to the infiltration of more CD4 + and CD8 + T cells in the tumor tissues. The application of TTVP also increased the expression of IL-12, which may be part of the mechanism of synergistic antitumor effect between the TTVP and aPD-1. These results suggest that the combination of the TTVP and immune checkpoint blockers could be an effective strategy for tumor treatment. Statement of significance Transcutaneous immunization has the advantages of safety, high efficiency, non-invasiveness and convenient use. In this study, a novel transcutaneous tumor vaccine patch (TTVP) was developed using tumor antigens-loaded ethosomes that can target dendritic cells percutaneously. Our data demonstrated that the TTVP can significantly inhibit tumor growth. Furthermore, the combination of TTVP and aPD-1 produced a synergistic anti-melanoma effect. Considering its convenience and non-invasiveness, this TTVP system could find good application prospects in immunotherapy. The combination of TTVP and aPD-1 could be a useful strategy for the prevention and treatment of tumors.
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SENSORS AND ACTUATORS B-CHEMICAL
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2021
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IF 7.46
Liyan Zhang,Xiaoting Liu,Nan Zhang,Xianqiang Liu,Wei Jiang
Sensitive and accurate detection of flap endonuclease 1 (FEN1) is essential to understand its roles in DNA replication and repair and explore its functions in tumor diagnosis and prognosis. Here, we designed a magnetic separation-assisted cascade hybridization chain reaction (HCR) amplification strategy for enzyme-free and sensitive detection of FEN1. Firstly, the forked dsDNAs contained the recognition site (5′ overhanging DNA flap) of FEN1 were modified on magbeads surface to form magnetic recognition probes. By the recognition and catalytic cleavage of FEN1, the 5′ flaps were removed into solution and then purified by magnetic separation. Then, the obtained flaps served as triggers to activate the linear-assembly of hairpin probes H1 and H2 (primary HCR), forming nicked double helices with split fragments. Finally, the fragments acted as new triggers to activate the branched-assembly of hairpin probes H3 and H4 (secondary HCR), causing fluorophore/quencher labeled on H3 far away and fluorescence recovery. Benefiting from the purification of triggers by magnetic separation and the signal amplification effect of cascade HCR, this strategy achieved a low detection limit of 3.6 × 10 −5 U μL −1 for FEN1, and enabled the assay of it in actual samples. The results demonstrate that our strategy will provide a potent approach for sensitive detection of FEN1 in early tumor diagnosis and prognosis.
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ACS Applied Materials & Interfaces
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2021
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IF 9.229
Di Wu,Xiangyu Zhu,Jian Ao,Erqun Song,Yang Song
Endosome capture is a major physiological barrier to the successful delivery of nanomedicine. Here, we found a strategy to deliver ultrasmall nanoparticles (<10 nm) to the cytosolic compartment of pyroptotic cells with spontaneous endosomal escape. To mimic pathological pyroptotic cells, J774A.1 macrophages were stimulated with lipopolysaccharide (LPS) plus nigericin (Nig) or adenosine triphosphate (ATP) to form specific gasdermin D protein-driven membrane pores at an N-terminal domain (GSDMDNterm). Through GSDMDNterm membrane pores, both anionic and cationic nanoparticles (NPs) with diameters less than 10 nm were accessed into the cytosolic compartment of pyroptotic cells in an energy- and receptor-independent manner, while NPs larger than the size of GSDMDNterm membrane pores failed to enter pyroptotic cells. NPs pass through GSDMDNterm membrane pores via free diffusion and then access into the cytoplasm of pyroptotic cells in a microtubule-independent manner. Interestingly, we found that LPS-primed NPs may act as Trojan horse, deliver extracellular LPS into normal cells through endocytosis, and in turn induce GSDMDNterm membrane pores, which facilitate further internalization of NPs. This study presented a straightforward method of distinguishing normal and pyroptotic cells through GSDMD membrane pores, implicating their potential application in monitoring the delivery of desired nanomedicines in pyroptosis-related diseases and conditions.
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ADVANCED FUNCTIONAL MATERIALS
·
2021
·Vol. 32
·期 8
·2107349
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IF 18.808
Mun Kyoung Kim,Hojeong Lee,Jong Ho Won,Woohyeong Sim,Shin Joon Kang,Hansaem Choi,Monika Sharma,Hyung-Suk Oh,Stefan Ringe,Youngkook Kwon,Hyung Mo Jeong
Electrochemical carbon dioxide reduction reaction (CO 2 RR) is a promising approach to mitigate CO 2 concentration and generate carbon feedstock. Recently, the (sub-)nanometer design of catalyst structures has been revealed as an efficient means to control the reaction process through the local reaction environment. Herein, the synthesis of a novel tin oxide (SnO x ) nanoparticle (NP) catalyst with highly controlled sub-nanoscale interplanar gaps of widths <1 nm (SnO x NP-s) is reported via the lithium electrochemical tuning (LiET) method. Transmission electron microscopy (TEM) and 3D-tomo-scanning TEM (STEM) analysis confirm the presence of a distinct segmentation pattern and the newly engineered interparticle confined space in the SnO x NP-s. The catalyst exhibits a significant increase in CO 2 RR versus hydrogen evolution selectivity by a factor of ≈5 with 20% higher formate selectivity relative to pristine SnO 2 NPs at −1.2 V RHE . Density functional theory calculations and cation-size-dependent experiments indicate that this is attributable to a gap-stabilization of the rate-limiting *OCHO and *COOH intermediates, the formation of which is driven by the interfacial electric field. Moreover, the SnO x NP-s exhibits stable performance during CO 2 RR over 50 h. These results highlight the potential of controlled atomic spaces in directing electrochemical reaction selectivity and the design of highly optimized catalytic materials.
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