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1.
Dr. Rosaria Cercola Dr. Kaitlyn C. Fischer Summer L. Sherman Prof. Dr. Etienne Garand Natalie G. K. Wong L. Anders Hammerback Dr. Jason M. Lynam Prof. Dr. Ian J. S. Fairlamb Dr. Caroline E. H. Dessent 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(45):10297-10306
PhotoCORMs are light-triggered compounds that release CO for medical applications. Here, we apply laser spectroscopy in the gas phase to TryptoCORM, a known photoCORM that has been shown to destroy Escherichia coli upon visible-light activation. Our experiments allow us to map TryptoCORM's photochemistry across a wide wavelength range by using novel laser-interfaced mass spectrometry (LIMS). LIMS provides the intrinsic absorption spectrum of the photoCORM along with the production spectra of all of its ionic photoproducts for the first time. Importantly, the photoproduct spectra directly reveal the optimum wavelengths for maximizing CO ejection, and the extent to which CO ejection is compromised at redder wavelengths. A series of comparative studies were performed on TryptoCORM-CH3CN which exists in dynamic equilibrium with TryptoCORM in solution. Our measurements allow us to conclude that the presence of the labile CH3CN facilitates CO release over a wider wavelength range. This work demonstrates the potential of LIMS as a new methodology for assessing active agent release (e.g. CO, NO, H2S) from light-activated prodrugs. 相似文献
2.
《应用有机金属化学》2017,31(2)
Two new photoactivatable carbon monoxide‐releasing molecules (CORMs), fac ‐[Mn(CO)3(BZM)Br] ( 1 ) and [RuCl2(BZM)(CO)2] ( 2 ), derived from the anti‐anxiety drug bromazepam (BZM) and capable of rapid release of CO upon the illumination with light‐emitting diode (LED) source light (470–525 nm) have been synthesized and characterized. The photo‐delivery of CO to myoglobin solution could be achieved via the illumination of 1 at 525 nm for 10 min or at 470 nm for 1 min. The addition of water to a dimethylsulfoxide (DMSO) solution of 1 increases its stability, but it decreases the rate of the CO‐releasing process. CORM 2 behaves as a good visible photoCORM, whereby its two CO molecules are released within 10 min upon exposure to LED light source at 470 nm in DMSO. The illumination profile of 2 was also examined using solution infrared spectroscopy. The cis /trans stereochemistry around the Ru(II) ion was determined using quantum chemical calculations. The formation of photoCORMs leads to an improvement in the toxicity of BZM against tested microbes. 相似文献
3.
《Acta Crystallographica. Section C, Structural Chemistry》2017,73(4):357-361
PhotoCORMs (photo‐active CO‐releasing molecules) have emerged as a class of CO donors where the CO release process can be triggered upon illumination with light of appropriate wavelength. We have recently reported an Mn‐based photoCORM, namely [MnBr(pbt)(CO)3] [pbt is 2‐(pyridin‐2‐yl)‐1,3‐benzothiazole], where the CO release event can be tracked within cellular milieu by virtue of the emergence of strong blue fluorescence. In pursuit of developing more such trackable photoCORMs, we report herein the syntheses and structural characterization of two MnI–carbonyl complexes, namely fac‐tricarbonylchlorido[2‐(pyridin‐2‐yl)‐1,3‐benzothiazole‐κ2N ,N ′]manganese(I), [MnCl(C12H8N2S)(CO)3], (1), and fac‐tricarbonylchlorido[2‐(quinolin‐2‐yl)‐1,3‐benzothiazole‐κ2N ,N ′]manganese(I), [MnCl(C16H10N2S)(CO)3], (2). In both complexes, the MnI center resides in a distorted octahedral coordination environment. Weak intermolecular C—H…Cl contacts in complex (1) and Cl…S contacts in complex (2) consolidate their extended structures. These complexes also exhibit CO release upon exposure to low‐power broadband visible light. The apparent CO release rates for the two complexes have been measured to compare their CO donating capacity. The fluorogenic 2‐(pyridin‐2‐yl)‐1,3‐benzothiazole and 2‐(quinolin‐2‐yl)‐1,3‐benzothiazole ligands provide a convenient way to track the CO release event through the `turn‐ON' fluorescence which results upon de‐ligation of the ligands from their respective metal centers following CO photorelease. 相似文献
4.
