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Prof. Dr. Koji Kano Toshiro Ochi Sayuri Okunaka Yusuke Ota Keiichi Karasugi Takunori Ueda Dr. Hiroaki Kitagishi 《化学:亚洲杂志》2011,6(11):2946-2955
Poly(acrylic acid) (PAA) is modified by 5‐(4‐β‐alanylaminophenyl)‐10,15,20‐tris(4‐sulfonatophenyl) porphinatoiron(III) to yield iron porphyrin‐bearing PAAs (FeP(n)s) through a condensation reaction. FeP(n)s were further functionalized by Py3CD, which is a per‐O‐methylated β‐cyclodextrin (CD) dimer with a pyridine linker and includes the porphyrin pendants to form ferric hemoCD‐P(n)s. Ferrous hemoCD‐P(3), having three porphyrin chromophores in a polymer chain, is shown to bind molecular oxygen (P1/2=7.9±1.4 Torr) in aqueous solution at pH 7.0 and 25 °C, affording oxy‐hemoCD‐P(3). Oxy‐hemoCD‐P(3) is biphasically autoxidized to ferric hemoCD‐P(3), with 27 % of the dioxygen adducts being rapidly oxidized. The rate of autoxidation of oxy‐hemoCD‐P(15), having 15 porphyrin chromophores in a polymer chain, was much faster than that of oxy‐hemoCD‐P(3), thus suggesting self‐catalyzed autoxidation of oxy‐hemoCD‐P(n)s. Oxy‐hemoCD‐P(n)s are markedly stabilized by catalase, thereby indicating that hydrogen peroxide generated from oxy‐hemoCD‐P(n) accelerates the autoxidation. Most of the hemoCD‐P(3) molecules injected into the femoral vein of a rat remained in the body, though about 16 % of the hemoCD‐P(3) molecules were excreted in the urine as a carbon monoxide adduct. 相似文献
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金溶液pH值及浸泡处理对Au/Al2O3催化剂上CO氧化反应活性的影响 总被引:2,自引:0,他引:2
采用阴离子浸渍法制备了Au/Al2O3催化剂,考察了溶液pH值及浸泡处理对催化剂上CO氧化反应的影响. 结果表明,催化剂的活性随着浸渍液氯金酸溶液pH值的升高而升高. 对于经300 ℃下H2还原处理的Au/Al2O3催化剂,无论用水浸泡还是用氨水浸泡,室温下CO转化率均可达到100%, 且催化剂具有良好的稳定性. 用氨水浸泡的催化剂经氧化处理后依然保持高活性,但用水浸泡的催化剂活性大幅度下降. XPS结果表明,用氨水浸泡的Au/Al2O3催化剂表面含有Al, O, C, N, Na和Au原子,但没有Cl原子存在. 这说明用氨水浸泡催化剂可有效除去Cl-离子而提高其催化活性. 相似文献
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Dr. Sandra García‐Gallego Dr. Gonçalo J. L. Bernardes 《Angewandte Chemie (International ed. in English)》2014,53(37):9712-9721
The development of carbon‐monoxide‐releasing molecules (CORMs) as pharmaceutical agents represents an attractive and safer alternative to administration of gaseous CO. Most CORMs developed to date are transition‐metal carbonyl complexes. Although such CORMs have showed promising results in the treatment of a number of animal models of disease, they still lack the necessary attributes for clinical development. Described in this Minireview are the methods used for CORM selection, to date, and how new insights into the reactivity of metal‐carbonyl complexes in vivo, together with advances in methods for live‐cell CO detection, are driving the design and synthesis of new CORMs, CORMs that will enable controlled CO release in vivo in a spatial and temporal manner without affecting oxygen transport by hemoglobin. 相似文献
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Spontaneous CO Release from RuII(CO)2–Protein Complexes in Aqueous Solution,Cells, and Mice 下载免费PDF全文
Dr. Miguel Chaves‐Ferreira Inês S. Albuquerque Dr. Dijana Matak‐Vinkovic Dr. Ana C. Coelho Dr. Sandra M. Carvalho Dr. Lígia M. Saraiva Prof. Carlos C. Romão Dr. Gonçalo J. L. Bernardes 《Angewandte Chemie (International ed. in English)》2015,54(4):1172-1175
We demonstrate that RuII(CO)2–protein complexes, formed by the reaction of the hydrolytic decomposition products of [fac‐RuCl(κ2‐H2NCH2CO2)(CO)3] (CORM‐3) with histidine residues exposed on the surface of proteins, spontaneously release CO in aqueous solution, cells, and mice. CO release was detected by mass spectrometry (MS) and confocal microscopy using a CO‐responsive turn‐on fluorescent probe. These findings support our hypothesis that plasma proteins act as CO carriers after in vivo administration of CORM‐3. CO released from a synthetic bovine serum albumin (BSA)–RuII(CO)2 complex leads to downregulation of the cytokines interleukin (IL)‐6, IL‐10, and tumor necrosis factor (TNF)‐α in cancer cells. Finally, administration of BSA–RuII(CO)2 in mice bearing a colon carcinoma tumor results in enhanced CO accumulation at the tumor. Our data suggest the use of RuII(CO)2–protein complexes as viable alternatives for the safe and spatially controlled delivery of therapeutic CO in vivo. 相似文献
