Dalton Transactions最新文献

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Synthesis and catalytic activity of heterobimetallic Au/M (M = RhIII, IrIII) complexes with ditopic mono- and triphosphane ligands 具有二价单膦和三膦配体的杂多金属 Au/M（M = RhIII、IrIII）配合物的合成与催化活性

IF 4 3区化学 Q1 Chemistry

Dalton Transactions

Pub Date : 2024-06-26 DOI: 10.1039/d4dt01247j

Ivana Predarska, Wieland Körber, Peter Lönnecke, Dmitri Gelman, Evamarie Hey-Hawkins

A series of heterobimetallic complexes Au/M (M = RhIII, IrIII) were prepared on the basis of two ditopic ligands: a monophosphane ligand L1H and a triphosphane ligand L2H. The complexes were fully characterised, including single-crystal X-ray diffraction studies. Catalytic activity of cationic L1/AuI/IrIII and L2/AuI/IrIII bis(trifluoromethane)sulfonimide was analysed through their capacity to induce allenyl ether rearrangement and cycloisomerisation of N-propargyl benzamide. While cationic L1/AuI/IrIII showed some ability to induce allenyl ether rearrangement, no conversion was observed for cationic L2/AuI/IrIII. Similarly, N-propargyl benzamide could undergo cycloisomerisation in the presence of cationic L1/AuI/IrIII, whereas cationic L2/AuI/IrIII was again inactive. These findings highlight how crucial the surroundings of the metal centre are to the catalytic activity. Catalytic activity is only possible when Au has a free coordination site; the gold complex becomes inactive when the tridentate ligand is present.

以两种二价配体（一膦烷配体 L1H 和三膦烷配体 L2H）为基础，制备了一系列异二金属配合物 Au/M（M = RhIII、IrIII）。对这些配合物进行了全面的表征，包括单晶 X 射线衍射研究。通过分析阳离子 L1/AuI/IrIII 和 L2/AuI/IrIII 双（三氟甲烷）磺酰亚胺诱导异烯醚重排和 N-丙炔基苯甲酰胺环异构化的能力，分析了它们的催化活性。阳离子 L1/AuI/IrIII 显示出一定的诱导异烯醚重排的能力，而阳离子 L2/AuI/IrIII 则未观察到任何转化。同样，在阳离子 L1/AuI/IrIII 的存在下，N-丙炔基苯甲酰胺可以发生环异构化，而阳离子 L2/AuI/IrIII 则没有活性。这些发现凸显了金属中心周围环境对催化活性的重要性。只有当金具有自由配位位点时，才可能产生催化活性；当存在三叉配体时，金配合物就失去活性。

引用次数: 0

F-block hydride complexes – Synthesis, Structure and Reactivity F 块氢化物配合物 - 合成、结构和反应活性

IF 4 3区化学 Q1 Chemistry

Dalton Transactions

Pub Date : 2024-06-26 DOI: 10.1039/d4dt00776j

Nicola L. Bell, Richard Drummond Turnbull

Complexes formed between the heaviest and lightest elements in the periodic table yield the f-block hydrides, a unique class of compounds with wide ranging utility and interest, from catalysis to light responsive materials and nuclear waste storage. Recent developments in syntheses and analytics such as exploiting low oxidation state metal ions and improvements in X-ray diffraction tools have transformed our ability to understand, access and manipulate these important species. This perspective brings together insights from binary metal hydrides, with molecular solution phase studies on heteroleptic complexes and gas phase investigations with the aim of providing an overview of how the f-element influences hydride formation, structure and reactivity as well as elucidating the power of co-ligands to tune their behaviour towards a variety of applications.

