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Mechanistic Insights into the Interaction between Strätlingite and I–/IO3–: Implications on the Iodine Migration in Alkali-Activated Slag Cement Strätlingite与I - /IO3 -相互作用的机理:对碱活化矿渣水泥中碘迁移的影响
IF 4.6 2区 化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR Pub Date : 2026-02-01 DOI: 10.1021/acs.inorgchem.5c04919
Binglin Guo,Cheng Wang,Ping Ye,Huyong Qin,Yuting Chu,Kaixuan Wang,Hengjun Mei,Peng Gao,Binggen Zhan,Qijun Yu,Keiko Sasaki,Yogarajah Elakneswaran
Alkali-activated slag cement (AAS) is a sustainable and promising matrix for immobilizing radioactive wastes. Strätlingite (siliceous AFm-type phase), a typical hydration product in AAS, plays a crucial role in stabilizing anionic species. However, the immobilization mechanisms of iodine species within strätlingite remain unclear. In this study, strätlingite demonstrated a greater affinity for IO3– than I–, with adsorption capacities of 0.291 and 0.0016 mmol/g, respectively. Approximate site energy distribution revealed a more diverse energy partitioning of adsorption sites for IO3– than I–, and strong interactions between IO3– and Ca sites through O–Ca bonds forming. Conversely, the differential charge density between I– and Ca sites was weak. The surface adsorption energy of IO3– to Ca sites was −5.05 eV, substantially higher than the −1.08 eV for I– adsorption. A stronger overlap between the 2p orbitals of O atoms and the 3d orbitals of Ca was observed upon IO3– adsorption than I– adsorption. Moreover, the anion selectivity of strätlingite followed the order: CO32– > SO42– ≥ IO3– > OH– > Cl– > NO3– ≥ I–. These findings provide valuable insights into the migration behavior of iodine species in repositories and alkaline environments.
碱活性矿渣水泥(AAS)是一种可持续的、有前景的放射性废物固定化基质。Strätlingite(硅质afm型相)是原子吸收光谱中典型的水化产物,在稳定阴离子中起着至关重要的作用。然而,碘在strätlingite内的固定机制尚不清楚。在本研究中,strätlingite对IO3 -的亲和力大于I -,吸附量分别为0.291和0.0016 mmol/g。近似的位置能量分布揭示了IO3 -吸附位点的能量分配比I -更多样化,并且IO3 -和Ca位点之间通过O-Ca键形成强相互作用。相反,I -和Ca位点之间的电荷密度差很弱。IO3 -对Ca的表面吸附能为- 5.05 eV,明显高于I -吸附能的- 1.08 eV。在IO3 -吸附过程中,O原子的2p轨道与Ca原子的3d轨道之间的重叠比I -吸附过程中更明显。strätlingite的阴离子选择性顺序为:CO32 - > SO42 -≥IO3 - > OH - > Cl - > NO3 -≥I -。这些发现为碘在储存库和碱性环境中的迁移行为提供了有价值的见解。
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引用次数: 0
Elevation from Binary to Ternary Resistive Switching Behaviors in Cubane-like Copper Iodide Clusters by Ligand Engineering 基于配体工程的类古巴铜碘化团簇从二元到三元电阻开关行为的提升
IF 4.6 2区 化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR Pub Date : 2026-02-01 DOI: 10.1021/acs.inorgchem.5c04773
Xueru Zhou,Yanfeng Du,Lintao Fan,Yuanzheng Liu,Junwei Liang,Zefeng Ma,Haohong Li,Huidong Zheng
Multilevel memory is a feasible solution for the explosive demand for data storage in the Big Data era. In this work, ligand engineering has been implemented in cubane-type Cu4I4L4 clusters to obtain three complexes: Cu4I4L4 (L = P(Ph-p-Cl)3 (1), PPh3 (2), P(Ph-p-OCH3)3 (3)), in which the substitutes on the p-position of benzyl vary from electron-withdrawing (–Cl) to electron-donating (−OCH3) groups. Interestingly, with enhancement of electron-donating ability, the trend of more distorted Cu4I4 cores, enhanced Cu···Cu interactions, and higher structural dimensions can be achieved. Consequently, in FTO/Cu4I4L4/Ag memristors, the electron-withdrawing group (–Cl) and neutral group (–H) exhibit bistable resistive switching performances, and a strong electron-donating group (−OCH3) can give ternary resistive switching behavior (OFF/ON1/ON2 current ratio: 1:102.74:103.73, VSet1/VSet2: 1.09/1.48 V). The mechanism about the elevation from binary to ternary memory behavior in these cubane-like Cu4I4L4 clusters has been clarified: the external voltage-induced I···Cl halogen bonding and C–H···π interaction contribute to the binary resistive switching performances in FTO/1/Ag and FTO/2/Ag, and the presence of the second conductive state in FTO/3/Ag stems from the injected carrier delocalization on the Cu4I4 core due to strong Cu···Cu interactions. The rules drawn in this work can provide a feasible strategy for the design of novel multilevel memories.