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Dr. Alice Boccia Dr. Fabio D'Orazi Dr. Elena Carabelli Dr. Rocco Bussolati Prof. Arturo Arduini Prof. Andrea Secchi Dr. Andrea G. Marrani Prof. Robertino Zanoni 《Chemistry (Weinheim an der Bergstrasse, Germany)》2013,19(24):7999-8006
The assembly of gold nanoparticles (AuNPs) on a hydrogenated Si(100) surface, mediated by a series of hierarchical and reversible complexation processes, is reported. The proposed multi‐step sequence involves a redox‐active ditopic guest and suitable calix[n]arene‐based hosts, used as functional organic monolayers of the two inorganic components. Surface reactions and controlled release of AuNPs have been monitored by application of XPS, atomic force microscopy (AFM), field‐emission scanning electron microscopy (FESEM) and electrochemistry. 相似文献
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Kai Klein Matthias Hayduk Sebastian Kollenda Marco Schmiedtchen Jens Voskuhl Matthias Epple 《Molecules (Basel, Switzerland)》2022,27(6)
Three different alkyne-terminated aggregation-induced emission molecules based on a para-substituted di-thioether were attached to the surface of ultrasmall gold nanoparticles (2 nm) by copper-catalyzed azide–alkyne cycloaddition (click chemistry). They showed a strong fluorescence and were well water-dispersible, in contrast to the dissolved AIE molecules. The AIE-loaded nanoparticles were not cytotoxic and easily penetrated the membrane of HeLa cells, paving the way for an intracellular application of AIE molecules, e.g., for imaging. 相似文献
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采用柠檬酸钠还原法制备粒径13 nm的金纳米颗粒(AuNPs)作为比色信号报告分子,3-氨基-5-巯基-1,2,4-三唑(AMT)作为Cr~(3+)的识别分子,构建了一种水中Cr~(3+)的比色传感检测方法。将AMT修饰于AuNPs表面,形成稳定的AMT-AuNPs水溶复合物;根据AMT与Cr~(3+)之间的特异性结合,引起溶液中AMT-AuNPs聚集,进而导致溶液颜色由红色变为蓝紫色以及最大吸收峰红移的现象,实现了水中Cr~(3+)的比色检测。在优化实验条件(AMT修饰浓度为0.8μmol/L,pH 7.0)下,该方法的检测范围为6~14μmol/L,检出限可达100 nmol/L,其他重金属离子几乎不存在干扰。由于该方法具有响应快(5 min)、制备和操作简单、无需读取装置等优点,可望用于水体中Cr~(3+)的现场快速检测。 相似文献
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E. M. S. Azzam A. A. Abd El-aal O. Shekhah H. Arslan Ch. Wöll 《Journal of Dispersion Science and Technology》2014,35(5):717-724
In this work, we investigated the fabrication of surface plasmon resonance (SPR) nanosensor using gold nanoparticles (AuNPs) chemisorbed onto self assembled monolayer of 10-(3-amino phenoxy) decane-1-thiol on gold substrate. The fabrication process of SPR nanosensor was characterized using different techniques such as infrared reflection-absorption spectra (IRRAS), xX-ray photoelectron spectroscopy (XPS), and atomic force microscope (AFM). The fabricated SPR nanosensor was used for detection of Cu2+ in an aqueous solution using surface plasmon resonance refractometer. The results confirm the fabrication of new SPR nanosensor. The fabricated SPR nanosensor showed a good activity toward the detection of Cu2+. The detection of Cu2+ in an aqueous solution using the fabricated SPR nansensor was enhanced in the presence of gold nanoparticles. 相似文献
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Assessing the Role of Capping Molecules in Controlling Aggregative Growth of Gold Nanoparticles in Heated Solution 下载免费PDF全文
This report describes findings of an investigation of the role of capping molecules in the size growth in the aggregative growth of pre‐formed small‐sized gold nanoparticles capped with alkanethiolate monolayers toward monodispersed larger sizes. The size controllability depends on the thiolate chain length and concentration in the thermal solution. The size evolution in solution at different concentrations of alkanethiols is analyzed in relation to adsorption isotherms and cohesive energy. The size dependence on thiolate chain length is also analyzed by considering the cohesive energy of the capping molecules, revealing the importance of cohesive energy in the capping structure. Theoretical and experimental comparisons of the surface plasmonic resonance optical properties have also provided new insights into the mechanism, thus enabling the exploitation of size‐dependent nanoscale properties. 相似文献