Dr. Mengfei Wang Dr. Kei Murata Yosuke Koike Dr. Gediminas Jonusauskas Dr. Amaury Furet Prof. Dario M. Bassani Daisuke Saito Prof. Masako Kato Yuushi Shimoda Dr. Kiyoshi Miyata Prof. Ken Onda Prof. Kazuyuki Ishii 《Chemistry (Weinheim an der Bergstrasse, Germany)》2022,28(48):e202200716
A complex comprising one [Re(CO)3]+ unit and a phthalocyanine (Pc) ligand ( Re1Pc ) is shown to function as a photo-induced CO-releasing molecule (photoCORM) in the presence of O2 and a coordinative solvent under irradiation with red light, which can deeply penetrate living tissues. Transient absorption spectroscopic measurements indicate very short excited-state lifetimes and ultrafast intersystem crossing for Re1Pc and Re2Pc , which contains two [Re(CO)3]+ units. The excited-state properties are ascribed to efficient spin–orbit coupling and large Franck–Condon factors originating from the complexes’ distorted structures, that is, unsymmetric coordination of [Re(CO)3]+ unit(s), one of which was confirmed by single-crystal X-ray analysis of a symmetrically substituted Pc with two [Re(CO)3]+ units. Re1Pc represents a promising red-light-driven photoCORM that can be applied in biological environments or therapeutic applications. 相似文献
5.
The use of Carbon Monoxide (CO) as a therapeutic agent has already been tested in human clinical trials. Pre-clinically, CO gas administration proved beneficial in animal models of various human diseases. However, the use of gaseous CO faces serious obstacles not the least being its well-known toxicity. To fully realise the promise of CO as a therapeutic agent, it is key to find novel avenues for CO delivery to diseased tissues in need of treatment, without concomitant formation of elevated, toxic blood levels of carboxyhemoglobin (COHb). CO-releasing molecules (CO-RMs) have the potential to constitute safe treatments if CO release in vivo can be controlled in a spatial and temporal manner. It has already been demonstrated in animals that CO-RMs can release CO and mimic the therapeutic effects of gaseous CO. While demonstrating the principle of treatment with CO-RMs, these first generation compounds are not suitable for human use. This tutorial review summarises the biological and chemical behaviour of CO, the current status of CO-RM development, and derives principles for the creation of the next generation of CO-RMs for clinical applications in humans. 相似文献
6.
《Acta Crystallographica. Section C, Structural Chemistry》2017,73(11):923-929
Carbon monoxide (CO) has recently been identified as a gaseous signaling molecule that exerts various salutary effects in mammalian pathophysiology. Photoactive metal carbonyl complexes (photoCORMs) are ideal exogenous candidates for more controllable and site‐specific CO delivery compared to gaseous CO. Along this line, our group has been engaged for the past few years in developing group‐7‐based photoCORMs towards the efficient eradication of various malignant cells. Moreover, several such complexes can be tracked within cancerous cells by virtue of their luminescence. The inherent luminecscent nature of some photoCORMs and the change in emission wavelength upon CO release also provide a covenient means to track the entry of the prodrug and, in some cases, both the entry and CO release from the prodrug. In continuation of the research circumscribing the development of trackable photoCORMs and also to graft such molecules covalently to conventional delivery vehicles, we report herein the synthesis and structures of three rhenium carbonyl complexes, namely, fac‐tricarbonyl[2‐(pyridin‐2‐yl)‐1,3‐benzothiazole‐κ2N ,N ′](4‐vinylpyridine‐κN )rhenium(I) trifluoromethanesulfonate, [Re(C7H7N)(C12H8N2S)(CO)3](CF3SO3), ( 1 ), fac‐tricarbonyl[2‐(quinolin‐2‐yl)‐1,3‐benzothiazole‐κ2N ,N ′](4‐vinylpyridine‐κN )rhenium(I) trifluoromethanesulfonate, [Re(C7H7N)(C16H10N2S)(CO)3](CF3SO3), ( 2 ), and fac‐tricarbonyl[1,10‐phenanthroline‐κ2N ,N ′](4‐vinylpyridine‐κN )rhenium(I) trifluoromethanesulfonate, [Re(C7H7N)(C12H8N2)(CO)3](CF3SO3), ( 3 ). In all three complexes, the ReI center resides in a distorted octahedral coordination environment. These complexes exhibit CO release upon exposure to low‐power UV light. The apparent CO release rates of the complexes have been measured to assess their comparative CO‐donating capacity. The three complexes are highly luminescent and this in turn provides a convenient way to track the entry of the prodrug molecules within biological targets. 相似文献
7.