多层次存储是大数据时代数据存储爆发式需求的可行解决方案。在本研究中,对Cu4I4L4型Cu4I4L4簇进行了配体工程,得到了Cu4I4L4 (L = P(Ph-p-Cl)3 (1), PPh3 (2), P(Ph-p-OCH3)3(3))三种配合物,其中苯基P位上的取代基从吸电子(-Cl)到供电子(-OCH3)变化。有趣的是,随着给电子能力的增强,Cu4I4核的畸变程度增加,Cu···Cu相互作用增强,结构尺寸增大。因此,在FTO/Cu4I4L4/Ag记忆电阻器中,吸电子基团(-Cl)和中性基团(-H)表现出双稳态电阻开关性能,强供电子基团(−OCH3)可以表现出三相电阻开关性能(OFF/ON1/ON2电流比:1:10 . 2.74:103.73,VSet1/VSet2: 1.09/1.48 V)。在这些类立方体Cu4I4L4簇中,由二元记忆行为提升到三元记忆行为的机制已经被阐明:外部电压诱导的I··Cl卤素键和C-H··π相互作用有助于FTO/1/Ag和FTO/2/Ag的二元电阻开关性能,而FTO/3/Ag中第二导电状态的存在源于Cu···Cu强相互作用在Cu4I4核心上注入的载流子离域。研究结果为新型多层存储器的设计提供了一种可行的策略。
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引用次数: 0
Electron Donor Regulation in A-D-A Type Metal-Organic Frameworks for Enhancing Visible-Light Driven Photocatalysis. A-D-A型金属-有机骨架中电子供体调控以增强可见光驱动光催化。
IF 4.6 2区 化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR Pub Date : 2026-01-31 DOI: 10.1021/acs.inorgchem.5c06064
Mingxue Shao,Huadong Guo,Chunyu Liu,Rao Bao,Song Wang,Xianmin Guo
Charge separation efficiency is the determinant factor for reactive oxygen species (ROS) involved in photocatalytic aerobic oxidation reaction. Metal-organic frameworks (MOFs) provided a formidable platform for designing a donor-acceptor (D-A) system with tunable photoexcited carrier dynamics. Herein, we reported a series of UiO-68 type MOFs (termed as UiO-68-A-D1-A, UiO-68-A-D2-A, and UiO-68-A-D3-A) based on linearly bridged bis-benzothiadiazole as A-D-A linkers. Experimental and density functional theory calculations revealed that regulating the donor units from benzene to naphthalene and anthracene with gradually improved electron-donating capacity significantly enhanced the photogenerated charge separation and transfer efficiency and hence facilitated the ROS generation. As expected, anthracene-containing UiO-68-A-D3-A displayed the highest activity for the visible-light driven aerobic oxidation of benzylamines coupling. This work demonstrated that linker engineering of D-A molecular junctions in MOFs by fine-tuning the electronic nature of donor and acceptor units and their connection mode is a promising strategy to develop novel photocatalysts for efficient organic transformation.
