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Synthesis of N-Sulfopropylated Hyperbranched Polyethyleneimine with Enhanced Biocompatibility and Antimicrobial Activity. 合成具有更强生物相容性和抗菌活性的正硫丙基超支化聚乙烯亚胺。
IF 3 4区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-09-22 DOI: 10.1002/cplu.202400454
Katerina N Panagiotaki, Kyriaki-Marina Lyra, Aggeliki Papavasiliou, Kostas Stamatakis, Zili Sideratou

Hyperbranched polyethyleneimine having 25,000 Da molecular weight was functionalized by a simple sulfopropylation reaction, affording a novel N-sulfopropylated PEI derivative (PEI-SO3 -). The successful introduction of N-sulfopropyl and sulfobetaine groups to the amino groups of PEI was spectroscopically confirmed. Furthermore, the antibacterial and anti-cyanobacterial activity of PEI-SO3 - in comparison to the parent PEI were investigated on two type heterotrophic bacteria, i. e., Gram (-) Escherichia coli and Gram (+) Staphylococcus Aureus bacteria, and one type of autotrophic cyanobacterium, i. e. Synechococcus sp. PCC 7942. Both PEI-SO3 - and PEI showed an enhanced, concentration-dependent antibacterial and anti-cyanobacterial activity against the tested bacteria strains, with PEI-SO3 - exhibiting higher activity than the parent PEI, signifying that the introduction of the sulfopropyl and sulfobetaine groups to the PEI amino groups enhanced the antibacterial and the anti-cyanobacterial properties of PEI. In the case of cyanobacteria, PEI-SO3 - was found to affect the integrity of the photosynthetic system by the inhibition of Photosystem-II electron transport activity. Cytocompatibility and hemocompatibility studies revealed that PEI-SO3 - exhibits high biocompatibility, suggesting that PEI-SO3 - could be considered as an attractive antibacterial and anti-cyanobacterial candidate for various applications in the disinfection industry and also against the harmful cyanobacterial blooms.

通过简单的磺丙基化反应对分子量为 25,000Da 的超支化聚乙烯亚胺进行了官能化,得到了一种新型 N-磺丙基聚乙烯亚胺衍生物(PEI-SO3-)。光谱学证实,N-磺丙基和磺基甜菜碱基团成功地引入了 PEI 的氨基。此外,还研究了 PEI-SO3- 与母体 PEI 相比,对两种异养细菌(即革兰氏(-)大肠杆菌和革兰氏(+)金黄色葡萄球菌)和一种自养蓝藻(即 Synechococcus sp.PCC 7942)的抗菌和抗蓝藻活性。PEI-SO3- 和 PEI 对测试菌株的抗菌和抗蓝藻活性均有所增强,且呈浓度依赖性,其中 PEI-SO3- 的活性高于母体 PEI,这表明在 PEI 氨基基团上引入磺丙基和磺基甜菜碱基团增强了 PEI 的抗菌和抗蓝藻特性。在蓝藻中,PEI-SO3- 可抑制光系统 II 的电子传递活性,从而影响光合作用系统的完整性。细胞相容性和血液相容性研究表明,PEI-SO3- 具有很高的生物相容性,这表明 PEI-SO3- 可被视为一种有吸引力的抗菌和抗蓝藻候选物质,可用于消毒行业的各种应用,也可用于对抗有害的蓝藻藻华。
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引用次数: 0
Inhibition of the Germination of Root Parasitic Plants by Zeolitic Imidazolate Framework-8. 沸石咪唑酸盐框架-8抑制根寄生植物的萌芽。
IF 3 4区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-09-22 DOI: 10.1002/cplu.202400457
Nouf Al Saleh, Lukman O Alimi, Muhammad Jamil, Somayah Qutub, Lamis Berqdar, Salim Al-Babili, Niveen M Khashab

Crystalline ZIF-8 (C-ZIF-8) and amorphous ZIF-8 (Am-ZIF-8) were prepared and investigated to control the germination of Striga hermonthica, a root parasitic plant, which threatens cereal crops production particularly in sub-Saharan Africa. We have demonstrated that Am-ZIF-8 shows a better performance than C-ZIF-8 in inhibiting Striga seeds germination. This efficient performance of Am-ZIF-8 materials can be attributed to the incomplete deprotonation of 2 methylimidazole (2MIM) during amorphization, leading to the presence of unsaturated Zn-N coordination with the uncoordinated -NH groups available to undergo hydrogen bonding with the strigolactone analog GR24 forming a more stable Am-ZIF-8⋅⋅⋅GR24 hydrogen bonded network. We further established that application of ZIF-8 materials generally has no adverse effects on the growth and quality of rice crops.

