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1-Iodoglycal: A Versatile Intermediate for the Synthesis of d-Glyco Amides and Esters Employing Carbonylative Cross-Coupling Reaction 1-Iodoglycal:利用羰基交叉偶联反应合成 d-甘氨酰酰胺和酯的多功能中间体
IF 4.1 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-11 DOI: 10.1021/acsomega.4c02645
Milene M. Hornink, Monica F. Z. J. Toledo, Daniel C. Pimenta, Caio Paschoalin, Pamela M. Silva, Giuseppe E. Figlino, Eurípedes Aguiar, Gustavo Cervi, Francisco W. M. Ribeiro, Thiago Carita Correra, Angélique Ferry, Hélio A. Stefani
In this study, we present the development of two catalytic processes: a Pd-PEPPSI-catalyzed aminocarbonylation and a Pd(OAc)2-Xantphos-catalyzed alkoxycarbonylation of d-glycals, utilizing carbonylative cross-coupling reactions. We explored successfully various types of aromatic amines, as well as alkyl amines and amino acids, to synthesize new d-glycal amides. However, we observed limitations in the reactivity of alkyl and heteroaromatic amines. The processes enabled the synthesis of 20 novel C1-branched glycoamides and 7 new d-gluco esters.
在本研究中,我们利用羰基化交叉偶联反应,开发了两种催化过程:Pd-PEPPSI 催化的氨基羰基化和 Pd(OAc)2-Xantphos 催化的 d-甘氨醛烷氧基羰基化。我们成功地探索了各种类型的芳香胺以及烷基胺和氨基酸来合成新的 d-甘氨酰酰胺。然而,我们发现烷基胺和杂芳香胺的反应能力有限。通过这些工艺,我们合成了 20 种新型 C1 支链糖酰胺和 7 种新型 d-糖酯。
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引用次数: 0
ToxTeller: Predicting Peptide Toxicity Using Four Different Machine Learning Approaches ToxTeller:使用四种不同的机器学习方法预测多肽毒性
IF 4.1 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-11 DOI: 10.1021/acsomega.4c04246
Jen-Hung Wang, Ting-Yi Sung
Examining the toxicity of peptides is essential for therapeutic peptide-based drug design. Machine learning approaches are frequently used to develop highly accurate predictors for peptide toxicity prediction. In this paper, we present ToxTeller, which provides four predictors using logistic regression, support vector machines, random forests, and XGBoost, respectively. For prediction model development, we construct a data set of toxic and nontoxic peptides from SwissProt and ConoServer databases with existence evidence levels checked. We also fully utilize the protein annotation in SwissProt to collect more toxic peptides than using keyword search alone. From this data set, we construct an independent test data set that shares at most 40% sequence similarity within itself and with the training data set. From a quite comprehensive list of 28 feature combinations, we conduct 10-fold cross-validation on the training data set to determine the optimized feature combination for model development. ToxTeller’s performance is evaluated and compared with existing predictors on the independent test data set. Since toxic peptides must be avoided for drug design, we analyze strategies for reducing false-negative predictions of toxic peptides and suggest selecting models by top sensitivity instead of the widely used Matthews correlation coefficient, and also suggest using a meta-predictor approach with multiple predictors.