电荷分离效率是光催化好氧反应中活性氧(ROS)的决定因素。金属有机骨架(MOFs)为设计具有可调谐光激发载流子动力学的供体-受体(D-A)系统提供了一个强大的平台。在此,我们报道了一系列UiO-68型mof(称为UiO-68- a - d1 - a, UiO-68- a - d2 - a和UiO-68- a - d3 - a)基于线性桥接的双苯并噻唑作为a - d - a连接体。实验和密度泛函理论计算表明,调节从苯到萘和蒽的供体单元,使其给电子能力逐渐提高,可以显著提高光生电荷分离和转移效率,从而促进ROS的生成。正如预期的那样,含蒽的UiO-68-A-D3-A在可见光驱动下对苄胺偶联的有氧氧化表现出最高的活性。这项工作表明,通过微调供体和受体单元的电子性质及其连接模式来实现mof中D-A分子连接的连接工程是开发高效有机转化的新型光催化剂的一种有前途的策略。
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引用次数: 0
A-Site Solid Solution Effects on Electrical Resistivity, Oxidation Resistance, and Hardness of MAX Phases V2(As1-xPx)C and V2(As1-xGex)C. a位固溶体对MAX相V2(As1-xPx)C和V2(As1-xGex)C电阻率、抗氧化性和硬度的影响
IF 4.6 2区 化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR Pub Date : 2026-01-31 DOI: 10.1021/acs.inorgchem.5c04921
Arya Loloee,Manuel Scharrer,Tullio S Geraci,Hui-Fei Zhai,Matt S Flores,Prajna Bhatt,Aysha A Riaz,Pardeep K Thakur,Tien-Lin Lee,Anna Regoutz,Jakoah Brgoch,Jason F Khoury,Alexandra Navrotsky,Christina S Birkel
MAX phases are a class of compounds known for having both metallic and ceramic properties, such as good electrical conductivity, oxidation resistance, and high hardness. The bulk of the research on their properties focuses on those with titanium at the M-site and metals from groups 13 to 15, e.g., aluminum, at the A-site. Here, we expand the properties repertoire with new arsenic-containing A-site solid solutions, V2(As1-xPx)C and V2(As1-xGex)C. The structure and elemental composition of the solid solutions were resolved with powder X-ray diffraction, scanning electron microscopy with energy-dispersive X-ray spectroscopy, and hard X-ray photoelectron spectroscopy. The electrical resistivity measurements show that both full series are metallic with the parent phases being the most conductive. Thermal analyses show V2GeC is the most oxidation resistant and V2AsC is the least, while substitutions decrease thermal stability, as oxidation resistance of the intermediate compositions shifts toward that of V2AsC. The V2(As1-xGex)C series shows little variation in hardness across compositions, while the incorporation of phosphorus noticeably increases hardness.
MAX相是一类已知具有金属和陶瓷性能的化合物,如良好的导电性、抗氧化性和高硬度。对其性质的大部分研究集中在钛在m位点和金属从13到15族,如铝,在a位点。在这里,我们用新的含砷a位固溶体V2(As1-xPx)C和V2(As1-xGex)C扩展了性质库。采用粉末x射线衍射、扫描电镜x射线能谱和硬x射线光电子能谱分析了固溶体的结构和元素组成。电阻率测量表明,这两个全系列都是金属的,母相的导电性最好。热分析表明,V2GeC的抗氧化性最强,而V2AsC的抗氧化性最低,而取代产物的热稳定性降低,中间成分的抗氧化性向V2AsC的抗氧化性转移。V2(As1-xGex)C系列的硬度在各组分中变化不大,而磷的掺入明显提高了硬度。
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引用次数: 0
A Strategy to Enhance Luminescence in Photochromic Coordination Polymers for Multi-Mode Smart Displays. 一种用于多模式智能显示器的光致变色配位聚合物增强发光策略。
IF 4.6 2区 化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR Pub Date : 2026-01-30 DOI: 10.1021/acs.inorgchem.5c05473
Yi-Feng Yuan,Yan Lin,Meng-Ting He,Jin-Ju Zhai,Yuan-Qing Xu,Jun-Xia Liu,Zhong-Yan Cao,Peng-Fei Zhang,Meng-Hua Li
Photocontrollable luminescent materials with highly efficient emission properties offer promising application prospects in the field of intelligent switches, information security, etc. Herein, two stimulus-responsive CPs (CPs 1-2) have been successfully synthesized based on the photoactive TPT ligand (2,4,6-tris-4-pyridyl-1,3,5-triazine) via the solvothermal method. Remarkably, CPs 1-2 exhibit distinct photochromism coupled with photocontrollable luminescence behaviors. Furthermore, by employing an in situ doping strategy, lanthanide ions were immobilized within the pores of CP 2 to generate Eu/Tb@CP 2 composites, which display significantly enhanced fluorescence (QY increased from 0.49% to 16.5%) without compromising photochromic properties. Moreover, leveraging their dynamic, efficient, and multicolor luminescence, these compounds enable the realization of multimode smart displays. This work offers valuable insights for designing novel stimulus-responsive materials with efficient and color-tunable luminescence via in situ doping strategies, thereby advancing the development of photochromic materials toward practical applications in multilevel information display and advanced data encryption.