元素周期表中最重和最轻的元素之间形成的络合物产生了 f 块氢化物，这是一类独特的化合物，具有广泛的用途和意义，从催化到光敏材料和核废料储存。最近在合成和分析方面的发展，如利用低氧化态金属离子和改进 X 射线衍射工具，改变了我们理解、获取和处理这些重要物种的能力。本研究汇集了二元金属氢化物、异性配合物的分子溶液相研究和气相研究的见解，旨在概述 f 元素如何影响氢化物的形成、结构和反应性，以及阐明共配体在调整其行为以适应各种应用方面的能力。

引用次数: 0

Chemical composition-induced evolution of the structure, domain and electrical properties of Sm-doped (1 - x)Pb(Ni_1/3Nb_2/3)O₃-xPbTiO₃. 化学成分诱导的掺杂 Sm 的 (1 - x)Pb(Ni1/3Nb2/3)O3-xPbTiO3 结构、畴和电学特性的演变。

IF 3.5 3区化学 Q1 Chemistry

Dalton Transactions

Pub Date : 2024-06-26 DOI: 10.1039/d4dt01398k

Haoran Yu, Jian Guo, Jiajia Wang, Ji Zhang, Shan-Tao Zhang

As the two typical basic binary solid solutions of the relaxor-PbTiO₃ family, Pb(Mg_1/3Nb_2/3)O₃-PbTiO₃ (PMN-PT) has been widely investigated, whereas Pb(Ni_1/3Nb_2/3)O₃-PbTiO₃ (PNN-PT) has not. Here, 1.5 mol% Sm-doped (1 - x)Pb(Ni_1/3Nb_2/3)O₃-xPbTiO₃, (1 - x)PNN-xPT:0.015Sm with x = 0.33-0.39, ceramics have been prepared and the chemical composition-induced evolution of crystal structure, domain, and electrical properties investigated systematically. With increasing PT content, evolution of the rhombohedral-tetragonal structure was observed. A rhombohedral-tetragonal morphotropic phase boundary occurred around x = 0.36-0.37, which showed a peak piezoelectric property with piezoelectric constant d₃₃ = 531 pC N^-1 and planar electromechanical coupling factor k_p = 0.37 at room temperature. At the same time, the x = 0.36 composition showed improved ferroelectric behavior with remanent polarization P_r = 13.4 μC cm^-2 and coercive field E_c = 3.2 kV cm^-1. Interestingly, different from its PMN-PT counterpart, there is no temperature-driven phase transition between room temperature and the Curie temperature for (1 - x)PNN-xPT:0.015Sm. These parameters indicated that the PNN-PT system is worthy of more attention and is a promising platform for further development of high-performance piezo/ferroelectric materials.

Pb(Mg1/3Nb2/3)O3-PbTiO3 (PMN-PT)和 Pb(Ni1/3Nb2/3)O3-PbTiO3 (PNN-PT)是弛豫体-PbTiO3家族中两种典型的基本二元固溶体，已被广泛研究，而 Pb(Ni1/3Nb2/3)O3-PbTiO3 (PNN-PT)则尚未被研究。本文制备了掺杂 1.5 mol% Sm 的（1 - x）Pb(Ni1/3Nb2/3)O3-xPbTiO3，即（1 - x）PNN-xPT:0.015Sm，x = 0.33-0.39，并系统地研究了化学成分诱导的晶体结构、畴和电性能演变。随着 PT 含量的增加，观察到了斜方四面体结构的演变。在 x = 0.36-0.37 附近出现了斜方体-四方体各向异性相界，在室温下显示出峰值压电特性，压电常数 d33 = 531 pC N-1，平面机电耦合因子 kp = 0.37。同时，x = 0.36 成分显示出更好的铁电行为，其剩磁极化 Pr = 13.4 μC cm-2 和矫顽力场 Ec = 3.2 kV cm-1。有趣的是，与 PMN-PT 不同，(1-x)PNN-xPT:0.015Sm 在室温和居里温度之间没有温度驱动的相变。这些参数表明，PNN-PT 系统值得更多关注，是进一步开发高性能压电/铁电材料的理想平台。

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引用次数: 0

A Pt nanoenzyme- and BODIPY-loaded nanoscale covalent organic framework for relieving intratumoural hypoxia to enhance photodynamic therapy 一种铂纳米酶和 BODIPY 负载纳米级共价有机框架，用于缓解瘤内缺氧以增强光动力疗法

IF 4 3区化学 Q1 Chemistry

Dalton Transactions

Pub Date : 2024-06-25 DOI: 10.1039/d4dt00999a

Kaixuan Zhang, Bo Wang, Wen-Yan Li, Yang Song, Tian Song, Yan-An Li, Yu-Bin Dong

Herein, we report a composite COF material loaded with a Pt nanoenzyme and an organic photosensitizer BODIPY, synthesized via a stepwise post-synthetic modification. The obtained Pt@COF-BDP nanoparticles can efficiently and continuously convert H2O2 to O2, thereby increasing the efficiency of single-linear oxygen production and achieving efficient tumor inhibition.