研究多肽的毒性对于基于多肽的治疗药物设计至关重要。机器学习方法常用于开发高精度的多肽毒性预测器。本文介绍了 ToxTeller,它提供了四种预测方法,分别使用逻辑回归、支持向量机、随机森林和 XGBoost。为了开发预测模型,我们从 SwissProt 和 ConoServer 数据库中构建了一个有毒和无毒多肽数据集,并检查了存在的证据级别。我们还充分利用了 SwissProt 中的蛋白质注释,从而收集到比单独使用关键词搜索更多的有毒肽。我们从这一数据集中构建了一个独立的测试数据集,该数据集与训练数据集的序列相似度不超过 40%。从 28 种特征组合的相当全面的列表中,我们对训练数据集进行了 10 倍交叉验证,以确定用于模型开发的优化特征组合。我们对 ToxTeller 的性能进行了评估,并在独立测试数据集上与现有预测器进行了比较。由于药物设计必须避免有毒多肽,我们分析了减少有毒多肽假阴性预测的策略,建议通过最高灵敏度而不是广泛使用的马修斯相关系数来选择模型,还建议使用具有多个预测因子的元预测方法。
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引用次数: 0
Exploring the Fibrous Nature of Single-Stranded DNA–Collagen Complexes: Nanostructural Observations and Physicochemical Insights 探索单链 DNA-胶原复合物的纤维性质:纳米结构观察与物理化学见解
IF 4.1 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-11 DOI: 10.1021/acsomega.4c04104
Nikolaos Pipis, Kevin A. Stewart, Mohammad Tabatabaei, Lakiesha N. Williams, Josephine B. Allen
Nucleic acid–collagen complexes (NACCs) are a self-assembled biomimetic fibrillary platform arising from the spontaneous complexation of single-stranded DNA (ssDNA) oligonucleotides and collagen. NACCs merge the extracellular matrix functionality of collagen with the tunable bioactivity of ssDNA as aptamers for broad biomedical applications. We hypothesize that NACCs offer a hierarchical architecture across multiple length scales that significantly varies compared to native collagen. We investigate this using atomic force microscopy and electron microscopy (transmission electron microscopy and cryogenic electron microscopy). Results demonstrate key topographical differences induced by adding ssDNA oligonucleotides to collagen type I. NACCs form a dense network of intertwined collagen fiber bundles in the microscale and nanoscale while retaining their characteristic D-band periodicities (∼67 nm). Additionally, our exploration of thermodynamic parameters governing the interaction indicates an entropically favorable NACC formation driven by ssDNA. Thermal analysis demonstrates the preservation of collagen’s triple helical domains and a more stabilized polypeptide structure at higher temperatures than native collagen. These findings offer important insights into our understanding of the ssDNA-induced complexation of collagen toward the further establishment of structure–property relationships in NACCs and their future development into practical biomaterials. They also provide pathways for manipulating and enhancing collagenous matrices’ properties without requiring complex chemical modifications or fabrication procedures.
核酸-胶原复合物(NACCs)是单链 DNA(ssDNA)寡核苷酸与胶原自发复合而成的一种自组装仿生纤维状平台。NACC 融合了胶原蛋白的细胞外基质功能和 ssDNA 的可调生物活性,可作为广泛生物医学应用的适配体。我们推测 NACCs 具有跨越多个长度尺度的分层结构,与原生胶原相比具有显著差异。我们使用原子力显微镜和电子显微镜(透射电子显微镜和低温电子显微镜)对此进行了研究。结果表明,在 I 型胶原蛋白中添加 ssDNA 寡核苷酸会诱发关键的地形差异。NACCs 在微观和纳米尺度上形成了胶原纤维束交织的密集网络,同时保留了其特有的 D 波段周期性(∼67 nm)。此外,我们对控制相互作用的热力学参数的研究表明,ssDNA 的驱动有利于 NACC 的形成。热分析表明,在比原生胶原蛋白更高的温度下,胶原蛋白的三重螺旋结构域和更稳定的多肽结构得以保留。这些发现为我们了解 ssDNA 诱导的胶原蛋白复合物提供了重要见解,有助于进一步建立 NACC 的结构-性能关系,并在未来将其开发成实用的生物材料。这些发现还为操纵和增强胶原蛋白基质的特性提供了途径,而无需复杂的化学修饰或制造程序。
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引用次数: 0
Synthesis of Cyclodextrin-Based Multifunctional Biocompatible Hydrogels and Their Use in the Prevention of Intrauterine Adhesions (Asherman’s Syndrome) after Surgical Injury 基于环糊精的多功能生物相容性水凝胶的合成及其在预防手术损伤后子宫内粘连(阿舍曼综合征)中的应用
IF 4.1 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-11 DOI: 10.1021/acsomega.4c03655
Busra Aksoy Erden, Meltem Kurus, Ilgin Turkcuoglu, Rauf Melekoglu, Sevgi Balcioglu, Birgul Yigitcan, Burhan Ates, Suleyman Koytepe
Asherman’s syndrome, which can occur during the regeneration of damaged uterine tissue after surgical interventions, is a significant health problem in women. This study aimed to acquire and characterize cyclodextrin-based hydrogels, which can be used to prevent Asherman’s syndrome, and investigate their effectiveness with biomedical applications. A series of hydrogels were synthesized from the cross-linking of β-cyclodextrin and different polyphenols with epoxy-functional PEG. Their chemical, physical, and biological properties were subsequently determined. The results demonstrated that the cyclodextrin-based hydrogels had a porous structure, high swelling ratio, good injectability, drug release ability, and antioxidant activity. Cell culture results illustrated that the hydrogels had no significant cytotoxicity toward L929 fibroblast cells. Considering all properties, the β-CD-PEG-600-Ec hydrogel showed the most satisfactory properties rather than other ones. The potential of this hydrogel in preventing Asherman’s syndrome was evaluated in a rat model. The results revealed that the β-estradiol- and melatonin-loaded cyclodextrin-based multifunctional hydrogel group both structurally and mechanically showed an antiadhesion effect in the uterus and a therapeutic effect on the damage with the β-estradiol and melatonin that it contains compared to the Asherman (ASH) group. This double drug-loaded hydrogel can be a promising candidate for preventing Asherman’s syndrome due to its versatile properties.
