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DFT Study of Structural, Elastic, Electronic, and Thermodynamic Properties of Compounds Cs2TiCl6 and Cs2TiBr6 化合物 Cs2TiCl6 和 Cs2TiBr6 的结构、弹性、电子和热力学性质的 DFT 研究
IF 2.1 3区 化学 Q3 CHEMISTRY, INORGANIC & NUCLEAR Pub Date : 2024-08-13 DOI: 10.1134/s0036023624601223
R. Ksouri, R. Maizi, A.-G. Boudjahem, N. Cheghib, I. Djaghout, M. Derdare

Abstract

We investigate the electronic, structural, elastic, and thermodynamic properties of Cs2TiX6 (X = Cl and Br) using DFT calculations. The generalized gradient approximation in the Perdew–Burke–Ernzerhof (PBE) form is used in this work to investigate the properties of the above compounds. The calculated lattice parameters of these compounds are in good agreement with the experimental data. The elastic constants obtained confirm the mechanical stability of Cs2TiX6 compounds. The calculated Pugh’s and Poisson’s ratios revealed that the Cs2TiCl6 and Cs2TiBr6 compounds are brittle materials. The band gaps of Cs2TiCl6 and Cs2TiBr6 compounds are, respectively, 2.27 and 1.45 eV. The thermodynamic properties of these compounds have also been investigated, and the thermodynamic parameters such as heat capacity (CV) and the thermal expansion (α) were calculated. The obtained values of CV were found to be 125 and 224 J mol–1 K–1 for Cs2TiCl6 and Cs2TiBr6, respectively. Debye temperatures for the studied compounds were also computed and discussed.

摘要 我们利用 DFT 计算研究了 Cs2TiX6(X = Cl 和 Br)的电子、结构、弹性和热力学性质。本文采用 Perdew-Burke-Ernzerhof (PBE) 形式的广义梯度近似来研究上述化合物的性质。计算得出的这些化合物的晶格参数与实验数据十分吻合。得到的弹性常数证实了 Cs2TiX6 化合物的机械稳定性。计算得出的普氏和泊松比表明,Cs2TiCl6 和 Cs2TiBr6 化合物是脆性材料。Cs2TiCl6 和 Cs2TiBr6 化合物的带隙分别为 2.27 和 1.45 eV。此外,还研究了这些化合物的热力学性质,并计算了热容(CV)和热膨胀(α)等热力学参数。结果发现,Cs2TiCl6 和 Cs2TiBr6 的 CV 值分别为 125 和 224 J mol-1 K-1。还计算并讨论了所研究化合物的德拜温度。
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引用次数: 0
Solubility in the MgSO4–NaCl–H2O System and Its Polythermal Diagram MgSO4-NaCl-H2O 系统中的溶解度及其多热图
IF 2.1 3区 化学 Q3 CHEMISTRY, INORGANIC & NUCLEAR Pub Date : 2024-08-13 DOI: 10.1134/s0036023624600473
U. D. Rakhmatzhanov, R. Ch. Yorbobaev, Kh. Ch. Mirzakulov

Abstract

The MgSO4–NaCl–H2O system was studied in the temperature range from –25 to 42°С by the visual polythermal method of solubility. A polythermal diagram of the solubility of this system was constructed on the basis of the solubility polytherms of binary systems and internal sections. On the phase diagram of the MgSO4–NaCl–H2O system the crystallization fields of ice, MgSO4∙H2O, MgSO4∙6H2O, MgSO4∙7H2O, MgSO4∙12H2O, NaCl∙H2O, and compound of the composition MgCl2 were delimited. The study results show that the MgSO4–NaCl–H2O system belongs to the complex eutonic type.