利用五羰基溴化锰和2-吡啶甲醛以及卤代苯胺通过一步法合成得到了3个含席夫碱配体的锰羰基配合物[Mn(CO)3(py(CH=N)ph-X)Br],其中X=Cl (1)、Br (2)、I (3),并采用核磁、X射线单晶衍射、红外光谱、紫外可见光谱和荧光光谱对其进行了表征。这类配合物在非光照下稳定,在可见光(LED蓝光、绿光和红光)作用下分解释放CO,可以作为光诱导的一氧化碳释放剂(photoCORMs)。研究表明蓝光是促进配合物分解释放CO的最有效光源。此外,CO释放动力学分析显示配合物分解释放CO过程符合一级动力学模型。配合物3的释放研究表明脱氧肌红蛋白能够捕捉所释放的CO。尽管这些配合物本身的细胞毒性(IC50)达到微摩尔级,但光照下的细胞兼容性有显著改善,上升为接近100微摩尔级。这些配合物具有荧光性质,在450 nm激发波长下在500~700 nm范围内发射一定强度的荧光,可以作为荧光标记物用以监测细胞或生物体内释放剂分布及CO释放情况。 相似文献
8.
Fabiola Vieira de Carvalho Ligia Nunes de Morais Ribeiro Ludmilla David de Moura Gustavo Henrique Rodrigues da Silva Hery Mitsutake Talita Cesarim Mendona Gabriela Geronimo Marcia Cristina Breitkreitz Eneida de Paula 《Molecules (Basel, Switzerland)》2022,27(24)
Breast cancer is the neoplasia of highest incidence in women worldwide. Docetaxel (DTX), a taxoid used to treat breast cancer, is a BCS-class-IV compound (low oral bioavailability, solubility and intestinal permeability). Nanotechnological strategies can improve chemotherapy effectiveness by promoting sustained release and reducing systemic toxicity. Nanostructured lipid carriers (NLC) encapsulate hydrophobic drugs in their blend-of-lipids matrix, and imperfections prevent drug expulsion during storage. This work describes the preparation, by design of experiments (23 factorial design) of a novel NLC formulation containing copaiba oil (CO) as a functional excipient. The optimized formulation (NLCDTX) showed approximately 100% DTX encapsulation efficiency and was characterized by different techniques (DLS, NTA, TEM/FE-SEM, DSC and XRD) and was stable for 12 months of storage, at 25 °C. Incorporation into the NLC prolonged drug release for 54 h, compared to commercial DTX (10 h). In vitro cytotoxicity tests revealed the antiproliferative effect of CO and NLCDTX, by reducing the cell viability of breast cancer (4T1/MCF-7) and healthy (NIH-3T3) cells more than commercial DTX. NLCDTX thus emerges as a promising drug delivery system of remarkable anticancer effect, (strengthened by CO) and sustained release that, in clinics, may decrease systemic toxicity at lower DTX doses. 相似文献
9.
Visible‐Light‐Induced CO Release from a Therapeutically Viable Tryptophan‐Derived Manganese(I) Carbonyl (TryptoCORM) Exhibiting Potent Inhibition against E. coli
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Jonathan S. Ward Dr. Jason M. Lynam Dr. James Moir Prof. Ian J. S. Fairlamb 《Chemistry (Weinheim an der Bergstrasse, Germany)》2014,20(46):15061-15068
The first visible‐light‐activated carbon‐monoxide‐releasing molecule (CO‐RM) to exhibit a potent effect against Escherichia coli is described. The easily prepared tryptophan‐derived manganese‐containing complex (TryptoCORM) released 1.4 moles of CO at 465 nm, and 2 moles at 400 nm. A comprehensive synthetic, mechanistic and microbiological study into the behaviour of TryptoCORM is reported. The complex is thermally stable (i.e., does not release CO in solution in the absence of light), shows low toxicity against mammalian cells and releases tryptophan on photoinduced degradation, all of which point to TryptoCORM being therapeutically viable. 相似文献
10.