在此，我们报告了一种负载有铂纳米酶和有机光敏剂 BODIPY 的复合 COF 材料，该材料是通过分步后合成修饰合成的。所获得的 Pt@COF-BDP 纳米颗粒能高效、持续地将 H2O2 转化为 O2，从而提高单线制氧效率，达到高效抑制肿瘤的目的。

引用次数: 0

Emerging trends in the development and applications of triazine-based covalent organic polymers: a comprehensive review. 三嗪基共价有机聚合物的开发和应用新趋势：全面综述。

IF 3.5 3区化学 Q1 Chemistry

Dalton Transactions

Pub Date : 2024-06-25 DOI: 10.1039/d4dt01127a

Simran Aggarwal, Satish Kumar Awasthi

Owing to unique structural features, triazine-based covalent organic polymers (COPs) have attracted significant attention and emerged as novel catalysts or support materials for an array of applications. Typically formed by reacting triazine-based monomers or the in situ creation of triazine rings from nitrile monomers, these COPs possess 2D/3D meso/microporous structures held together via strong covalent linkages. The quest for efficient, stable and recyclable catalytic systems globally necessitates the need for a well-structured and comprehensive review summarizing the synthetic methodologies and applications of triazine-based COPs. This review explores the various synthetic routes and applications of these COPs in photocatalysis, heterogeneous catalysis, electrocatalysis, adsorption and sensing. By exploring the latest advancements and future directions, this review offers valuable insights into the synthesis and applications of triazine-based COPs.

三嗪基共价有机聚合物（COPs）因其独特的结构特征而备受关注，并已成为一系列应用领域的新型催化剂或支撑材料。这些 COPs 通常由三嗪基单体反应形成，或由腈类单体原位生成三嗪环，具有二维/三维中孔/微孔结构，通过强共价键连接在一起。全球对高效、稳定和可回收催化系统的需求促使我们需要一篇结构合理、内容全面的综述，总结基于三嗪的 COP 的合成方法和应用。本综述探讨了这些 COPs 的各种合成路线以及在光催化、异相催化、电催化、吸附和传感方面的应用。通过探讨最新进展和未来方向，本综述为三嗪基 COPs 的合成和应用提供了宝贵的见解。

引用次数: 0

Disentangling the “tip-effects” enhanced antibacterial mechanism of Ag nanoparticles 厘清银纳米粒子的 "尖端效应 "增强抗菌机制

IF 4 3区化学 Q1 Chemistry

Dalton Transactions

Pub Date : 2024-06-25 DOI: 10.1039/d4dt01173b

Shenli Wang, Yanping Zhang, Xuan Chen, Stefanos Mourdikoudis, Shengshi Fan, Haoyu Li, Sergio Gomez, Shuncheng Ren, Guangchao Zheng

: Silver nanoparticles (Ag NPs) exhibit strong antibacterial activity and are widely used in industries such as medical, food and cosmetics. In this study, Ag nanospheres and Ag nanotriangles are selected as antibacterial agents to reveal the distinct mechanism of tip effects towards their antibacterial performance. A series of antibacterial experiments were implemented, including in-situ monitoring as well as studying and determining of the evolution of the inhibition zone, minimum inhibitory concentration (MIC)/minimum bactericidal concentration (MBC) values, growth kinetics, bactericidal curve, bacterial morphologies and intracellular reactive oxygen species (ROS). Ag nanotriangles can eradicate E. coli and S. aureus at extremely low concentrations in comparison to Ag nanospheres, in particular under sunshine irradiation. The destroyed bacterial cell walls were examined by scanning electron microscopy. Through the investigation of ROS production, the generation efficiency of ROS is improved by the merit of sunshine irradiation thanks to the localized surface plasmon resonance (LSPR) property of Ag NPs. However, a more significant improvement of ROS generation efficiency occurred in the presence of Ag nanotriangles contributed by the pronounced “tip effects”. This study sheds light on the relationship of structure-performance for the rational design of antibacterial agents.