摘要 采用可视多热效应溶解度法研究了 MgSO4-NaCl-H2O 体系在 -25 至 42°С 温度范围内的溶解度。根据二元体系的溶解度聚醚和内部截面,构建了该体系的溶解度聚热图。在 MgSO4-NaCl-H2O 系统的相图上,划定了冰、MgSO4∙H2O、MgSO4∙6H2O、MgSO4∙7H2O、MgSO4∙12H2O、NaCl∙H2O 和成分为 MgCl2 的化合物的结晶区域。研究结果表明,MgSO4-NaCl-H2O 系统属于复合优素体类型。
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引用次数: 0
Effectiveness of B12N12 Nanocage as a Stabilizer and Delivery Carrier for Thymol and Carvacrol Essential Oils and their Influence on Escherichia coli and Staphylococcus aureus Bacteria: A Comprehensive Analysis using DFT, QTAIM, Multiwfn, and Molecular Docking B12N12 纳米笼作为百里酚和香芹酚精油的稳定剂和输送载体的有效性及其对大肠杆菌和金黄色葡萄球菌的影响:利用 DFT、QTAIM、Multiwfn 和分子对接进行综合分析
IF 2.1 3区 化学 Q3 CHEMISTRY, INORGANIC & NUCLEAR Pub Date : 2024-08-13 DOI: 10.1134/s0036023624601235
A. Mahal, A. M. Almaamuri, S. S. Noori, S. Chandra, A. Elawady, A. J. Obaidullah, M. H. Shuhata Alubiady, S. H. Zain Al-Abdeen, R. Zainul

Abstract

Bacteria have developed a tolerance due to the overuse of antibiotics. Even though thyme essential oils have antibacterial properties, their utilization is restricted because of their instability. To overcome these limitations, one strategy is to interact the oils with other molecules. This research delved into the effective role of B12N12 in attaching thymol and carvacrol oils as a nanocarrier in drug delivery using density functional calculations (DFT) in both gas and solvent phases. Thymol and carvacrol oils have been found to interact with B12N12 through oxygen atoms, resulting in adsorption energies (Ead) of –12.49 and –12.39 kcal/mol on the nanocage, respectively. The adsorption and solvation energy values, along with notable alterations in the polarity of the complexes, indicated the potential of the B12N12 nanocage as an effective delivery carrier for the oils. The analysis of the quantum theory of atoms in molecules (QTAIM), the electron localization function (ELF), localized orbital locator (LOL), and density of states (DOS) showed that the nature of the interaction between the oils and the nanocage is non-covalent, which is beneficial for the release of the oils in drug delivery. The quantum molecular descriptors (QMDs) and the vibrational frequency calculations indicated that the complexes are stable. Moreover, Mulliken population analysis (MPA), molecular electrostatic potential (MEP), UV-Vis spectra, and thermodynamic parameters for the molecules were calculated. In silico molecular docking, 4WUB and 3VSL receptors were used to investigate thymol, carvacrol, thymol/B12N12, and carvacrol/B12N12 compounds inhibitor properties. The molecular docking analysis showed that the thymol/B12N12 and carvacrol/B12N12 compounds have the free negative binding energy values and low Ki (inhibition constant) values. This suggests that these compounds are more suitable for interacting with the 4WUB and 3VSL receptor targets compared to the Thymol and Carvacrol oils.