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Dr. Carmen Martin Dr. Katharina Kastner Dr. Jamie M. Cameron Elizabeth Hampson Dr. Jesum Alves Fernandes Dr. Emma K. Gibson Dr. Darren A. Walsh Dr. Victor Sans Dr. Graham N. Newton 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(34):14437-14441
We report the design and preparation of multifunctional hybrid nanomaterials through the stabilization of gold nanoparticles with thiol-functionalised hybrid organic–inorganic polyoxometalates (POMs). The covalent attachment of the hybrid POM forms new nanocomposites that are stable at temperatures and pH values which destroy analogous electrostatically functionalised nanocomposites. Photoelectrochemical analysis revealed the unique photochemical and redox properties of these systems. 相似文献
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Wenxin Dai Dr. Xun Chen Xiangping Zheng Zhengxin Ding Dr. Xuxu Wang Prof. Dr. Ping Liu Prof. Dr. Xianzhi Fu Prof. Dr. 《Chemphyschem》2009,10(2):411-419
On the surface : Adsorption of O2 at the surface oxygen vacancy (SOV) sites of TiO2 reconstructs the lattice oxygen (healing SOVs), resulting in a decrease of the photocatalytic activity of oxidizing CO over vacuum‐pretreated TiO2 with increasing temperature (see scheme). Adsorption of H2 produces new SOVs at the TiO2 surface and stabilizes the photocatalytic activity.
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以有序的中孔炭材料CMK-3为模板,以硝酸铈为前体,利用纳米铸型法合成了具有规则结构的中孔氧化铈,考察了模板脱除温度对中孔氧化铈微结构的影响.热重、元素分析、X射线衍射、透射电镜和氮气物理吸附结果表明,炭模板的脱除温度可低至350℃,所得氧化铈具有二维六方规则结构,比表面积高达167 m~2/g,孔径分布集中在3~5nm.采用胶体沉积法将2-5nm的金溶胶粒子沉积到所得氧化铈表面制得了Au/CeO_2催化剂,考察了Au/CeO_2在CO氧化反应中的活性.结果表明,该催化剂的活性较常规氧化铈制备的金催化利有明显提高,这可能与载体的规则结构有关. 相似文献
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Atefeh Ghorbani Aghdam Iran Almzadeh Majid Zeinali 《Journal of Dispersion Science and Technology》2013,34(8):1062-1065
Gold nanoparticles are potentially very attractive components for therapeutic delivery since they can be synthesized with any diameter from 1 to 200 nm to carry a payload of therapeutic molecules into a cell without triggering an immune response. Gold nanoparticles must undergo surface transformations before coupling to therapeutic molecules to become eligible for this purpose. It is now more understood that amine groups can bind to gold nanoparticles strongly, which has enabled surface modification of gold nanoparticles with amino acid lysine through its amine group. These lysine capped gold nanoparticles can further be coupled to therapeutic molecules for delivery purposes. In this study gold nanoparticles were first synthesized and capped with lysine molecules. TEM and FTIR measurements demonstrated the synthesis of lysine-capped gold nanoparticles with an average diameter of 10 nanometers. Interferon alpha molecules-one of the most important therapeutic protein were then chemically bound to lysine-capped gold nanoparticles through a two-step process of diimide-activated amidation. The conjugation of interferon molecules to lysine capped gold nanoparticles was carried out via the reaction between the free amine group of lysine and carboxyl groups of interferon using N-ethyl-N′-13-dimethyl-aminopropyl (EDAC) as a coupling agent. The process of conjugation has also been studied by transmission electron microscopy. 相似文献
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Yun‐Long Wu Jun Li Prof. Dr. 《Angewandte Chemie (International ed. in English)》2009,48(21):3842-3845
The CD ' s stuck : Poly(ethylene glycol) chains anchored onto gold nanoparticles (AuNPs) are threaded by multiple α‐cyclodextrin (α‐CD) rings to form a supramolecular outer layer composed of pseudopolyrotaxane columns perpendicular to the nanoparticle surface. Capping the polymer ends confines α‐CD on the nanoparticle surface, cross‐linking the α‐CD rings and then removing the AuNP cores produces supramolecular nanocapsules.