具有高效发射特性的光可控发光材料在智能开关、信息安全等领域具有广阔的应用前景。本文以具有光活性的TPT配体(2,4,6-三-4-吡啶-1,3,5-三嗪)为基础,通过溶剂热法成功合成了两个刺激响应的CPs (CPs 1-2)。值得注意的是,CPs 1-2具有明显的光致变色和光可控发光行为。此外,采用原位掺杂策略,将镧系离子固定在CP 2的孔内,生成Eu/Tb@CP 2复合材料,其荧光(QY从0.49%增加到16.5%)显着增强,而不影响光致变色性能。此外,利用其动态,高效和多色发光,这些化合物能够实现多模式智能显示器。这项工作为通过原位掺杂策略设计具有高效和颜色可调发光的新型刺激响应材料提供了有价值的见解,从而推动了光致变色材料在多层次信息显示和高级数据加密方面的实际应用。
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引用次数: 0
Exceptional Long-Term Stability in Hydrogen Evolution via Defect-Engineered MIL-100 Synthesized by Controlled Thermolysis. 通过控制热裂解合成的缺陷工程MIL-100在氢演化中的特殊长期稳定性。
IF 4.6 2区 化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR Pub Date : 2026-01-30 DOI: 10.1021/acs.inorgchem.5c04976
Minoo Bagheri,Fatemeh Momeni,Mohammad Yaser Masoomi
Two quasi-iron-based metal-organic frameworks, Q-MIL-100 and Q-MIL-101, were prepared via thermal partial deligandation to create large-scale structural defects. This pore engineering enhanced the density of unsaturated iron sites and created hierarchical porosity, serving as active centers for the catalytic hydrogen generation from NaBH4 hydrolysis. While pristine MIL-101 demonstrated higher activity than MIL-100, defect engineering reversed this trend, resulting in Q-MIL-100 achieving a superior hydrogen generation rate of 5360 mL·min-1·g-1 at 298 K, compared to 3360 mL·min-1·g-1 for Q-MIL-101. This enhanced performance is attributed to the synergistic combination of accessible active sites and an optimally restructured hierarchical pore architecture. Thermal activation to 313 K dramatically enhanced the hydrogen generation rates to 12,160 and 10,160 mL·min-1·g-1 for Q-MIL-100 and Q-MIL-101, respectively─a 2.3- to 3.0-fold increase over their performance at 298 K. The calculated activation energies were 41.7 kJ·mol-1 for Q-MIL-100 and 56.2 kJ·mol-1 for Q-MIL-101. A kinetic isotope effect indicated that the O-H bond cleavage in water was the rate-determining step. Q-MIL-100 demonstrated exceptional stability, retaining 92% of its initial activity after 16 reuse cycles. This work highlights the novel long-term stability of the engineered catalyst for practical hydrogen generation.
采用热局部委托法制备了两种准铁基金属有机骨架Q-MIL-100和Q-MIL-101,以制造大规模的结构缺陷。这种孔隙工程增强了不饱和铁位点的密度,并形成了分层孔隙,作为催化NaBH4水解制氢的活性中心。虽然原始的MIL-101表现出比MIL-100更高的活性,但缺陷工程逆转了这一趋势,导致Q-MIL-100在298 K下获得了5360 mL·min-1·g-1的更好的氢生成速率,而Q-MIL-101则为3360 mL·min-1·g-1。这种增强的性能归因于可访问的活性位点和优化重组的分层孔隙结构的协同结合。热活化至313 K时,Q-MIL-100和Q-MIL-101的产氢率分别显著提高至12,160和10,160 mL·min-1·g-1,比298 K时的产氢率提高了2.3至3.0倍。Q-MIL-100和Q-MIL-101的活化能分别为41.7 kJ·mol-1和56.2 kJ·mol-1。动力学同位素效应表明,氧氢键在水中的裂解是反应速率的决定步骤。Q-MIL-100表现出优异的稳定性,在16次重复使用后仍保持了92%的初始活性。这项工作强调了用于实际制氢的工程催化剂的新型长期稳定性。
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引用次数: 0
EXAFS Analysis of Ru265 and Ru360 in Human Blood. 人血液中Ru265和Ru360的EXAFS分析。
IF 4.6 2区 化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR Pub Date : 2026-01-30 DOI: 10.1021/acs.inorgchem.5c05608
Ani T Baker,James H Lovett,Haipei Zou,Justin J Wilson,Hugh H Harris
The dinuclear ruthenium (Ru) compounds Ru265 and Ru360 are inhibitors of the mitochondrial calcium uniporter (MCU) and potential therapeutic agents for conditions associated with mitochondrial calcium (mt-Ca2+) dysregulation. The nitrido-bridged Ru265 offers improved cell permeability and redox stability relative to the oxo-bridged analogue, Ru360, while maintaining high selectivity and potency. In this study, extended X-ray absorption fine-structure (EXAFS) spectroscopy interrogated the stability of these compounds in buffer, saline/DMSO solutions, and human blood by probing the sensitive Ru─X─Ru scattering signal. Both dinuclear compounds remained intact in a pH 7.4 buffered solution, even in the presence of glutathione (5 mol equiv). Following addition to whole blood, EXAFS identified the presence of diaqua-capped Ru265', indicating axial ligand substitution but confirming stability of the Ru─N─Ru backbone during incubation (1 h, 37 °C). In contrast, Ru360' rapidly degraded in saline/DMSO at room temperature, as evidenced by the diminished intensity of the Ru···Ru peak at ∼3.65 Å in the EXAFS Fourier transform. Subsequently, the mononuclear Ru360' degradation products displayed negligible uptake into red blood cells. These findings support previous studies highlighting the improved stability of Ru265 and provide validation of the structure and coordination environment of the complex in an ex vivo human blood sample.