我们制备并研究了结晶 ZIF-8(C-ZIF-8)和无定形 ZIF-8(Am-ZIF-8),用于控制 Striga hermonthica 的萌发,Striga hermonthica 是一种根部寄生植物,对撒哈拉以南非洲地区的谷类作物生产构成威胁。我们已经证明,在抑制 Striga 种子萌发方面,Am-ZIF-8 的表现优于 C-ZIF-8。Am-ZIF-8 材料的这种高效性能可归因于 2 甲基咪唑(2MIM)在非晶化过程中的不完全去质子化,从而导致不饱和 Zn-N 配位的存在,未配位的 -NH 基团可与绞股蓝内酯类似物 GR24 发生氢键作用,形成更稳定的 Am-ZIF-8-GR24 氢键网络。我们进一步证实,应用 ZIF-8 材料一般不会对水稻作物的生长和品质产生不利影响。
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引用次数: 0
Photoelectrocatalytic CO2 Reduction to Formate Using a BiVO4/ZIF-8 Heterojunction. 使用 BiVO4/ZIF-8 异质结的光电催化 CO2 还原成甲酸酯。
IF 3 4区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-09-22 DOI: 10.1002/cplu.202400452
Zhi Yang, Jiaqi Yang, Huimin Yang, Fanfan Gao, Cheng Nan, Rui Chen, Yi Zhang, Xuemei Gao, Yue Yuan, Yibo Jia, Yuanjing Yang

Converting CO2 into high-value chemical fuels through green photoelectrocatalytic reaction path is considered as a potential strategy to solve energy and environmental problems. In this work, BiVO4/ZIF-8 heterojunctions are prepared by in-situ synthesis of ZIF-8 nanocrystals with unique pore structure on the surface of BiVO4. The experimental results show that the silkworm pupa-like BiVO4 is successfully combined with porous ZIF-8, and the introduction of ZIF-8 can provide more sites for CO2 capture. The optimal composite ratio of 4 : 1-BiVO4/ZIF-8 exhibits excellent CO2 reduction activity and the lowest electrochemical transport resistance. In the electrocatalytic system, the formate Faraday efficiency of 4 : 1-BiVO4/ZIF-8 at -1.0 V vs. RHE is 82.60 %. Furthermore, in the photoelectrocatalytic system, the Faraday efficiency increases to 91.24 % at -0.9 V vs. RHE, which is 10.8 times higher than the pristine BiVO4. The results show that photoelectric synergism can not only reduce energy consumption, but also improve the Faraday efficiency of formate. In addition, the current density did not decrease during 34 h electrolysis, showing long-term stability. This work highlights the importance of the construction of heterojunction to improve the performance of photoelectrocatalytic CO2 reduction.

通过绿色光电催化反应途径将二氧化碳转化为高价值的化学燃料被认为是解决能源和环境问题的潜在策略。本研究通过在 BiVO4 表面原位合成具有独特孔隙结构的 ZIF-8 纳米晶体,制备了 BiVO4/ZIF-8 异质结。实验结果表明,蚕蛹状 BiVO4 与多孔 ZIF-8 成功结合,ZIF-8 的引入可为二氧化碳捕集提供更多的位点。4:1-BiVO4/ZIF-8的最佳复合比例显示出优异的二氧化碳还原活性和最低的电化学传输电阻。在电催化系统中,4:1-BiVO4/ZIF-8 与 RHE 相比,在 -1.0 V 时的甲酸法拉第效率为 82.60%。此外,在光电催化系统中,当 - 0.9 V 对 RHE 时,法拉第效率增加到 91.24%,是原始 BiVO4 的 10.8 倍。结果表明,光电协同作用不仅能降低能耗,还能提高甲酸盐的法拉第效率。此外,在 34 小时的电解过程中,电流密度没有降低,显示出长期稳定性。这项工作凸显了构建异质结对提高光电催化二氧化碳还原性能的重要性。
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引用次数: 0
How Flexible Is the Hydrogen Sulfide Molecule Structure? Influence of Hydrogen Sulfide Molecule Geometry on Its Hydrogen Bonds. 硫化氢分子结构有多灵活?硫化氢分子几何形状对其氢键的影响。
IF 3 4区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-09-21 DOI: 10.1002/cplu.202400511
Milan R Milovavnović, Snežana D Zarić