阿舍曼氏综合征可能发生在手术治疗后受损子宫组织的再生过程中,是妇女的一个重大健康问题。本研究旨在获得可用于预防阿舍曼氏综合征的环糊精基水凝胶,并对其生物医学应用的有效性进行研究。一系列水凝胶是由β-环糊精和不同的多酚与环氧官能团 PEG 交联合成的。随后测定了它们的化学、物理和生物特性。结果表明,环糊精水凝胶具有多孔结构、高溶胀率、良好的注射性、药物释放能力和抗氧化活性。细胞培养结果表明,水凝胶对 L929 成纤维细胞没有明显的细胞毒性。考虑到所有特性,β-CD-PEG-600-Ec 水凝胶比其他水凝胶表现出最令人满意的特性。在大鼠模型中评估了这种水凝胶在预防阿什曼氏综合症方面的潜力。结果显示,与阿舍曼(ASH)组相比,β-雌二醇和褪黑素载药的环糊精基多功能水凝胶组在结构和机械方面都显示出抗子宫粘连的效果,而且它所含的β-雌二醇和褪黑素对损伤有治疗作用。这种双重载药水凝胶因其多功能特性,有望成为预防阿舍曼氏综合征的候选药物。
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引用次数: 0
The Electrical and Photodetector Characteristics of the Graphene:PVA/p-Si Schottky Structures Depending on Illumination Intensities 石墨烯:PVA/p-Si 肖特基结构的电学和光电探测器特性取决于照明强度
IF 4.1 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-11 DOI: 10.1021/acsomega.4c05219
Murat Ulusoy, Serhat Koçyiğit, Adem Tataroğlu, S. Altındal Yerişkin
Five samples were fabricated to obtain a diode with a PVA interface, both with and without graphene doping at different rates with high rectification in the dark. The electrospinning method was employed to apply the doped and undoped solutions, creating the interlayers. Since the diode with a 1 wt % graphene-doped PVA interlayer outperformed the other samples, the main electrical and photodetector characteristics of this structure were investigated. The electrical parameters of the diode were probed by the TE, Norde, and Cheung methods, and the parameters (n and ϕB) acquired by both approaches were significantly influenced by illumination and voltages. The interface/surface state intensity values (Nss) were also calculated in the dark and under each illumination as a function of the band/energy gap depth (EssEv). The time-dependent steady-state conditions and rise-decay behavior of the photocurrents during illumination were also investigated. Due to the high photocurrent values, the photosensitivity at zero bias is approximately 1.4 × 104 at 100 mW cm–2. The responsivity and detectivity values appear to be altered significantly with changes in the illumination and voltage. Additionally, a double logarithmic plot of Iph vs P reveals good linearity with slope values ranging from 0.5 to 1.