:银纳米粒子（Ag NPs）具有很强的抗菌活性，被广泛应用于医疗、食品和化妆品等行业。本研究选择银纳米球和银纳米三角形作为抗菌剂，以揭示尖端效应对其抗菌性能的独特机制。研究人员进行了一系列抗菌实验，包括原位监测以及研究和确定抑菌区的演变、最低抑菌浓度（MIC）/最低杀菌浓度（MBC）值、生长动力学、杀菌曲线、细菌形态和细胞内活性氧（ROS）。与纳米银球相比，纳米银矩阵能以极低的浓度根除大肠杆菌和金黄色葡萄球菌，尤其是在阳光照射下。用扫描电子显微镜检查了被破坏的细菌细胞壁。通过对 ROS 生成情况的研究发现，由于银纳米粒子的局部表面等离子体共振（LSPR）特性，ROS 的生成效率在阳光照射下得到了提高。然而，由于银纳米三角形具有明显的 "尖端效应"，ROS 生成效率的提高更为显著。这项研究为合理设计抗菌剂揭示了结构与性能之间的关系。

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引用次数: 0

Complex Isomerism Influencing the Texture Properties of Organometallic [Cu(salen)] Porous Polymers: Paramagnetic Solid-State NMR Characterization and Heterogeneous Catalysis 影响有机金属[Cu(salen)]多孔聚合物质地特性的络合物异构现象：顺磁固态核磁共振表征与异相催化

IF 4 3区化学 Q1 Chemistry

Dalton Transactions

Pub Date : 2024-06-25 DOI: 10.1039/d4dt01305k

David Šorm, Jan Blahut, Bogdana Bashta, Ivana Cisarova, Eva Vrbková, Eliska Vyskocilova, Jan Sedláček

While the organometallic porous polymer networks are recognized as promising heterogeneous catalysts, the relation between ligand/monomer geometry and network parameters is usually not well understood due to the lack of atom-resolved characterization methods in the amorphous network matrix. In this work, a series of copper(II) salen-type metal complexes was synthesized, using trans- and cis-1,2-diaminocyclohexane segments, and thoroughly characterized by single-crystal X-ray diffraction, solution- and solid-state NMR spectroscopy. Terminal ethynyl groups of the complexes were then transformed into polyacetylene chains by coordination chain-growth homopolymerization, resulting in highly porous (458–655 m²/g) organometallic polymer networks with copper(II) ions content of about 12 wt.%. The presence of paramagnetic copper(II) moieties in complexes and respective polymer networks required the application of tailored NMR techniques and together with X-ray crystallography and DFT calculations of the paramagnetic NMR shifts made it possible to investigate the differences of complex geometry in liquid, powder and crystalline form and compare it with complex geometry in polymer networks. All prepared organometallic polymer networks were also tested as heterogeneous catalysts of styrene oxidation with uncommonly high substrate conversions and compared with their low-molecular-weight analogues. The high reusability of such heterogeneous polymer-based catalysts was also proven.

虽然有机金属多孔聚合物网络被认为是一种前景广阔的异相催化剂，但由于缺乏对无定形网络基体进行原子分辨的表征方法，配体/单体几何形状与网络参数之间的关系通常并不十分清楚。本研究利用反式和顺式-1,2-二氨基环己烷段合成了一系列铜（II）沙林型金属配合物，并通过单晶 X 射线衍射、溶液和固态核磁共振光谱对其进行了全面表征。然后，通过配位链增长均聚合作用将复合物的末端乙炔基转化为聚乙炔链，从而得到铜（II）离子含量约为 12 wt.%的高多孔性（458-655 m2/g）有机金属聚合物网络。由于配合物和相应聚合物网络中存在顺磁性铜（II）分子，因此需要应用定制的核磁共振技术，并结合 X 射线晶体学和顺磁核磁共振位移的 DFT 计算，研究配合物在液态、粉末和晶体形态下的几何形状差异，并将其与聚合物网络中的配合物几何形状进行比较。所有制备的有机金属聚合物网络还作为苯乙烯氧化的异相催化剂进行了测试，其底物转化率之高实属罕见，并与它们的低分子量类似物进行了比较。研究还证明了这种基于异质聚合物的催化剂的高重复利用率。