Dr. Lenka Štacková Marina Russo Dr. Lucie Muchová Vojtěch Orel Prof. Libor Vítek Dr. Peter Štacko Prof. Petr Klán 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(58):13184-13190
Carbon monoxide (CO) is an endogenous signaling molecule that controls a number of physiological processes. To circumvent the inherent toxicity of CO, light-activated CO-releasing molecules (photoCORMs) have emerged as an alternative for its administration. However, their wider application requires photoactivation using biologically benign visible and near-infrared (NIR) light. In this work, a strategy to access such photoCORMs by fusing two CO-releasing flavonol moieties with a NIR-absorbing cyanine dye is presented. These hybrids liberate two molecules of CO in high chemical yields upon activation with NIR light up to 820 nm and exhibit excellent uncaging cross-sections, which surpass the state-of-the-art by two orders of magnitude. Furthermore, the biocompatibility and applicability of the system in vitro and in vivo are demonstrated, and a mechanism of CO release is proposed. It is hoped that this strategy will stimulate the discovery of new classes of photoCORMs and accelerate the translation of CO-based phototherapy into practice. 相似文献
11.
Elvan Üstün Aykut Özgür Kübra A. Coşkun Serpil Demir İsmail Özdemir Yusuf Tutar 《Journal of Coordination Chemistry》2016,69(22):3384-3394
Carbon monoxide (CO) is an important signaling molecule which plays significant roles in the pathogenesis of cancer. CO is produced by enzymatic degradation of heme in mammals. Heme oxygenase 1 (HO-1) catalyzes the breakdown of heme into CO, ferrous iron, and biliverdin. CO induces HO-1 and inhibits cell proliferation. Cancer cells exposed to several stress factors (hypoxia, reactive oxygen species, cis-platin, and oxidative stress), and HO-1 displays cytoprotective role against oxidative stress and inhibits apoptosis, metastases, angiogenesis, and cell proliferation processes. Therefore, metal containing CO-releasing molecules (CORMs) have been designed as an effective cancer treatment strategy. CORMs are responsible for releasing controlled amounts of CO to cells and tissues. Thus, we synthesized [Mn(CO)3(bpy)L]X manganese containing CORMs [bpy = 2,2′-bipyridine, X = hexafluorophosphate (PF6), trifluoromethanesulfonate (OTf), L = imidazole, methylimidazole, benzimidazole, N-benzylbenzimidazole, N-(4-chlorobenzyl)benzimidazole] to release CO in human invasive ductal breast (MCF-7) cell line. In vitro experiments indicated that the compounds inhibited cell proliferation and exhibited cytotoxic effect on breast cancer cells. Moreover, side groups of the compounds enhanced the anticancer effects in MCF-7 cell line. These manganese containing CORMs gave promising results and may be used as a drug template for effective treatment of invasive ductal breast carcinoma. 相似文献
12.
Baoqing Liu Wenzhi Yang Chengchuan Che Jinfeng Liu Meiru Si Zhijin Gong Ruixia Gao Prof. Ge Yang 《ChemistryOpen》2021,10(4):408-413
A novel method for the preparation of antitumor drug vehicles has been optimized. Biological materials of chitosan oligosaccharide (CO) and γ-polyglutamic acid (γ-PGA) have previously been employed as modifiers to covalently modify graphene oxide (GO), which in turn loaded doxorubicin (DOX) to obtain a nano drug delivery systems of graphene oxide based composites (GO-CO-γ-PGA-DOX). The system was not equipped with the ability of initiative targeting, thus resulting into toxicity and side effects on normal tissues or organs. In order to further improve the targeting property of the system, the nucleic acid aptamer NH2-AS1411 (APT) of targeted nucleolin (C23) was used to conjugate on GO-CO-γ-PGA to yield the targeted nano drug delivery system APT-GO-CO-γ-PGA. The structure, composition, dispersion, particle size and morphology properties of the synthesized complex have been studied using multiple characterization methods. Drug loading and release profile data showed that APT-GO-CO-γ-PGA is provided with high drug loading capacity and is capable of controlled and sustained release of DOX. Cell experimental results indicated that since C23 was overexpressed on the surface of Hela cells but not on the surface of Beas-2B cells, APT-GO-CO-γ-PGA-DOX can target Hela cells and make increase toxicity to Hela cells than Beas-2B cells, and the IC50 value of APT-GO-CO-γ-PGA-DOX was 3.23±0.04 μg/mL. All results proved that APT-GO-CO-γ-PGA can deliver antitumor drugs in a targeted manner, and achieve the effect of reducing poison, which indicated that the targeted carrier exhibits a broad application prospect in the field of biomedicine. 相似文献
13.