我们制作了五个样品,以获得具有 PVA 接口的二极管,其中既有掺杂石墨烯的,也有未掺杂石墨烯的,掺杂率各不相同,在黑暗中具有较高的整流性。采用电纺丝方法应用掺杂和未掺杂溶液,形成夹层。由于掺杂了 1 wt % 石墨烯的 PVA 夹层二极管的性能优于其他样品,因此研究了这种结构的主要电气和光电探测器特性。采用 TE、Norde 和 Cheung 方法探测了二极管的电学参数,这两种方法获得的参数(n 和 ϕB)受光照和电压的影响很大。此外,还计算了暗态和各种光照下的界面/表面态强度值(Nss)与能带/能隙深度(Ess-Ev)的函数关系。此外,还研究了照明期间光电流随时间变化的稳态条件和上升-衰减行为。由于光电流值较高,在 100 mW cm-2 时,零偏压下的光灵敏度约为 1.4 × 104。随着光照度和电压的变化,响应度和检测度值似乎会发生显著变化。此外,Iph 与 P 的双对数图显示出良好的线性关系,斜率值在 0.5 到 1 之间。
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引用次数: 0
Investigation of Unresolved Interface “Rag Layer” in Athabasca Oil Sand Bitumen In Situ Recovery 阿萨巴斯卡油砂沥青原位采收中未解决的界面 "抹布层 "调查
IF 4.1 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-11 DOI: 10.1021/acsomega.4c04946
Evgeniya Hristova, Stanislav R. Stoyanov, Richard McFarlane, Kasra Nikooyeh
Steam-assisted gravity drainage (SAGD), the leading commercial in situ bitumen recovery process, involves the underground injection of steam and produces at the well head a hot fluid containing water, hydrocarbons, and sand. This fluid is subjected to separation by diluent addition and gravity in several parallel treaters. Occasionally, the separation may be disrupted in one or few treaters by the occurrence of an unresolved interface or “rag layer” while continuing without disruption in the rest of the treaters. In the current study, we investigate “rag layer” occurrence based on the quantification of laboratory-scale and SAGD field tests and imaging of the “rag layer” morphology. The quantification results show that the formation and volume of the “rag layer” are affected by solids, mixing speed, and solvent addition. The microscopic images demonstrate the presence of both water-in-oil or oil-in water emulsions with a distinct transition between the continuous phases. The visual detection boundaries of the “rag layer” are defined as the threshold between the agglomerated and individual droplet layers. The extent of agglomeration increases in the proximity to the oil–water interface. The contribution of hydrophobic fine inorganic solids (less than 10 μm) to forming a “rag layer” is supported by their accumulation observed at the treaters’ oil–water interface, compared to the feed. In well-controlled field operations, the perceived randomness of “rag layer” occurrence could be associated with the fluctuation of fine solid contents in the feed.
蒸汽辅助重力泄油(SAGD)是一种主要的商业原地沥青回收工艺,包括向地下注入蒸汽,并在井口产生含有水、碳氢化合物和沙子的热流体。这种流体在几个平行的处理机中通过添加稀释剂和重力作用进行分离。有时,在一个或几个处理池中,分离过程会因出现未解决的界面或 "碎布层 "而中断,而在其他处理池中则不会中断。在本研究中,我们根据实验室规模和 SAGD 现场测试的量化结果以及 "碎布层 "形态的成像,对 "碎布层 "的出现进行了研究。量化结果表明,"碎布层 "的形成和体积受固体、混合速度和溶剂添加量的影响。显微图像显示存在油包水型或水包油型乳液,连续相之间有明显的过渡。抹布层 "的视觉检测边界被定义为团聚层和单个液滴层之间的临界点。越靠近油水界面,团聚程度越高。疏水性细小无机固体(小于 10 μm)对形成 "碎布层 "的作用,可以从与进料相比,它们在处理剂油水界面上的累积情况中得到证实。在控制良好的现场操作中,"碎布层 "出现的随机性可能与进料中细固体含量的波动有关。
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引用次数: 0
Experimental and Computational Anticorrosion Behaviors of Pyrazole s-Triazine/anilino-morpholino Derivatives for Steel in Acidic Solutions 吡唑 s-三嗪/苯胺基吗啉基衍生物在酸性溶液中对钢的实验和计算防腐行为
IF 4.1 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-11 DOI: 10.1021/acsomega.4c02569
Hassan H. Hammud, Waleed A. Aljamhi, Ihab Shawish, Nur Hazimah B. Z Arfan, Malai Haniti S. A. Hamid, Nadeem S. Sheikh, Hany M. Abd El-Lateef, Assem Barakat, Ayman El-Faham
The corrosion inhibition of C-steel by two s-triazine/morpholino-anilino-pyrazole derivatives, namely, 4-(3,5-dimethyl-1H-pyrazol-1-yl)-6-morpholino-N-phenyl-1,3,5-triazin-2-amine (1) and N-(4-bromophenyl)-4-(3,5-dimethyl-1H-pyrazol-1-yl)-6-morpholino-1,3,5-triazin-2-amine (2) was investigated by impedimetric and potentiometric studies. It was found that (1) and (2) acted as cathodic-type corrosion inhibitors that retard the hydrogen evolution reaction. The percent corrosion inhibition, 98.5% for compound (2) (with bromo substituent) at 80 ppm, was slightly higher than 97.8% for (1) at 100 ppm. Thus, the replacement of a –H with –Br substituent increased the corrosion inhibition properties. Compound (2) exhibited Temkin isotherm adsorption, whereas compound (1) exhibited Langmuir adsorption. Scanning electron microscopy (SEM) analysis of the steel surface indicated that the inhibitors caused protection of the surface. The weight loss experiment also proved the decrease in the corrosion rate when inhibitors were added. The difference in inhibitory efficiency between compounds (1) and (2) was investigated by density functional theory (DFT) to study neutral and protonated species in gaseous and aqueous phases. The theoretical analysis demonstrated that compound (2) exhibited higher inhibitory activity on a metal surface compared to compound (1), aligning with the experimental results. The energy associated with the metal/adsorbate arrangement, represented by dEads/dNi, was higher for (2) (−380.91 kcal mol–1) compared to (1) (−371.64 kcal mol–1). This indicated better adsorption of (2) over (1).