双核钌(Ru)化合物Ru265和Ru360是线粒体钙单转运体(MCU)的抑制剂,也是线粒体钙(mt-Ca2+)失调相关疾病的潜在治疗剂。与氧桥接类似物Ru360相比,氮桥接的Ru265具有更好的细胞渗透性和氧化还原稳定性,同时保持了高选择性和效力。在这项研究中,扩展X射线吸收精细结构(EXAFS)光谱通过探测敏感的Ru─X─Ru散射信号来询问这些化合物在缓冲液、生理盐水/DMSO溶液和人体血液中的稳定性。两种双核化合物在pH 7.4的缓冲溶液中保持完整,即使在谷胱甘肽(5摩尔当量)的存在下也是如此。在全血中添加后,EXAFS发现了双水帽Ru265'的存在,表明轴向配体取代,但证实了Ru─N─Ru主链在孵育期间(1小时,37°C)的稳定性。相反,室温下,Ru360'在盐水/DMSO中迅速降解,EXAFS傅里叶变换中Ru···Ru峰在~ 3.65 Å处强度减弱。随后,单核Ru360降解产物被红细胞吸收的情况可以忽略不计。这些发现支持了先前强调Ru265稳定性提高的研究,并在离体人类血液样本中验证了该复合物的结构和协调环境。
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引用次数: 0
Synthesis, Characterization, and Polymerization of Ge- and Sn-Substituted [2.2]Paracyclophanes toward Poly(para-xylylene) Films and Their Mechanical Properties. 锗和锡取代[2.2]对环蒽的合成、表征和聚对二甲苯薄膜的聚合及其力学性能。
IF 4.6 2区 化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR Pub Date : 2026-01-30 DOI: 10.1021/acs.inorgchem.5c04945
Moena Hirao,Lukas Bichlmaier,Tetsuhiko F Teshima,Rebecca Wilhelm,Shigeyoshi Inoue
Polymers have had widespread applications in industry over the past few decades. Recently, polymers incorporating heavier group 14 elements (Ge, Sn, and Pb) have gained interest since their oxides are promising for semiconductor applications due to their high dielectric constants and charge mobility. Poly(p-xylylene) (PPX), an important class of polymer, is widely recognized for its transparency, biocompatibility, and the conformality afforded by its polymerization method, chemical vapor deposition (CVD). In this work, PPXs incorporating germanium or tin are prepared via CVD polymerization and the optimal pyrolysis temperatures of their precursors are determined. The ductility, thermal stability, crystallinity, surface topography, and comprehensive and surface chemical compositions are investigated. Sequential changes in the surface oxidation state are confirmed following exposure to air and subsequent oxygen plasma treatment. Comparison of the obtained PPXs with the widely applied chlorinated version PPX-Cl (trade name Parylene C) revealed preserved ductility while exhibiting distinct trends in softness.