The geometry of hydrogen sulfide was studied by calculating potential energy surface (PES) with over 1800 configurations. The calculations were performed at very accurate CCSD(T)/aug-cc-pvz5 level. The most stable geometry on the PES has bond angle (H-S-H) of 92.40° and bond length (S-H) of 1.338 Å. The PES shows that hydrogen sulfide is a quite flexible molecule. Namely, it can change the bonding angle (H-S-H) in the range of 15.6° (from 84.6° to 100.2°) and the bond lengths (S-H) in the range of 0.082 Å (from 1.299 Å to 1.381 Å) with an energy increase of only 1.0 kcal/mol. An influence of hydrogen sulfide geometry on its hydrogen bonds was studied on several hydrogen sulfide/hydrogen sulfide and water/hydrogen sulfide dimers. It showed that the change of hydrogen sulfide geometry does not influence the strength of hydrogen bond. Fully optimized geometries in gas and water solution phases revealed structural differences of both monomers and dimers in gas phase and water phase. SAPT analysis of the optimized dimer geometries showed that in all the dimers electrostatic is the most dominant contribution, while, in the dimers with hydrogen sulfide, the influence of dispersion contribution becomes quite pronounced.

通过计算 1800 多种构型的势能面 (PES),研究了硫化氢的几何形状。计算是在非常精确的 CCSD(T)/aug-cc-pvz5 水平上进行的。PES 上最稳定的几何构型的键角(H-S-H)为 92.40⁰,键长(S-H)为 1.338 Å。也就是说,它可以在 15.6⁰(从 84.6⁰到 100.2⁰)的范围内改变成键角 (H-S-H),在 0.082 Å(从 1.299 Å 到 1.381 Å)的范围内改变成键长度 (S-H),而能量仅增加 1.0 kcal/mol。在硫化氢/硫化氢和水/硫化氢二聚物上研究了硫化氢几何形状对其氢键的影响。结果表明,硫化氢几何形状的改变不会影响氢键的强度。在气相和水溶液相中完全优化的几何形状显示了单体和二聚体在气相和水相中的结构差异。对优化后的二聚体几何结构进行的 SAPT 分析表明,在所有二聚体中,静电作用是最主要的影响因素,而在含有硫化氢的二聚体中,分散作用的影响变得相当明显。
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引用次数: 0
4,4'-Sulfonyldianiline Derived Aggregation-Induced Emission Luminogen for the Detection of Ofloxacin. 用于检测氧氟沙星的 4,4'-磺酰基二苯胺衍生 AIE 发光体。
IF 3 4区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-09-21 DOI: 10.1002/cplu.202400537
Dhvani A Patel, Thangaraj Anand, Bigyan R Jali, Suban K Sahoo

The excessive use of antibiotic ofloxacin (Oflx) can cause serious detrimental effects to human health. Therefore, the utmost research priority is required to develop facile methods to detect Oflx. Herein, a V-shaped aggregation-induced emission (AIE) active Schiff base SDANA was introduced for the fluorescent turn-on detection of Oflx. The Schiff base SDANA was synthesized by condensing 4,4'-sulfonyldianiline with two equivalents of 2-hydroxy-1-naphthaldehyde. The nearly non-fluorescent SDANA in DMSO showed strong orange emission with the increase in HEPES buffer (H2O, 10 mM, pH 7.4) fractions in DMSO from 70 %-95 % due to the combined effects of AIE and ESIPT. The DLS and SEM analyses were performed to complement the formation of self-aggregates of SDANA. With the addition of Oflx, the fluorescence emission of AIE luminogen (AIEgen) SDANA (λem=575 nm, λex=400 nm) was blue-shifted and enhanced at 530 nm. The interactions of Oflx over the surface of SDANA aggregates disrupted the intramolecular charge transfer and aggregation morphology of SDANA, which gave a distinct fluorescence response to detect Oflx. The detection limit for Oflx was estimated as 0.81 μM, and the developed probe AIEgen SDANA was applied for the quantification of Oflx in human blood serum.