和 N-(4-溴苯基)-4-(3,5-二甲基-1H-吡唑-1-基)-6-吗啉基-N-苯基-1,3,5-三嗪-2-胺(2)。研究发现,(1) 和 (2) 可作为阴极型缓蚀剂,延缓氢演化反应。化合物 (2)(带溴取代基)在 80 ppm 时的缓蚀百分率为 98.5%,略高于 (1) 在 100 ppm 时的 97.8%。因此,用 -Br 取代基取代 -H 增加了缓蚀性能。化合物(2)表现出滕金等温吸附,而化合物(1)则表现出郎穆尔吸附。钢表面的扫描电子显微镜(SEM)分析表明,抑制剂对钢材表面起到了保护作用。失重实验也证明了加入抑制剂后腐蚀速率的降低。密度泛函理论(DFT)研究了化合物 (1) 和 (2) 在气相和水相中的中性和质子化物种,从而探讨了它们在抑制效率上的差异。理论分析表明,与化合物 (1) 相比,化合物 (2) 在金属表面表现出更高的抑制活性,这与实验结果一致。以 dEads/dNi 表示的与金属/吸附剂排列相关的能量(-380.91 kcal mol-1)对 (2) 而言高于 (1) (-371.64 kcal mol-1)。这表明 (2) 比 (1) 有更好的吸附性。
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引用次数: 0
Ni–Unsymmetrical Salen Complex-Catalyzed One-Pot Multicomponent Reactions for Efficient Synthesis of Biologically Active 2-Amino-3-cyano-4H-pyrans 镍-不对称萨伦络合物催化的单锅多组分反应,用于高效合成具有生物活性的 2-氨基-3-氰基-4H-吡喃
IF 4.1 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-10 DOI: 10.1021/acsomega.4c03528
Sushree Aradhana Patra, Monojit Nandi, Mannar R. Maurya, Gurunath Sahu, Deepika Mohapatra, Hans Reuter, Rupam Dinda
In this report, four new Ni(II)–unsymmetrical salen complexes, [NiL1–4], were prepared by refluxing Ni(Ac)2·4H2O with unsymmetrical salen ligands, H2L1–4. All of the synthesized ligands and complexes were characterized by various physicochemical methods. Also, the solid-state structures of [NiL1], [NiL2], and [NiL4] were defined through single-crystal X-ray diffraction methods. The catalytic potential of [NiL1–4] was investigated by economic and environmentally friendly one-pot-three-component reactions (using reagent: 1,3-dicarbonyls, malononitrile, benzaldehyde, or its derivatives) for the synthesis of biologically active 2-amino-3-cyano-4H-pyran derivatives (total 16 derivatives). After optimization of the reaction conditions, this new synthetic protocol by taking Ni(II)–unsymmetrical salen complexes as catalysts shows excellent conversion with a maximum yield of up to 98% of the effective catalytic products within 1 h of reaction time. In addition, it was observed that the aromatic aldehyde containing an electron-withdrawing group as a ring substituent shows better conversion (up to 98%), and the electron-donating group substituent shows similar or less conversion compared to benzaldehyde under the optimized reaction conditions. From the comparison of results between all these Ni complexes, it was found that the efficiency of the catalytic performance follows the order [NiL1] > [NiL3] > [NiL2] > [NiL4]. A possible reaction pathway was predicted and established through UV–vis spectroscopy. Intermediate II proposed in the reaction pathway was also trapped and characterized through 1H and 13C NMR.