摘要 由于过度使用抗生素,细菌产生了耐药性。尽管百里香精油具有抗菌特性,但由于其不稳定性,其使用受到了限制。为了克服这些限制,一种策略是将精油与其他分子相互作用。本研究利用气相和溶剂相的密度泛函计算(DFT),探讨了 B12N12 在附着百里酚和香芹醇油作为纳米载体给药方面的有效作用。研究发现,百里酚和香芹醇油通过氧原子与 B12N12 相互作用,在纳米载体上产生的吸附能(Ead)分别为 -12.49 和 -12.39 kcal/mol。这些吸附能和溶解能值以及复合物极性的显著变化表明,B12N12 纳米笼具有作为油类有效输送载体的潜力。对分子中原子量子理论(QTAIM)、电子定位功能(ELF)、局部轨道定位器(LOL)和状态密度(DOS)的分析表明,油类与纳米囊之间的相互作用性质是非共价的,这有利于在给药过程中释放油类。量子分子描述符(QMDs)和振动频率计算表明,复合物是稳定的。此外,还计算了分子的 Mulliken 种群分析(MPA)、分子静电位(MEP)、紫外可见光谱和热力学参数。利用硅分子对接、4WUB 和 3VSL 受体研究了百里酚、香芹酚、百里酚/B12N12 和香芹酚/B12N12 复合物的抑制特性。分子对接分析表明,百里酚/B12N12 和香芹酚/B12N12 化合物具有自由负结合能值和较低的 Ki(抑制常数)值。这表明,与百里酚和香芹醇油相比,这些化合物更适合与 4WUB 和 3VSL 受体靶标相互作用。
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引用次数: 0
A Novel Multichromic Cd(II) Coordination Polymer Based on a Viologen Ligand Exhibiting Multichroism, Aniline Detection and Luminescence Properties 一种基于病毒配体的新型多色镉(II)配位聚合物,具有多色性、苯胺检测和发光特性
IF 2.1 3区 化学 Q3 CHEMISTRY, INORGANIC & NUCLEAR Pub Date : 2024-08-13 DOI: 10.1134/s0036023624601119
Ran Tao, Xiuyan Wang, Xin Wang, Zirui Huang, Shanshan Jin, Hongqiang Wang

Abstract

As a powerful strategy to precisely fabricate multifunctional materials with unique optoelectronic properties, donor-acceptor (D–A) alignment, which integrates D–A pairs into the modular and versatile crystalline cation metal–organic frameworks (CMOFs) and cation coordination polymers (CCPs) is applied at the molecular level. In this paper, a photo- and thermochromic CCP, named [Cd (PTA)0.5(bcbpy)0.5Br] (1), was successfully produced by the self-assembly of a photo- and thermoactive 1,1'-bis((3-carboxylatobenzyl)-4,4'-bipyridinium)-dibromo ligand (H2bcbpy·2Br) with cadmium chloride and terephthalic acid (PTA). This complex is characterized by single-crystal X-ray diffraction, powder X-ray diffraction and it exhibits high sensitivity to both heat and different illuminant. The exceptional difunctional characteristics of electron-transfer (ET) thermochromism and photochromism in 1 are mostly influenced by the photosensitivity and thermal sensitivity of H2bcbpy·2Br. Otherwise, during the coloration-decoloration phase, there is a photoluminescence “on/off switch” which would direct the synthesis of new crystals.

摘要 作为精确制备具有独特光电特性的多功能材料的有力策略,供体-受体(D-A)配位将 D-A 对整合到模块化的多功能结晶阳离子金属有机框架(CMOFs)和阳离子配位聚合物(CCPs)的分子水平上。在本文中,氯化镉和对苯二甲酸(PTA)通过光热活性 1,1'-双((3-羧基阿托苄基)-4,4'-联吡啶鎓)-二溴配体(H2bcbpy-2Br)的自组装,成功制备了一种光热变色 CCP,命名为[Cd (PTA)0.5(bcbpy)0.5Br](1)。该复合物通过单晶 X 射线衍射和粉末 X 射线衍射进行表征,对热和不同光源均表现出高度敏感性。1 中电子转移(ET)热致变色和光致变色的特殊双功能特性主要受到 H2bcbpy-2Br 的光敏性和热敏性的影响。否则,在着色-脱色阶段,光致发光的 "开关 "将引导新晶体的合成。
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引用次数: 0
Synthesis, Structure, and Magnetic Properties of Mn-Substituted Magnetite for Magnetorheological Materials 用于磁流变材料的锰取代磁铁矿的合成、结构和磁性能
IF 2.1 3区 化学 Q3 CHEMISTRY, INORGANIC & NUCLEAR Pub Date : 2024-08-09 DOI: 10.1134/s0036023624601065
Yu. S. Haiduk, E. V. Korobko, L. V. Radkevich, R. P. Golodok, A. E. Usenka, V. V. Pankov

Abstract

Iron(II) manganese(II) ferrite Mn0.3Fe2.7O4 was synthesized by co-precipitation (with various options for the subsequent heat and mechanical treatment of the precipitate). The material was studied by powder X-ray diffraction, infrared spectroscopy, scanning electron microscopy, and magnetometry. The powder that was annealed under argon at 740°С (8.0 h) and subjected to high-energy milling (1.0 h) at the final stage of the synthesis is a promising functional filler for magnetorheological materials, owing to high shear stress (3500 Pa at 625 mT) of an oil suspension based on this powder and high oil absorption capacity, which ensures sedimentation stability of the suspension.