过量使用抗生素氧氟沙星(Oflx)会对人类健康造成严重危害。因此,当务之急是开发简便的方法来检测氧氟沙星。本文介绍了一种 V 型聚集诱导发射(AIE)活性席夫碱 SDANA,用于荧光开启式检测氧氟沙星。希夫碱 SDANA 是由 4,4'-磺酰基二苯胺与两当量的 2-羟基-1-萘甲醛缩合而成。在 AIE 和 ESIPT 的共同作用下,随着二甲基亚砜中 HEPES 缓冲液(H2O,10 mM,pH 7.4)馏分含量从 70% 增加到 95%,二甲基亚砜中几乎无荧光的 SDANA 显示出强烈的橙色发射。DLS 和 SEM 分析对 SDANA 自聚物的形成进行了补充。加入 Oflx 后,AIE 发光剂(AIEgen)SDANA(lem = 575 nm,lex = 400 nm)的荧光发射在 530 nm 处发生蓝移并增强。Oflx在SDANA聚集体表面的相互作用破坏了SDANA的分子内电荷转移和聚集形态,从而产生了明显的荧光响应,可用于检测Oflx。据估计,Oflx的检测限为0.81 µM,所开发的探针AIEgen SDANA被用于定量检测人血清中的Oflx。
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引用次数: 0
Platelet Ceria Catalysts from Solution Combustion and Effect of Iron Doping for Synthesis of Dimethyl Carbonate from CO2 溶液燃烧生成的小板铈催化剂及掺铁对二氧化碳合成碳酸二甲酯的影响
IF 3.4 4区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-09-20 DOI: 10.1002/cplu.202400521
Nicoletta Rusta, Valentina Mameli, Pier Carlo Ricci, Stefania Porcu, Panpailin Seeharaj, Aryane Marciniak, Evelyn Santos, Odivaldo Cambraia Alves, Claudio Mota, Elisabetta Rombi, Carla Cannas
Solution combustion (SC) remains among the most promising synthetic strategies for the production of crystalline nanopowders from an aqueous medium, due to its easiness, time and cost-effectiveness, scalability and eco-friendliness. In this work, this method was selected to obtain anisometric ceria-based nanoparticles applied as catalysts for the direct synthesis of dimethyl carbonate. The catalytic performances were studied for the ceria and Fe-doped ceria from SC (CeO2-SC, Ce0.9Fe0.1O2-SC) in comparison with the ceria nanorods (CeO2-HT, Ce0.9Fe0.1O2-HT) obtained by hydrothermal (HT) method, one of the most studied systems in the literature. Indeed, the ceria nanoparticles obtained by SC were found to be highly crystalline, platelet-shaped, arranged in a mosaic-like assembly and with smaller crystallite size (≈6 nm vs. ≈17 nm) and higher surface area (80 m2 g-1vs. 26 m2 g-1) for the undoped sample with respect to the Fe-doped counterpart. Although all samples exhibit an anisometric morphology that should favor the exposition of specific crystalline planes, HT-samples showed better performances due to higher oxygen vacancies concentration and lower amount of strong basic and acid sites.
溶液燃烧法(SC)因其简便易行、省时省力、成本效益高、可扩展性强和生态友好等优点,仍然是从水介质中生产结晶纳米粉体的最有前途的合成策略之一。在这项工作中,我们选择了这种方法来获得异性铈基纳米粒子,并将其用作直接合成碳酸二甲酯的催化剂。研究了来自 SC 的铈和掺铁铈(CeO2-SC、Ce0.9Fe0.1O2-SC)与通过水热法(HT)获得的铈纳米棒(CeO2-HT、Ce0.9Fe0.1O2-HT)的催化性能,后者是文献中研究最多的体系之一。事实上,通过水热法获得的铈纳米粒子具有高结晶性、板状、马赛克状排列,与掺杂铁的样品相比,未掺杂样品的结晶尺寸更小(≈6 nm 对 ≈17 nm),比表面积更大(80 m2 g-1 对 26 m2 g-1)。虽然所有样品都呈现出异相形态,有利于特定晶面的暴露,但 HT 样品由于氧空位浓度较高,强碱和强酸位点较少,因此性能更好。
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引用次数: 0
Interplay between the N→C Dative Bond, Intramolecular Chalcogen Bond and π Conjugation in the Complexes Formed by Cyclo[18]carbon and C14 Polyyne with 1,2,5-Chalcogenadiazoles 环[18]碳和 C14 聚炔与 1,2,5-Chalcogenadiazoles 形成的复合物中 N→C 衍生键、分子内链原键和π共轭之间的相互作用
IF 3.4 4区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-09-20 DOI: 10.1002/cplu.202400557
Weizhou Wang, Yu Zhang