本报告通过将 Ni(Ac)2-4H2O 与非对称沙林配体 H2L1-4 进行回流,制备了四种新的 Ni(II)- 非对称沙林配合物 [NiL1-4]。所有合成的配体和配合物都通过各种理化方法进行了表征。此外,还通过单晶 X 射线衍射方法确定了 [NiL1]、[NiL2] 和 [NiL4] 的固态结构。通过经济、环保的一锅三组分反应(使用试剂:1,3-二羰基、丙二腈、苯甲醛或其衍生物)合成具有生物活性的 2-氨基-3-氰基-4H-吡喃衍生物(共 16 种衍生物),研究了 [NiL1-4] 的催化潜能。在优化反应条件后,以 Ni(II)-unsymmetrical salen 复合物为催化剂的这一新合成方案显示出极佳的转化率,在 1 小时的反应时间内,有效催化产物的最高收率可达 98%。此外,据观察,在优化的反应条件下,与苯甲醛相比,含环取代基撤电子基团的芳香醛的转化率更高(高达 98%),而取代基为电子供体的芳香醛的转化率相近或更低。通过比较所有这些 Ni 复合物的结果发现,催化效率遵循[NiL1] > [NiL3] > [NiL2] > [NiL4]的顺序。通过紫外可见光谱预测并确定了可能的反应途径。还通过 1H 和 13C NMR 捕获并表征了反应途径中提出的中间体 II。
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引用次数: 0
Antimicrobial Activity against Fusarium oxysporum f. sp. dianthi of TiO2/ZnO Thin Films under UV Irradiation: Experimental and Theoretical Study 紫外线照射下 TiO2/ZnO 薄膜对 Fusarium oxysporum f. sp. dianthi 的抗菌活性:实验和理论研究
IF 4.1 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-10 DOI: 10.1021/acsomega.4c01287
Cesar Quiñones, Martha Posada, Angie Hormiga, Julian Peña, Carlos Diaz-Uribe, William Vallejo, Amner Muñoz-Acevedo, Vanesa Roa, Eduardo Schott, Ximena Zarate
We deposited bare TiO2 and TiO2/ZnO thin films to study their antimicrobial capacity against Fusarium oxysporum f. sp. dianthi. The deposit of TiO2 was performed by spin coating and the ZnO thin films were deposited onto the TiO2 surface by plasma-assisted reactive evaporation technique. The characterization of the compounds was carried out by scanning electron microscopy (SEM) and powder X-ray diffraction techniques. Furthermore, density functional theory (DFT) and time-dependent DFT (TDDFT) calculations were performed to support the observed experimental results. Thus, the removal of methylene blue (MB) by adsorption and posterior photocatalytic degradation was studied. Adsorption kinetic results showed that TiO2/ZnO thin films were more efficient in MB removal than bare TiO2 thin films, and the pseudo-second-order model was suitable to describe the experimental results for TiO2/ZnO (qe = 12.9 mg/g; k2 = 0.14 g/mg/min) and TiO2 thin films (qe = 12.0 mg/g; k2 = 0.13 g/mg/min). Photocatalytic results under UV irradiation showed that TiO2 thin films reached 10.9% of MB photodegradation (k = 1.0 × 10–3 min–1), whereas TiO2/ZnO thin films reached 20.6% of MB photodegradation (k = 3.9 × 10–3 min–1). Both thin films reduced the photocatalytic efficiency by less than 3% after 4 photocatalytic tests. DFT study showed that the highest occupied molecular orbital–lowest unoccupied molecular orbital (HOMO–LUMO) energy gap decreases for the mixed nanoparticle system, showing its increased reactivity. Furthermore, the chemical hardness shows a lower value for the mixed system, whereas the electrophilicity index shows the biggest value, supporting the larger reactivity for the mixed nanoparticle system. Finally, the antimicrobial activity against F. oxysporum f. sp. dianthi showed that bare TiO2 reached a growth reduction of 68% while TiO2/ZnO reached a growth reduction of 90% after 250 min of UV irradiation.
