The heterostructure Ag–Au bimetallic nanocrystals supported on Fe3O4@carbon composite microspheres were synthesized by one facile and controllable approach, wherein the Ag nanocrystals attached on the Fe3O4@carbon microspheres were prepared first and served as reductant for the galvanic replacement reaction with the Au precursor (HAuCl4). Upon varying the feeding amounts of the Au precursor, the bimetallic compositions on the Fe3O4@carbon microsphere could be readily tuned resulting in a series of composite microspheres with different Au-to-Ag molar ratios. Subsequently, we thus investigated the catalytic activity and selectivity of the magnetic composite catalysts from two sides. First, 4-nitrophenol (4-NP) was applied as a model molecule to study the effect of different Au-to-Ag molar ratios on catalytic capabilities of the resulting composite microspheres. It was found that upon the addition of NaBH4 the catalytic capability was markedly enhanced when the Au content was increased. The maximum activity parameter value reached 1580 s–1 g–1, which is far higher than those of known monometallic composites. Also, they could give the equally high yields for other nitroaromatic compounds with various substituents, irrespective of the linked electron-donating or electron-withdrawing groups. Second, the synergistic effects of the carbon substrate in the catalysis reaction were demonstrated. When compared with colloidal SiO2, TiO2, and poly(styrene-co-acrylic acid) substrates, the carbon support not only facilitated the enhancement of the catalytic performance of the noble metal nanocrystals but was also more suitable for the in situ preparation of Au–Ag bimetallic nanocrystals using the GRR. Besides, the particles’ convenience in terms of their magnetic separability and outstanding reusability was validated through many successive reduction reaction cycles. In light of these unique characteristics, the Fe3O4@C@Ag–Au composite microspheres show promising and great potential for practical applications.
Ascorbic acid (AA) is capable of inhibiting cancer cell growth by perturbing the normal redox state of cells and causing toxic effects through the generation of abundant reactive-oxygen species (ROS). However, the clinical utility of AA at a tolerable dosage is plagued by a relatively low in vivo efficacy. This study describes the development of a peroxidase-like composite nanoparticle for use in an AA-mediated therapeutic strategy. On the basis of a high-throughput, one-pot solvothermal approach, Fe3O4@C nanoparticles (NPs) were synthesized and then modified with folic acid (FA) on the surface. Particular focus is concentrated on the assessment of peroxidase-like catalytic activity by a chromogenic reaction in the presence of H2O2. The carbon shell of Fe3O4@C NPs contains partially graphitized carbon and thus facilitates electron transfer in the catalytic decomposition of H2O2, leading to the production of highly reactive hydroxyl radicals. Along with magnetic responsiveness and receptor-binding specificity, the intrinsic peroxidase-like catalytic activity of Fe3O4@C-FA NPs pronouncedly promotes AA-induced oxidative stress in cancer cells and optimizes the ROS-mediated antineoplastic efficacy of exogenous AA. In vitro experiments using human prostate cancer PC-3 cells demonstrate that Fe3O4@C-FA NPs serve as a peroxidase mimic to create hydroxyl radicals from endogenous H2O2 that is yielded in response to exogenous AA via an oxidative stress process. The usage of a dual agent leads to the enhanced cytotoxicity of PC-3 cells, and, because of the synergistic effect of NPs, the administrated dosage of AA is reduced markedly. However, because normal cells (HEK 293T cells) appear to have a higher capacity to cope with additionally generated ROS than cancer cells, the NP-AA combination shows little damage in this case, proving that selective killing of cancer cells could be achieved owing to preferential accumulation of ROS in cancer cells. A possible ROS-mediated mechanism is discussed to elucidate the pharmaceutical profile of the NP-AA agent. In general, this foundational study reveals that the peroxidase-like nanomaterials are applicable for modulating oxidative stress for the selective treatment of cancer cells by generating a high level of endogenous ROS.
Highly active surface-enhanced Raman scattering (SERS) substrates of Ag nanoparticle (Ag-NP) modified Fe(3)O(4)@carbon core-shell microspheres were synthesized and characterized. The carbon coated Fe(3)O(4) microspheres were prepared via a one-pot solvothermal method and were served as the magnetic supporting substrates. The Ag-NPs were deposited by in situ reduction of AgNO(3) with butylamine and the thickness of the Ag-NP layer was variable by controlling the AgNO(3) concentrations. The structure and integrity of the Fe(3)O(4)@C@Ag composite microspheres were confirmed by TEM, XRD, VSM and UV-visible spectroscopy. In particular, the Ag-NP coated Fe(3)O(4)@carbon core-shell microspheres were shown to be highly active for SERS detections of pentachlorophenol (PCP), diethylhexyl phthalate (DEHP) and trinitrotoluene (TNT). These analytes are representatives of environmentally persistent organic pollutants with typically low SERS activities. The results suggested that the interactions between the carbon on the microsphere substrates and the aromatic cores of the target molecules contributed to the facile pre-concentration of the analytes near the Ag-NP surfaces.