The N→C dative bond (DB), intramolecular chalcogen bond and π conjugation play important roles in determining the structures and properties of some molecular carbon materials and organic/polymeric photovoltaic materials. In this work, the interplay between the N→C dative bond, intramolecular chalcogen bond and π conjugation in the complexes formed by cyclo[18]carbon and C14 polyyne with 1,2,5-chalcogenadiazoles has been investigated in detail by using reliable quantum chemical calculations. This study has made four main findings. First, only the Te-containing complexes bound by N→C dative bonds are much more stable than their corresponding van der Waals (vdW) complexes. Second, in addition to through-bond π conjugations, through-space π conjugations also exist in some Se/Te-containing complexes bound by N→C dative bonds. Third, the cooperativity between intramolecular chalcogen bond, π conjugation between two monomers and N→C dative bond is not very strong and can be ignored. Fourth, compared to π conjugations, intramolecular Ch···C (Ch = O, S, Se, Te) chalcogen bonds play a secondary role in stabilizing the complexes bound by N→C dative bonds. These findings clearly indicate that the role of “conformational lock”, popular in the field of organic optoelectronic materials, may have been greatly overestimated.
N→C原生键(DB)、分子内胆原键和π共轭在决定一些分子碳材料和有机/聚合物光伏材料的结构和性质方面发挥着重要作用。本研究通过可靠的量子化学计算,详细研究了环[18]碳和 C14 聚炔与 1,2,5-查尔根二唑形成的配合物中 N→C 共价键、分子内查尔根键和π共轭之间的相互作用。这项研究有四个主要发现。首先,只有通过 N→C 负键结合的含碲复合物才比相应的范德华(vdW)复合物稳定得多。其次,除了通键π共轭外,一些以 N→C 配位键结合的含 Se/Te 复合物中还存在通空π共轭。第三,分子内查尔根键、两个单体间的π共轭和 N→C 二价键之间的合作性不是很强,可以忽略。第四,与π共轭相比,分子内的Ch---C(Ch = O、S、Se、Te)共价键在稳定由N→C共价键结合的配合物方面起次要作用。这些发现清楚地表明,有机光电材料领域流行的 "构象锁定 "的作用可能被大大高估了。
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引用次数: 0
A QSPR Model for Henry’s Law Constants of Organic Compounds in Water and Ethanol for Distilled Spirits 蒸馏酒水和乙醇中有机化合物亨利定律常数的 QSPR 模型
IF 3.4 4区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-09-20 DOI: 10.1002/cplu.202400459
John White, Johnathan Graf, Samuel Haines, Noppadon Sathitsuksanoh, Robert Eric Berson, Vance Jaeger
Henry’s law describes the vapor-liquid equilibrium for dilute gases dissolved in a liquid solvent phase. Descriptions of vapor-liquid equilibrium allow the design of improved separations in the food and beverage industry. The consumer experience of taste and odor are greatly affected by the liquid and vapor phase behavior of organic compounds. This study presents a machine learning (ML) based model that allows quick, accurate predictions of Henry’s law constants (kH) for many common organic compounds. Users input only a Simplified Molecular-Input Line-Entry System (SMILES) string or a common English name, and the model returns Henry’s law estimates for compounds in water and ethanol. Training was performed on 5,690 compounds. Training data were gathered from an existing database and were supplemented with quantum mechanical (QM) calculations. An extra trees regression model was generated that predicts kH with a mean absolute error of 1.3 in log space and an R2 of 0.98. The model is applied to common flavor and odor compounds in bourbon whiskey as a test case for food and beverage applications.
亨利定律描述了溶解在液态溶剂中的稀释气体的汽液平衡。通过对汽液平衡的描述,可以改进食品和饮料行业的分离设计。消费者对味道和气味的体验在很大程度上受到有机化合物液相和气相行为的影响。本研究提出了一种基于机器学习(ML)的模型,可以快速、准确地预测许多常见有机化合物的亨利定律常数(kH)。用户只需输入一个简化分子输入行输入系统(SMILES)字符串或一个常见的英文名称,模型就会返回水和乙醇中化合物的亨利定律估计值。对 5,690 种化合物进行了训练。训练数据来自现有数据库,并辅以量子力学(QM)计算。生成的额外树回归模型预测 kH 的对数空间平均绝对误差为 1.3,R2 为 0.98。该模型适用于波本威士忌中常见的风味和气味化合物,作为食品和饮料应用的测试案例。
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引用次数: 0
Front Cover: Photocatalytic Transformation of Organics to Valuable Chemicals – Quo Vadis? (ChemPlusChem 9/2024) 封面:光催化有机物转化为有价值的化学品--何去何从? (ChemPlusChem 9/2024)
IF 3 4区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-09-13 DOI: 10.1002/cplu.202480901
Wiktoria Adamowicz, Dr. Kasidid Yaemsunthorn, Dr. Marcin Kobielusz, Prof. Wojciech Macyk