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引用次数: 0

Na Ion-Exchanged Zirconium Phosphate Crystal with High Calcium Ion Selectivity 具有高钙离子选择性的 Na 离子交换磷酸锆晶体

IF 4 3区化学 Q1 Chemistry

Dalton Transactions

Pub Date : 2024-06-25 DOI: 10.1039/d4dt01289e

Fumitaka Hayashi, Yuka Shirasu, Kazunori Fujisawa, Mongkol Tipplook, Tetsuya Yamada, Katsuya Teshima

We demonstrate hydrothermally grown sodium hydrogen zirconium phosphate ((Na,H)-ZrP) crystals exhibiting high calcium ion selectivity. The standard Gibbs free energies for Ca²⁺ exchange on (Na,H)-ZrP and γ-type ZrP were estimated to be ‒10.1 and ‒4.69 kJ mol^-1, respectively. The high Ca²⁺ selectivity of (Na,H)-ZrP could be attributed to the size matching between the ion exchange site of (Na,H)-ZrP and Ca²⁺.

我们展示了水热法生长的磷酸氢锆钠（(Na,H)-ZrP）晶体，它具有很高的钙离子选择性。据估计，(Na,H)-ZrP 和 γ 型 ZrP 上 Ca2+ 交换的标准吉布斯自由能分别为 -10.1 和 -4.69 kJ mol-1。(Na,H)-ZrP对Ca2+的高选择性可归因于(Na,H)-ZrP的离子交换位点与Ca2+之间的尺寸匹配。

引用次数: 0

Efficient narrowband yellow organic light-emitting diodes based on iridium(III) complexes with rigid indolo[3,2,1-jk]carbazole unit 基于具有刚性吲哚并[3,2,1-jk]咔唑单元的铱(III)配合物的高效窄带黄色有机发光二极管

IF 4 3区化学 Q1 Chemistry

Dalton Transactions

Pub Date : 2024-06-25 DOI: 10.1039/d4dt01018c

Qi-Ming Liu, Xiao-Jia Liu, Xiao-Sheng Zhong, Zhong-Zhong Huo, Zhen Shen, You-Xuan Zheng

Phosphorescent material with narrowband emission is crucial for advancing wide-color-gamut organic light-emitting diode (OLED). In this work, two iridium(III) complexes, (PhthzICz)2Ir(tmd) and (thzICz)2Ir(tmd), using rigid 2-(benzothiazole-2-yl)indolo[3,2,1-jk]carbazole (PhthzICz) and 2-(thiazole-2-yl)indolo[3,2,1-jk]carbazole (thzICz) as cyclometalated ligands and 2,2,6,6-tetramethyl-3,5-heptanedione (tmd) as ancillary ligands were synthesized. When these complexes were doped into the host material 3,3′-di(9H-carbazol-9-yl)-1,1′-biphenyl, the doped films exhibit yellow photoluminescence (PL) peaking at 537 and 531 nm, full width at half maximum (FWHM) bands of 35 and 60 nm, and PL quantum yields of 89.9% and 85.9%, respectively. OLEDs based on these two emitters display moderate performance characteristics with maximum external quantum efficiencies of 25.2% and 22.7%. Notably, the device based on (PhthzICz)2Ir(tmd) exhibits a narrow FWHM of 31 nm. Overall, the study highlights the practicality of incorporating rigid groups into the cyclometalated ligands of Ir(III) complexes as a viable strategy for achieving efficient Ir(III) complexes for OLEDs with narrow emission and high efficiency.