我们沉积了裸TiO2和TiO2/ZnO薄膜,以研究它们对镰孢菌(Fusarium oxysporum f. sp. dianthi)的抗菌能力。二氧化钛的沉积是通过旋涂法进行的,氧化锌薄膜则是通过等离子体辅助反应蒸发技术沉积到二氧化钛表面的。化合物的表征采用了扫描电子显微镜(SEM)和粉末 X 射线衍射技术。此外,还进行了密度泛函理论(DFT)和随时间变化的 DFT(TDDFT)计算,以支持观察到的实验结果。因此,研究了亚甲基蓝(MB)的吸附去除和后光催化降解。吸附动力学结果表明,与裸 TiO2 薄膜相比,TiO2/ZnO 薄膜去除甲基蓝的效率更高,伪二阶模型适合描述 TiO2/ZnO(qe = 12.9 mg/g;k2 = 0.14 g/mg/min)和 TiO2 薄膜(qe = 12.0 mg/g;k2 = 0.13 g/mg/min)的实验结果。紫外线照射下的光催化结果表明,TiO2 薄膜对甲基溴的光降解率为 10.9%(k = 1.0 × 10-3 min-1),而 TiO2/ZnO 薄膜对甲基溴的光降解率为 20.6%(k = 3.9 × 10-3 min-1)。经过 4 次光催化测试后,两种薄膜的光催化效率都降低了不到 3%。DFT 研究表明,混合纳米粒子系统的最高占位分子轨道-最低未占位分子轨道(HOMO-LUMO)能隙减小,表明其反应活性增强。此外,混合体系的化学硬度值较低,而亲电性指数值最大,证明混合纳米粒子体系的反应性更强。最后,对 F. oxysporum f. sp. dianthi 的抗菌活性表明,裸 TiO2 在紫外线照射 250 分钟后可减少 68% 的生长,而 TiO2/ZnO 则可减少 90% 的生长。
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引用次数: 0
Antibacterial and Cytotoxicity of Extracts and Isolated Compounds from Artemisia abyssinica: A Combined Experimental and Computational Study 阿比西尼亚蒿提取物和分离化合物的抗菌性和细胞毒性:实验与计算相结合的研究
IF 4.1 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-10 DOI: 10.1021/acsomega.4c01096
Dawit Tesfaye, Milkyas Endale, Venkatesha Perumal Ramachandran, Emebet Getaneh, Guta Amenu, Leta Guta, Taye B. Demissie, Japheth O. Ombito, Rajalakshmanan Eswaramoorthy, Yadessa Melaku
Artemisia abyssinica is a widely cultivated hedge plant in Ethiopia. Traditionally, they have been used to treat a variety of health conditions, including intestinal problems, infectious diseases, tonsillitis, and leishmaniasis. Silica gel chromatographic separation of the methanol and ethyl acetate extracts of the leaves, roots, and stem barks of A. abyssinica led to the isolation of 12 compounds, labeled as 1–12. Among these, compounds 1, 3, 4, 5, and 7–11 are reported as new to the genus Artemisia. The extracts and isolated compounds from A. abyssinica were evaluated for their in vitro antibacterial activity against four bacterial strains: Streptococcus pyogenes, Staphylococcus aureus, Pseudomonas aeruginosa, and Escherichia coli, using the disc diffusion assay. All of the extracts displayed weak antibacterial activity, with inhibition zone diameters (IZDs) ranging from 6.10 ± 0.3 to 9.30 ± 0.20 mm. The isolated compounds, on the other hand, exhibited weak to moderate antibacterial activity, with IZDs ranging from 6.00 ± 0.300 to 13.50 ± 0.50 mm. The most potent antibacterial activity was observed for compound 6, which showed an IZD of 13.30 ± 0.50 mm against E. coli and 13.50 ± 0.50 mm against P. aeruginosa. This activity was comparable to that of the positive control ceftriaxone, which had IZDs of 14.1 ± 0.3 and 13.8 ± 0.5 mm against E. coli and P. aeruginosa, respectively. The