在过去的几十年里,聚合物在工业上得到了广泛的应用。最近,含有较重的14族元素(Ge, Sn和Pb)的聚合物引起了人们的兴趣,因为它们的氧化物由于其高介电常数和电荷迁移率而在半导体应用中有前景。聚(对二甲苯)(PPX)是一类重要的聚合物,因其透明、生物相容性和化学气相沉积(CVD)聚合方法所提供的一致性而被广泛认可。本文通过CVD聚合法制备了含锗或锡的ppx,并确定了其前驱体的最佳热解温度。研究了材料的延展性、热稳定性、结晶度、表面形貌、综合化学成分和表面化学成分。暴露于空气和随后的氧等离子体处理后,表面氧化态的顺序变化得到证实。将得到的PPXs与广泛应用的氯化版本PPX-Cl(商品名聚对二甲苯C)进行比较,发现保留了延展性,同时表现出明显的柔软性趋势。
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引用次数: 0
Endohedral [Au@In10]9- Cluster: Synthesis and Characterization of Na3+xA6-xIn10Au (x = 0, 0.25; A = Rb, Cs). 内嵌体[Au@In10]9-簇:Na3+xA6-xIn10Au (x = 0,0.25; A = Rb, Cs)的合成与表征。
IF 4.6 2区 化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR Pub Date : 2026-01-30 DOI: 10.1021/acs.inorgchem.5c04619
Melissa Janesch,Florian Pielnhofer,Michal Dušek,Ilya G Shenderovich,Stefanie Gärtner
The synthesis and characterization of two new compounds Na3Rb6In10Au and Na3.25Cs5.75In10Au are reported, which contain [Au@In10]9- clusters as anionic entities. Single-crystal X-ray structure analysis shows that the alkali metal composition is the key factor for structure formation, while the anionic entity remains unchanged. The chemical composition was confirmed by SEM/EDS measurements, and the given compositions of both compounds are fixed according to the line compounds. Quantum chemical calculations for the compound Na3Rb6In10Au were performed and show a band gap at the Fermi level, classifying the materials as salt-like, including endohedral [Au@In10]9- Zintl-type clusters. Dissolution experiments in liquid ammonia were carried out, revealing In2Au as the reaction product.
报道了两种新化合物Na3Rb6In10Au和Na3.25Cs5.75In10Au的合成和表征,它们含有[Au@In10]9-簇作为阴离子实体。单晶x射线结构分析表明,碱金属成分是结构形成的关键因素,而阴离子实体保持不变。经SEM/EDS测定,确定了两种化合物的化学组成,并根据谱线确定了两种化合物的给定组成。对化合物Na3Rb6In10Au进行了量子化学计算,并在费米能级上显示了一个带隙,将材料分类为盐状,包括内嵌[Au@In10]9- zintl型簇。在液氨中进行了溶解实验,发现反应产物为In2Au。
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引用次数: 0
A DFT Re-Examination of the Acid Catalyzed Aquation of Hexaammineruthenium(II), Ru(NH3)62. 钌(NH3)62酸催化水化反应的DFT复核。
IF 4.6 2区 化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR Pub Date : 2026-01-30 DOI: 10.1021/acs.inorgchem.5c04087
Leroy E Laverman,Kalju Kahn,Peter C Ford
Described are multiple approaches using density functional theory to probe the acid catalyzed aquation of the hexaammineruthenium(II) cation (Ru(NH3)62+ + H3O+ → Ru(NH3)5(H2O)2+ + NH4+) reported initially by Taube and co-workers. These computations support the proposal that the initial step is protonation of the Ru(II) center and/or the metal-NH3 bond, thereby activating the latter toward dissociation. DFT analysis was also carried out for the hypothetical acid-mediated aquation of the isoelectronic hexaamminerhodium(III) complex, Rh(NH3)63+. The computations suggest a key mechanistic difference for the latter pathway, namely that protonation of the NH3 occurs late in a reaction coordinate involving dissociation of the Rh-NH3 with no direct interaction of H+ with the metal center. Furthermore, while the calculated activation energy is considerably higher in the latter case, the calculations suggest that protonation could play an important role in such ligand substitution reactions.
描述了多种方法,使用密度泛函理论来探测酸催化的六胺矿铵(II)阳离子(Ru(NH3)62+ + h30 +→Ru(NH3)5(H2O)2+ + NH4+)的水化,最初由Taube和同事报道。这些计算支持了最初步骤是Ru(II)中心和/或金属- nh3键的质子化,从而激活后者解离的建议。DFT分析还进行了假设的酸介导的六胺矿(III)配合物Rh(NH3)63+的水化。计算表明了后一种途径的关键机制差异,即NH3的质子化发生在涉及Rh-NH3解离的反应坐标的后期,而H+与金属中心没有直接相互作用。此外,虽然后一种情况下计算的活化能要高得多,但计算表明质子化可能在这种配体取代反应中起重要作用。
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引用次数: 0
期刊
Inorganic Chemistry
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