摘要 通过共沉淀法合成了铁(II)锰(II)铁氧体 Mn0.3Fe2.7O4(沉淀物的后续热处理和机械处理有多种选择)。通过粉末 X 射线衍射、红外光谱、扫描电子显微镜和磁力测定法对该材料进行了研究。该粉末在氩气环境下于 740°С 下退火(8.0 小时),并在合成的最后阶段进行了高能研磨(1.0 小时),由于基于该粉末的油悬浮液具有高剪切应力(625 mT 时为 3500 Pa)和高吸油能力,从而确保了悬浮液的沉降稳定性,因此是一种很有前途的磁流变材料功能填料。
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引用次数: 0
Study of Co-crystallization of Neodymium and Strontium Sulfates in the Absence of Potassium Ions 硫酸钕和硫酸锶在无钾离子情况下的共晶体化研究
IF 2.1 3区 化学 Q3 CHEMISTRY, INORGANIC & NUCLEAR Pub Date : 2024-08-09 DOI: 10.1134/s0036023624601168
N. N. Bushuev, G. K. Tatosyan

Abstract

Co-crystallization of neodymium and strontium sulfates was studied using powder X-ray diffraction, energy dispersive X-ray spectroscopy, and microscopy. High absorption activity of crystalline matrices, trigonal SrSO4∙0.5H2O and dehydrated monoclinic SrSO4, towards the isomorphic heterovalent inclusion of Nd3+ ions to give solid solutions stable in the absence of water was established for the first time. The unit cell parameters and the structural similarity of the solid solutions were determined. In a moist environment, solid solutions degrade within 6–10 h to give stable poorly soluble single compounds Nd2(SO4)3∙8H2O and orthorhombic SrSO4.

摘要 利用粉末 X 射线衍射、能量色散 X 射线光谱和显微镜研究了钕和锶硫酸盐的共晶。首次确定了晶体基质(三棱 SrSO4∙0.5H2O 和脱水单斜 SrSO4)对 Nd3+ 离子的同构异价包合的高吸收活性,从而得到在无水条件下稳定的固溶体。确定了固溶体的单胞参数和结构相似性。在潮湿环境中,固溶体会在 6-10 小时内降解,生成稳定的难溶单一化合物 Nd2(SO4)3∙8H2O 和正方体 SrSO4。
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引用次数: 0
Influence of the Composition of the MF–HCl (M = Li+, Na+, $${text{NH}}_{4}^{ + }$$ ) Etching System on the Gas-Sensing Properties of Ti3C2Tx/TiOx Nanocomposites MF-HCl(M = Li+、Na+、$${text{NH}}_{4}^{ + }$$)蚀刻体系的成分对 Ti3C2Tx/TiOx 纳米复合材料气体传感性能的影响
IF 2.1 3区 化学 Q3 CHEMISTRY, INORGANIC & NUCLEAR Pub Date : 2024-07-31 DOI: 10.1134/s0036023624600837
E. P. Simonenko, A. S. Mokrushin, I. A. Nagornov, V. M. Sapronova, Yu. M. Gorban, Ph. Yu. Gorobtsov, T. L. Simonenko, N. P. Simonenko, N. T. Kuznetsov