in silico molecular docking analysis against DNA gyrase B revealed that compound 5 showed a higher binding affinity (−6.9 kcal/mol), followed by compound 10 (−6.7 kcal/mol) and compound 12 (−6.3 kcal/mol), whereas ciprofloxacin showed −7.3 kcal/mol. The binding affinities of compounds 5, 11, 10, and 9 were found to be −5.0, −4.3, −4.2, and −4.0 kcal/mol against S. aureus Pyruvate kinase, respectively, whereas ciprofloxacin showed a binding affinity of −4.9 kcal/mol, suggesting that compound 5 had a better binding affinity compared with ciprofloxacin. The effect of extracts of A. abyssinica was evaluated for cytotoxic activity against the breast cancer cell line (MCF-7) by the MTT assay. The extracts induced a decrease in cell viability and exerted a cytotoxic effect at a concentration of 20 μg/mL. The highest percent cell viability was observed for the methanol extract of the stem (92.9%), whereas the least was observed for the methanol extract of the root (34.5%). The result of the latter was significant compared with the positive control. The binding affinities of the isolated compounds were also assessed against human topoisomerase inhibitors IIβ. Results showed that compound 5 showed a binding affinity of −6.0 kcal/mol, followed by 11 (−5.4 kcal/mol), 10 (−5.0 kcal/mol), and 11 (−4.9 kcal/mol). Similar to ciprofloxacin, compounds 4, 5, 6, 9, 10, and <
阿比西尼亚蒿(Artemisia abyssinica)是埃塞俄比亚广泛种植的一种绿篱植物。传统上,它们被用来治疗各种健康问题,包括肠道疾病、传染病、扁桃体炎和利什曼病。对 A. abyssinica 的叶、根和茎皮的甲醇和乙酸乙酯提取物进行硅胶色谱分离后,分离出 12 种化合物,标记为 1-12。其中,化合物 1、3、4、5 和 7-11 是蒿属的新化合物。评估了 A. abyssinica 的提取物和分离化合物对四种细菌菌株的体外抗菌活性:采用盘扩散法评估了它们对四种细菌菌株的体外抗菌活性:化脓性链球菌、金黄色葡萄球菌、绿脓杆菌和大肠杆菌。所有提取物都显示出微弱的抗菌活性,抑菌区直径(IZD)从 6.10 ± 0.3 毫米到 9.30 ± 0.20 毫米不等。另一方面,分离出的化合物表现出弱到中等的抗菌活性,抑菌区直径(IZD)从 6.00 ± 0.300 毫米到 13.50 ± 0.50 毫米不等。化合物 6 的抗菌活性最强,对大肠杆菌的 IZD 为 13.30 ± 0.50 mm,对绿脓杆菌的 IZD 为 13.50 ± 0.50 mm。该活性与阳性对照头孢曲松的活性相当,后者对大肠杆菌和绿脓杆菌的 IZD 分别为 14.1 ± 0.3 mm 和 13.8 ± 0.5 mm。针对 DNA 回旋酶 B 的硅学分子对接分析表明,化合物 5 的结合亲和力较高(-6.9 kcal/mol),其次是化合物 10(-6.7 kcal/mol)和化合物 12(-6.3 kcal/mol),而环丙沙星的结合亲和力为-7.3 kcal/mol。化合物 5、11、10 和 9 与金黄色葡萄球菌丙酮酸激酶的结合亲和力分别为-5.0、-4.3、-4.2 和-4.0 kcal/mol,而环丙沙星的结合亲和力为-4.9 kcal/mol,这表明化合物 5 与环丙沙星相比具有更好的结合亲和力。通过 MTT 试验评估了 A. abyssinica 提取物对乳腺癌细胞株(MCF-7)的细胞毒性作用。在浓度为 20 μg/mL 时,提取物会导致细胞存活率下降并产生细胞毒性作用。细胞存活率最高的是茎的甲醇提取物(92.9%),最低的是根的甲醇提取物(34.5%)。与阳性对照相比,后者的结果非常显著。还评估了分离出的化合物与人类拓扑异构酶抑制剂 IIβ 的结合亲和力。结果显示,化合物 5 的结合亲和力为 -6.0 kcal/mol,其次是 11(-5.4 kcal/mol)、10(-5.0 kcal/mol)和 11(-4.9 kcal/mol)。与环丙沙星类似,化合物 4、5、6、9、10 和 12 也符合利宾斯基的五位法则。总之,对这些化学成分及其生物活性的全面研究加强了 A. abyssinica 的传统药用价值,值得进一步将这种植物作为新型治疗药物的来源进行研究。
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