Anticancer Potencies of PtII‐ and PdII‐linked M2L4 Coordination Capsules with Improved Selectivity
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Dr. Anife Ahmedova Dr. Denitsa Momekova Masahiro Yamashina Dr. Pavletta Shestakova Prof. Dr. Georgi Momekov Prof. Dr. Munetaka Akita Dr. Michito Yoshizawa 《化学:亚洲杂志》2016,11(4):474-477
PtII‐ and PdII‐linked M2L4 coordination capsules, providing a confined cavity encircled by polyaromatic frameworks, exhibit anticancer activities superior to cisplatin against two types of leukemic cells (HL‐60 and SKW‐3) and pronounced toxicity against cisplatin‐resistant cells (HL‐60/CDDP). Notably, the cytotoxic selectivities of the PtII and PdII capsules toward cancerous cells are up to 5.3‐fold higher than that of cisplatin, as estimated through the non‐malignant/malignant‐cells toxicity ratio employing normal kidney cells (HEK‐293). In addition, the anticancer activity of the coordination capsules can be easily altered upon encapsulation of organic guest molecules. 相似文献
14.
Xiaoming Ma Dr. Yongli Shen Dr. Shuang Yao Miao Shu Prof. Rui Si Prof. Changhua An 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(18):4143-4149
The key to the electrochemical conversion of CO2 lies in the development of efficient electrocatalysts with ease of operation, good conductivity, and rich active sites that fulfil the desired reaction direction and selectivity. Herein, an oxidative etching of Au20Cu80 alloy is used for the synthesis of a nanoporous Au3Cu alloy, representing a facile strategy for tuning the surface electronic properties and altering the adsorption behavior of the intermediates. HRTEM, XPS, and EXAFS results reveal that the curved surface of the synthesized nanoporous Au3Cu is rich in gold with unsaturated coordination conditions. It can be used directly as a self-supported electrode for CO2 reduction, and exhibits high Faradaic efficiency (FE) of 98.12 % toward CO at a potential of −0.7 V versus the reversible hydrogen electrode (RHE). The FE is 1.47 times that over the as-made single nanoporous Au. Density functional theory reveals that *CO has a relatively long distance on the surface of nanoporous Au3Cu, making desorption of CO easier and avoiding CO poisoning. The Hirshfeld charge distribution shows that the Au atoms have a negative charge and the Cu atoms exhibit a positive charge, which separately bond to the C atom and O atom in the *COOH intermediate through a bidentate mode. This affords the lowest *COOH adsorption free energy and low desorption energy for CO molecules. 相似文献
15.
A site‐selective controlled delivery system for controlled drug release is fabricated through the in situ assembly of stimuli‐responsive ordered SBA‐15 and magnetic particles. This approach is based on the formation of ordered mesoporous silica with magnetic particles formed from Fe(CO)5 via the surfactant‐template sol‐gel method and control of transport through polymerization of N‐isopropyl acrylamide inside the pores. Hydrophobic Fe(CO)5 acts as a swelling agent as well as being the source of the magnetic particles. The obtained system demonstrates a high pore diameter (7.1 nm) and pore volume (0.41 cm3 g?1), which improves drug storage for relatively large molecules. Controlled drug release through the porous network is demonstrated by measuring the uptake and release of ibuprofen (IBU). The delivery system displays a high IBU storage capacity of 71.5 wt %, which is almost twice as large as the highest value based on SBA‐15 ever reported. In vitro testing of IBU loading and release exhibits a pronounced transition at around 32 °C, indicating a typical thermosensitive controlled release. 相似文献
16.