Abstract

A study was made of the effect of the nature of the MF–HCl (M = Li+, Na+, ({text{NH}}_{4}^{ + })) etching systems on the synthesis of Ti3C2Tx MXenes based on the Ti3AlC2 MAX phase, microstructure, phase purity, interlayer distance, composition of functional surface groups, thermal behavior, and work function of the resulting products. The gas-sensing properties of Ti3C2Tx receptor layers deposited by microplotter printing were tested to a wide range of gaseous analytes (H2, CO, NH3, NO2, O2, benzene, acetone, methane, and ethanol) at room temperature. An increased sensitivity to ammonia was detected for MXenes produced by exposure to hydrochloric acid solutions of sodium and ammonium fluorides, and an elevated sensitivity to carbon monoxide was determined for a sample synthesized using the LiF–HCl system. High responses (~20–30% per 100 ppm NO2) were measured for all three receptor materials; however, sensor recovery processes were much more difficult. To improve the sensory characteristics, the sensitive Ti3C2Tx layers were subjected to relatively low temperature heat-treatment in an air atmosphere to form Ti3C2Tx/TiOx nanocomposites. It was detected that partially oxidized MXenes exhibit a high selective response to oxygen at very low operating temperatures (125–175°C), which is especially typical of the material produced using the HCl–NaF system.

摘要 研究了 MF-HCl(M = Li+、Na+、({text{NH}}_{4}^{ + }) 蚀刻体系的性质对基于 Ti3AlC2 MAX 相的 Ti3C2Tx MXenes 的合成、微观结构、相纯度、层间距离、功能表面基团的组成、热行为和所得产物的功函数的影响。在室温下,测试了通过微绘图仪印刷沉积的 Ti3C2Tx 受体层对多种气体分析物(H2、CO、NH3、NO2、O2、苯、丙酮、甲烷和乙醇)的气敏特性。在接触氟化钠和氟化铵的盐酸溶液后生成的 MXenes 中,检测到对氨的灵敏度增加;在使用 LiF-HCl 系统合成的样品中,检测到对一氧化碳的灵敏度增加。对所有三种受体材料都测得了较高的响应(每 100 ppm NO2 约 20-30%);但是,传感器的恢复过程要困难得多。为了改善传感特性,敏感的 Ti3C2Tx 层在空气环境中进行了相对低温的热处理,形成了 Ti3C2Tx/TiOx 纳米复合材料。研究发现,在极低的工作温度(125-175°C)下,部分氧化的 MXenes 对氧气有很高的选择性反应,这在使用 HCl-NaF 系统生产的材料中尤为典型。
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引用次数: 0
Features of the Structure and Thermal Properties of Borate Tungstates LnBWO6 (Ln = La; La0.999Nd0.001 and La0.99Gd0.01) Synthesized by the Sol–Gel Method 溶胶-凝胶法合成的硼酸盐钨酸盐 LnBWO6(Ln = La;La0.999Nd0.001 和 La0.99Gd0.01)的结构和热性能特征
IF 2.1 3区 化学 Q3 CHEMISTRY, INORGANIC & NUCLEAR Pub Date : 2024-07-31 DOI: 10.1134/s0036023624600394
V. A. Krut’ko, M. G. Komova, R. D. Svetogorov, A. V. Khoroshilov, N. N. Efimov, E. A. Ugolkova

Abstract

Borate tungstates LnBWO6 (Ln = La; La0.999Nd0.001 and La0.99Gd0.01) are synthesized by the Pechini method followed by annealing of the intermediates and examined by X-ray diffraction (XRD) and differential scanning calorimetry (DSC). The crystallographic parameters of the synthesized LnBWO6 are refined by powder X-ray diffraction in two crystal systems: monoclinic (space group P21) and orthorhombic (space group P222). Reversible first-order phase transitions in the synthesized LnBWO6 are detected by the DSC method, and the temperatures and enthalpies of phase transformations are determined. The doping of LnBWO6 with Nd3+ and Gd3+ ions is shown to decrease the temperature of the LT (low-temperature) → HT (high-temperature) phase transition of LaBWO6. Two independent positions of Gd in the La0.99Gd0.01BWO6 structure are determined from the experimental electron paramagnetic resonance (EPR) data.