The front cover article describes the recent progress in the field of photocatalytic transformation of organics to valuable chemicals. This comprehensive review highlights how photocatalysis can be involved in selective transformations of organic compounds, including reduction and coupling reactions such as C-C and C-N couplings. By examining intrinsic and extrinsic factors, the authors provide insights into the rational design of efficient and stable photocatalytic systems dedicated to the synthesis of fine chemicals. More details can be found in the Review by Marcin Kobielusz, Wojciech Macyk, and co-workers (DOI: 10.1002/cplu.202400171).

封面文章介绍了光催化将有机物转化为有价值化学品领域的最新进展。这篇综述重点介绍了光催化如何参与有机化合物的选择性转化,包括还原和偶联反应,如 C-C 和 C-N 偶联。通过研究内在和外在因素,作者深入探讨了如何合理设计专用于精细化学品合成的高效、稳定的光催化系统。更多详情,请参阅 Marcin Kobielusz、Wojciech Macyk 及合作者的评论文章(DOI: 10.1002/cplu.202400171)。
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引用次数: 0
Colloidal Bimetallic RuNi Particles and their Behaviour in Catalytic Quinoline Hydrogenation 胶体双金属 RuNi 粒子及其在催化喹啉加氢反应中的行为
IF 3.4 4区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-09-13 DOI: 10.1002/cplu.202400516
Miquel Cardona-Farreny, Hiroya Ishikawa, Abolanle Olatilewa Odufejo Ogoe, Sonia Mallet-Ladeira, Yannick Coppel, Pierre Lecante, Jerome Esvan, Karine Philippot, M. Rosa Axet
Colloidal metal nanoparticles exhibit interesting catalytic properties for the hydrogenation of (hetero)arenes. Catalysts based on precious metals, such as Ru and Rh, proceed efficiently under mild reaction conditions. In contrast, heterogeneous catalysts based on earth‐abundant metals can selectively hydrogenate (hetero)arenes but require harsher reaction conditions. Bimetallic catalysts that combine precious and earth‐abundant metals are interesting materials to mitigate the drawbacks of each component. To this end, RuNi nanoparticles bearing a phosphine ligand were prepared through the decomposition of [Ru(η4‐C8H12)(η6‐C8H10)] and [Ni(η4‐C8H12)2] by H2 at 85°C. Wide angle X‐ray scattering confirmed a bimetallic segregated structure, with Ni predominantly on the surface. Spectroscopic analyses revealed that the phosphine ligand coordinated to the surface of both metals, suggesting, as well, a partial Ni shell covering the Ru core. The RuNi‐based nanomaterials were used as catalysts in the hydrogenation of quinoline to assess the impact of the metallic composition and of the stabilizing agent on their catalytic performance.
胶体金属纳米粒子在(杂)炔的氢化反应中表现出有趣的催化特性。基于贵金属(如 Ru 和 Rh)的催化剂可在温和的反应条件下高效地进行反应。相比之下,基于富土金属的异相催化剂可以选择性地氢化(杂)炔,但需要更苛刻的反应条件。结合了贵金属和富土金属的双金属催化剂是一种有趣的材料,可以减轻每种成分的缺点。为此,我们在 85°C 下通过 H2 分解[Ru(η4-C8H12)(η6-C8H10)]和[Ni(η4-C8H12)2]制备了带有膦配体的 RuNi 纳米粒子。广角 X 射线散射证实了双金属偏析结构,镍主要位于表面。光谱分析显示,膦配体同时配位在两种金属的表面,这也表明在 Ru 内核上有部分 Ni 外壳。RuNi 基纳米材料被用作喹啉氢化的催化剂,以评估金属成分和稳定剂对其催化性能的影响。
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引用次数: 0
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