Graphene@Fe3O4@C core–shell nanosheets are synthesized by a one-pot solvothermal method, which are promising candidates as anodes in LIB applications.
In this study, a class of surface enhanced Raman spectroscopy (SERS) encoded core-shell nanospheres was synthesized as nano-SERS-tags for detecting specific DNA targets based on the sandwich hybridization assays. These core-shell nanospheres were synthesized by first depositing a layer of Ag-NPs (nanoparticles) onto the poly(styrene-co-acrylic acid) core and then the formation of a layer of uniform silica as the outer shell. The Ag-NPs served as SERS substrates with Raman active molecular probes adsorbed onto the Ag-NPs as indicative SERS molecular barcodes, and the silica coating shell was used for protecting the Ag-NPs and the Raman molecules from the exterior chemical and biological interference. The silica surfaces of nano-SERS-tags were further conjugated with probe DNA (pDNA) (nano-SERS-probes). The detection of single-stranded oligonucleotide (ssDNA) targets was successfully accomplished using the nano-SERS-probes in a chip-based sandwich hybridization assay in a mixed ssDNA target solution. The as-prepared nano-SERS-probes exhibited high chemical stability during the laser SERS experiments and the results were reproducible after a long-term storage. At least four different tags (a four ''color'' system) were quantitatively differentiated when simultaneously applied in the assays, indicating an excellent multiplexing potential of the method. Therefore, the as-prepared nano-SERS-probes are suitable for high specific detection of biomolecules with high sensitivity and remarkable multiplexing capability associated with the SERS method.
The discovery of novel, effective, and botanical pesticides is one of the main strategies for modern plant protection and insect pest control. During the search for novel botanical pesticides from natural sources, the seeds of Sophora tonkinensis were systematically investigated to obtain 11 new matrine-type alkaloids (1–11), including one novel matrine-type alkaloid featuring an unprecedented 5/6/6/6 tetracyclic skeleton (1), along with 16 known compounds (12–27). Their structures were elucidated by comprehensive spectroscopic data analysis (IR, UV, NMR, and HRESIMS), ECD calculations, and single-crystal X-ray diffraction. The anti-tobacco mosaic virus (TMV) activity and insecticidal activities against Aphis fabae and Tetranychus urticae of the compounds were also respectively screened using the half-leaf method and spray method. Biological tests indicated that compounds 2, 4, 6, and 26 displayed significant anti-TMV biological activities compared with the positive control ningnanmycin. Compounds 7, 17, and 26 presented moderate activities against A. fabae with LC50 values of 38.29, 18.63, and 23.74 mg/L, respectively. Moreover, compounds 13 and 26 exhibited weak activities against T. urticae.
Selective enrichment of glycopeptides from complicated biological samples is essential for MS-based glycoproteomics, but still remains a great challenge. In this study, we report an unprecedented ligandfree strategy for the selective enrichment of glycopeptides by simply utilizing the multivalent interaction between glycopeptides and silver nanoparticles (Ag-NPs) coated magnetic nanoarchitectures. The composite microspheres were deliberately designed to be constructed with a high-magnetic-response magnetic colloid nanocrystal cluster (MCNC) core, a poly(methacrylic acid) (PMAA) interim layer and a Ag-NPs functional shell with high coverage. Taking advantage of the reversible interaction of glycans with Ag-NPs and the high magnetic susceptibility of the magnetite core, the MCNC@PMAA@Ag-NPs microspheres possess remarkable selectivity for glycopeptides even at a low molar ratio of glycopeptides/non-glycopeptides (1 : 100) with a very rapid enrichment speed (only 1 min needed) and a simple operation procedure using magnetic separation. Applying this approach, we identified 127 unique glycopeptides mapped to 51 different glycoproteins from only 1 mL rat serum samples. These results clearly demonstrated that the MCNC@PMAA@Ag-NPs have great potential for purifying and identifying the low-abundant glycopeptides in complex biological samples.
As part of our ongoing investigation of pesticide active quinolizidine alkaloids (QAs) from the family Fabaceae, the chemical constituents of the seeds of Thermopsis lanceolata R. Br. were systematically investigated. Bioassay-guided fractionation and purification of the crude extract led to the isolation of seventeen new QAs (1−17), including three new naturally occurring compounds (15−17), along with 15 known compounds (18−32). Their structures were elucidated by comprehensive spectroscopic data analysis (IR, UV, NMR, and HRESIMS) and quantum chemistry calculations ( 13 C NMR and ECD). The antitomato spotted wilt virus activities and insecticidal activities against Aphis fabae, Nilaparvata lugens (Stal), and Tetranychus urticae of compounds 1− 32 were screened using the lesion counting method, spray method, and rice-stem dipping method, respectively. Biological tests indicated that compounds 6, 9, 10, and 18 displayed significant anti-TSWV activities compared with the positive control ningnanmycin.
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