摘要 通过佩奇尼法合成了硼钨酸盐 LnBWO6(Ln = La;La0.999Nd0.001 和 La0.99Gd0.01),然后对中间产物进行退火处理,并通过 X 射线衍射 (XRD) 和差示扫描量热 (DSC) 进行了检验。合成的 LnBWO6 的晶体学参数通过粉末 X 射线衍射细化为两个晶系:单斜晶系(空间群 P21)和正交晶系(空间群 P222)。利用 DSC 方法检测了合成 LnBWO6 中的可逆一阶相变,并确定了相变的温度和焓。结果表明,在 LnBWO6 中掺杂 Nd3+ 和 Gd3+ 离子可降低 LaBWO6 的 LT(低温)→HT(高温)相变温度。根据电子顺磁共振(EPR)实验数据确定了 Gd 在 La0.99Gd0.01BWO6 结构中的两个独立位置。
{"title":"Features of the Structure and Thermal Properties of Borate Tungstates LnBWO6 (Ln = La; La0.999Nd0.001 and La0.99Gd0.01) Synthesized by the Sol–Gel Method","authors":"V. A. Krut’ko, M. G. Komova, R. D. Svetogorov, A. V. Khoroshilov, N. N. Efimov, E. A. Ugolkova","doi":"10.1134/s0036023624600394","DOIUrl":"https://doi.org/10.1134/s0036023624600394","url":null,"abstract":"<h3 data-test=\"abstract-sub-heading\">Abstract</h3><p>Borate tungstates LnBWO<sub>6</sub> (Ln = La; La<sub>0.999</sub>Nd<sub>0.001</sub> and La<sub>0.99</sub>Gd<sub>0.01</sub>) are synthesized by the Pechini method followed by annealing of the intermediates and examined by X-ray diffraction (XRD) and differential scanning calorimetry (DSC). The crystallographic parameters of the synthesized LnBWO<sub>6</sub> are refined by powder X-ray diffraction in two crystal systems: monoclinic (space group <i>P</i>2<sub>1</sub>) and orthorhombic (space group <i>P</i>222). Reversible first-order phase transitions in the synthesized LnBWO<sub>6</sub> are detected by the DSC method, and the temperatures and enthalpies of phase transformations are determined. The doping of LnBWO<sub>6</sub> with Nd<sup>3+</sup> and Gd<sup>3+</sup> ions is shown to decrease the temperature of the LT (low-temperature) → HT (high-temperature) phase transition of LaBWO<sub>6</sub>. Two independent positions of Gd in the La<sub>0.99</sub>Gd<sub>0.01</sub>BWO<sub>6</sub> structure are determined from the experimental electron paramagnetic resonance (EPR) data.</p>","PeriodicalId":762,"journal":{"name":"Russian Journal of Inorganic Chemistry","volume":"74 1","pages":""},"PeriodicalIF":2.1,"publicationDate":"2024-07-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141863661","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
In situ Synthesis of Nano-CeO2 Composite with Chitosan 与壳聚糖原位合成纳米二氧化钴复合材料
IF 2.1 3区 化学 Q3 CHEMISTRY, INORGANIC & NUCLEAR Pub Date : 2024-07-31 DOI: 10.1134/s0036023624600515
L. A. Zemskova, V. E. Silant’ev, D. Kh. Shlyk

Abstract

Nanosized cerium oxide (CeO2) particles were prepared by co-precipitation using chitosan as a template, cerium(III) nitrate and cerium(IV) sulfate as starting substances, and aqueous ammonia as a precipitating agent. According to powder X-ray diffraction data, cerianite with face-centered cubic phase is formed in the reaction systems. The size of the coherent scattering regions is not more than ⁓3 nm. Fourier transform IR spectroscopy data indicate to interaction of polymer molecules with the inorganic component. The shift of N–H absorption bands for composites containing Ce(III) and Ce(IV) compared to those of chitosan indicates that amino groups interact with CeO2 particles loaded in the polymer. The use of chitosan as a matrix for the synthesis of CeO2 nanoparticles showed that this approach is more economical and facile to produce nanomaterials for various applications.