Lars Hemmersbach Yannick Schreiner Xinmiao Zhang Finn Dicke Leon Hünemeyer Dr. Jörg-Martin Neudörfl Dr. Thomas Fleming Prof. Dr. Benito Yard Prof. Dr. Hans-Günther Schmalz 《Chemistry (Weinheim an der Bergstrasse, Germany)》2022,28(50):e202201670
Due to the beneficial effects of carbon monoxide as a cell-protective and anti-inflammatory agent, CO-releasing molecules (CORMs) offer some promising potential applications in medicine. In this context, we synthesized a set of acyloxy-cyclohexadiene-Fe(CO)3 complexes, all displaying a N-methyl-pyridinium triflate moiety in the ester side chain, as mitochondria-targeting esterase-triggered CORM prodrugs. Whereas the compounds in which the acyloxy substituent is attached to the 2-position of the diene-Fe(CO)3 unit (A series) spontaneously release CO upon dissolution in phosphate buffer, which remarkably is partly suppressed in the presence of porcine liver esterase (PLE), the 1-substituted isomers (B series) show the expected PLE-induced release of CO (up to 3 equiv.). The biological activity of Mito-CORMs 2 / 3 - B and their isophorone-derived analogs 2/3 - A ’, which also displayed PLE-induced CO release, was assessed by using human umbilical vein endothelial cells (HUVEC). Whereas Mito-CORMs 2/3 - B were not cytotoxic up to 500 μM (MTT assay), Mito-CORMs 2 / 3 - A ’ caused significant toxicity at concentrations above 50 μM. The anti-inflammatory potential of both Mito-CORM variants was demonstrated by concentration-dependent down-regulation of the pro-inflammatory markers VCAM-1, ICAM-1 and CXCL1 as well as induction of HO-1 in TNFα-stimulated human umbilical vein endothelial cells (HUVECs; western blotting and qPCR). Energy phenotyping by seahorse real-time cell metabolic analysis, revealed opposing shifts of metabolic potentials in cells treated either with Mito-CORMs 2/3 - B (increased mitochondrial respiration and glycolytic activity) or Mito-CORMs 2/3 - A ’ (suppressed mitochondrial respiration and increased glycolytic activity). Thus, the Mito-CORMs represent valuable tools for the safe and targeted delivery of CO to mitochondria as a subcellular compartment to induce positive anti-inflammatory effects with only minor shifts in cellular energy metabolism. Also, due to their water solubility, these compounds provide a promising starting point for further pharmacological studies. 相似文献
17.
本文设计合成了一系列具有共轭结构的二茂铁咪唑衍生物,它们在质子的作用下呈现显著的光谱、核磁及电化学响应.在中性(或碱性)环境中,其氧化还原波处于低电位,表现为分子"关"的状态;在酸性环境中,其氧化还原波处于高电位,表现为分子"开"的状态;通过酸碱的调控作用其氧化还原波可以在高、低电位之间可逆转换,能够作为一类新型的电化... 相似文献
18.
Miguel Chaves‐Ferreira Inês S. Albuquerque Dijana Matak‐Vinkovic Ana C. Coelho Sandra M. Carvalho Lígia M. Saraiva Carlos C. Romo Gonalo J. L. Bernardes 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2015,127(4):1188-1191
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
19.
利用五羰基溴化锰和2-吡啶甲醛以及卤代苯胺通过一步法合成得到了3个含席夫碱配体的锰羰基配合物[Mn (CO)3(py (CH=N) ph-X) Br],其中X=Cl (1)、Br (2)、I (3),并采用核磁、X射线单晶衍射、红外光谱、紫外可见光谱和荧光光谱对其进行了表征。这类配合物在非光照下稳定,在可见光(LED蓝光、绿光和红光)作用下分解释放CO,可以作为光诱导的一氧化碳释放剂(photoCORMs)。研究表明蓝光是促进配合物分解释放CO的最有效光源。此外,CO释放动力学分析显示配合物分解释放CO过程符合一级动力学模型。配合物3的释放研究表明脱氧肌红蛋白能够捕捉所释放的CO。尽管这些配合物本身的细胞毒性(IC50)达到微摩尔级,但光照下的细胞兼容性有显著改善,上升为接近100微摩尔级。这些配合物具有荧光性质,在450 nm激发波长下在500~700 nm范围内发射一定强度的荧光,可以作为荧光标记物用以监测细胞或生物体内释放剂分布及CO释放情况。 相似文献
20.
Dr. Xiao‐Na Li Dr. Zi‐Yu Li Hai‐Fang Li Prof. Dr. Sheng‐Gui He 《Chemistry (Weinheim an der Bergstrasse, Germany)》2016,22(26):9024-9029
Time‐of‐flight mass spectrometry experiments demonstrated that laser ablation generated and mass selected Au2TiO4? cluster anions can unexpectedly oxidize three CO molecules in an ion trap reactor. This is an improvement on the more commonly observed oxidation of at most two CO molecules by a doped cluster. Quantum chemistry calculations were performed to rationalize the reactions. The lowest energy isomer of Au2TiO4? contains a superoxide unit, the participation of which in CO oxidation can be promoted by the Au2 dimer. The Au2 dimer functions as a rather flexible electron reservoir in each CO oxidation step in terms of the release and storage of electrons to drive the dissociation of superoxide to peroxide and then to lattice oxygen atoms, which can be removed by reaction with CO molecules. This gas‐phase study enriches our understanding toward the nature of reactive oxygen species involved in gold‐catalyzed oxidation reactions. 相似文献