具有窄带发射的磷光材料对于推动宽色域有机发光二极管（OLED）的发展至关重要。在这项工作中，两种铱（III）配合物 (PhthzICz)2Ir(tmd) 和 (thzICz)2Ir(tmd) 以刚性 2-(苯并噻唑-2-基)吲哚并[3,2,1-jk]咔唑 (PhthzICz) 和 2-(噻唑-2-基)吲哚并[3、2,1-jk]咔唑 (thzICz) 作为环甲基配体，2,2,6,6-四甲基-3,5-庚二酮 (tmd) 作为辅助配体。当这些配合物掺杂到宿主材料 3,3′-二（9H-咔唑-9-基）-1,1′-联苯中时，掺杂的薄膜在 537 和 531 nm 处呈现黄色光致发光（PL）峰值，半最大值全宽（FWHM）带分别为 35 和 60 nm，PL 量子产率分别为 89.9% 和 85.9%。基于这两种发光体的有机发光二极管显示出适中的性能特征，最大外部量子效率分别为 25.2% 和 22.7%。值得注意的是，基于 (PhthzICz)2Ir(tmd) 的器件显示出 31 nm 的窄 FWHM。总之，该研究强调了在 Ir(III)配合物的环甲基化配体中加入刚性基团的实用性，这是实现高效 Ir(III)配合物的一种可行策略，可用于具有窄发射和高效率的有机发光二极管。

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引用次数: 0

σ–Arsolido complexes σ-Arsolido 复合物

IF 4 3区化学 Q1 Chemistry

Dalton Transactions

Pub Date : 2024-06-24 DOI: 10.1039/d4dt01308e

Anthony Hill, Ryan M. Kirk

The σ-stannyl complexes [M(SnnBu3)(CO)_n(η⁵-C₅H₅)] (n = 3, M = Mo, W; n = 2, M = Fe) serve as mild reagents for the installation of σ-arsolyl ligands in transmetallation reactions with As-chloroarsoles ClAsC₄R₄ (R = Me, Ph) to afford [M(σ-AsC4R4)(CO)n(η⁵-C₅H₅)]. The reaction of [Cr(SnⁿBu₃)(CO)₃(η⁵-C₅H₅)] with ClAsC₄Ph₄ most likely proceeds in a similar manner but is immediately followed by rapid formation of (AsC₄Ph₄)₂ and [Cr₂(CO)₆(η⁵-C₅H₅)₂]. The reacton of [Mo(SnⁿBu₃)(CO)₃(η⁵-C₅H₅)] with ClAsC_₄(SiMe₃)-2,5-Me_₂-3,4 is accompanied by monodesilylation to afford [Mo{σ-AsC₄(SiMe₃)-2-Me₂-3,4}(CO)₃(η⁵-C₅H₅)]. The slow reacton of [Fe(SnⁿBu₃)(CO)₂(η⁵-C₅H₅)] with ClAsC₄Me_₄ produced only traces of [Fe(σ-AsC₄Me₄)(CO)₂(η⁵-C₅H₅)] due to competition with the Diels-Alder type dimerisation of the haloarsole. Although attempts to decarbonylate the σ-arsolyl complexes were unsuccessful, computational analysis suggests that the trigonal ‘XL’ arsolenium coordination mode is viable.

σ-烷基配合物[M(SnnBu3)(CO)n(η5-C5H5)]（n = 3，M = Mo、W；n = 2，M = Fe）可作为温和的试剂，用于在与砷氯胂 ClAsC4R4（R = Me、Ph）的反金属化反应中安装σ-烯丙基配体，从而得到[M(σ-AsC4R4)(CO)n(η5-C5H5)]。Cr(SnnBu3)(CO)3(η5-C5H5)]与 ClAsC4Ph4 的反应很可能以类似的方式进行，但紧接着会迅速生成 (AsC4Ph4)2 和 [Cr2(CO)6(η5-C5H5)2]。Mo(SnnBu3)(CO)3(η5-C5H5)]与 ClAsC4(SiMe3)-2,5-Me2-3,4 发生单去硅反应，生成 [Mo{σ-AsC4(SiMe3)-2-Me2-3,4}(CO)3(η5-C5H5)]。[Fe(SnnBu3)(CO)2(η5-C5H5)]与 ClAsC4Me4 的缓慢反应只产生了微量的[Fe(σ-AsC4Me4)(CO)2(η5-C5H5)]，这是由于与卤代醛酸的 Diels-Alder 型二聚反应竞争所致。虽然对 σ-胂络合物进行脱羰基处理的尝试没有成功，但计算分析表明，三方 "XL "胂配位模式是可行的。

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