摘要 以壳聚糖为模板,硝酸铈(III)和硫酸铈(IV)为起始物质,氨水为沉淀剂,采用共沉淀法制备了纳米氧化铈(CeO2)颗粒。根据粉末 X 射线衍射数据,反应体系中形成了面心立方相的铈镧矿。相干散射区的大小不超过 ⁓3 nm。傅立叶变换红外光谱数据表明聚合物分子与无机成分发生了相互作用。与壳聚糖相比,含有 Ce(III) 和 Ce(IV) 的复合材料的 N-H 吸收带发生了移动,这表明氨基与聚合物中的 CeO2 颗粒发生了相互作用。使用壳聚糖作为合成 CeO2 纳米粒子的基质表明,这种方法更经济、更容易生产出用于各种应用的纳米材料。
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引用次数: 0
Synthesis of La2Ti2O7 Nanoscale Powder and Ceramics Based on It by Sol–Gel Synthesis and Spark Plasma Sintering 通过溶胶-凝胶合成和火花等离子烧结法合成 La2Ti2O7 纳米粉末及其陶瓷材料
IF 2.1 3区 化学 Q3 CHEMISTRY, INORGANIC & NUCLEAR Pub Date : 2024-07-31 DOI: 10.1134/s0036023624600424
O. O. Shichalin, E. K. Papynov, A. A. Belov, K. A. Pervakov, S. S. Gribanova, S. M. Pisarev, A. N. Fedorets, A. V. Pogodaev, A. O. Lembikov, Ya. G. Zernov, P. A. Marmaza, O. V. Kapustina, E. A. Gridasova, I. Yu. Buravlev

Abstract

The use of ceramics as matrices for immobilization of radionuclides for the purpose of their safe long-term disposal or useful application is studied with an emphasis placed on phase stability, structural integrity, hydrolytic stability, etc. This work implements a combined approach based on the sol–gel citrate synthesis of nanosized La2Ti2O7 powder and its subsequent spark plasma sintering to produce dense ceramics. The phase composition and structure of the nanosized La2Ti2O7 powder and the ceramic samples obtained in the temperature range of 900–1300°C were studied by powder X-ray diffraction and SEM. It was shown that the conditions of synthesis of the powder ensure the formation of nanosized crystalline La2Ti2O7 grains, consolidation of which under spark plasma heating is accompanied by a change in the phase composition of La2Ti2O7 from a single-phase monoclinic structure to orthorhombic structure with a LaTiO3 impurity at temperatures above 1200°C. It was found that a change in the ceramic structure is accompanied by the formation of non-porous and defect-free monolithic samples. This type of change was shown to lead to an increase in the relative density (81.3–95.7%) and compressive strength (78–566 MPa) of the ceramics. However, the hydrolytic stability decreases, as indicated by increasing La3+ leaching rate from 10–7 to 10–5 g/(cm2 day). The obtained results are useful for the systematic study of materials suitable for immobilization of radioactive waste in ceramics.

摘要 研究了利用陶瓷作为固定放射性核素的基质,以实现长期安全处置或有用应用的目的,重点是相稳定性、结构完整性、水解稳定性等。这项工作采用了一种基于柠檬酸溶胶-凝胶法合成纳米级 La2Ti2O7 粉末的组合方法,并随后采用火花等离子烧结法生产致密陶瓷。通过粉末 X 射线衍射和扫描电镜研究了纳米 La2Ti2O7 粉末和在 900-1300°C 温度范围内获得的陶瓷样品的相组成和结构。结果表明,粉末的合成条件确保了纳米级结晶 La2Ti2O7 晶粒的形成,在火花等离子体加热条件下,这些晶粒固结的同时,La2Ti2O7 的相组成也发生了变化,从单相单斜结构变为温度高于 1200°C 时带有 LaTiO3 杂质的正方体结构。研究发现,陶瓷结构的变化伴随着无孔和无缺陷整体样品的形成。这种变化导致陶瓷的相对密度(81.3%-95.7%)和抗压强度(78-566 兆帕)增加。然而,正如 La3+ 浸出率从 10-7 g/(cm2 天)增加到 10-5 g/(cm2 天)所表明的那样,水解稳定性降低了。所获得的结果有助于系统研究适合在陶瓷中固定放射性废物的材料。
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引用次数: 0
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Russian Journal of Inorganic Chemistry
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