First TPymT-Ln complexes (TPymT = 2,4,6-Tris(2-pyrimidyl)-1,3,5-triazine; Ln = Eu, Gd, Tb, Dy): Solvothermal synthesis, structure, magnetic and photoluminescent properties

IF 3.4 3区化学 Q2 CHEMISTRY, INORGANIC & NUCLEAR

Solid State Sciences Pub Date : 2024-10-16 DOI:10.1016/j.solidstatesciences.2024.107723

Burak Ay , Rina Takano , Takayuki Ishida

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Abstract

Four novel mononuclear lanthanide complexes, [Ln(TPymT)(NO₃)₃(H₂O)₂] (Ln: Eu³⁺ (1), Gd³⁺ (2), Tb³⁺ (3) and Dy³⁺ (4)), have been solvothermally synthesized using multidentate 2,4,6-tris(2-pyrimidyl)-1,3,5-triazine (TPymT). Compounds 1–3 have been characterized by means of elemental analysis, FT-IR, and single-crystal/powder X-ray diffraction analysis. Compound 4 was structurally characterized. The Ln³⁺ ion in 1–4 is ten-coordinated, where TPymT serves as an N₃ donor in an isostructural series. The alternating-current magnetic studies showed frequency dependence below ca. 10 K for 3, as an indication of a single-ion magnet. The activation energy for the magnetization reorientation was estimated as U_eff/k_B = 95(9) K after applying a dc bias field 2000 Oe for 3. The photoluminescent studies clarified that 1 and 3 behaved as red and green light emitters with quantum yields as high as 17 and 39 %, respectively. The TD-DFT calculation supports the energy level scheme of ground and excited states of TPymT together with the reference compound 4′-phenyl-2,2’:6′,2″-terpyridine. The present work suggests a broad chance and motivation to apply TPymT to the field of 4f coordination chemistry.

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首个 TPymT-Ln 复合物（TPymT = 2,4,6-三(2-嘧啶基)-1,3,5-三嗪；Ln = Eu、Gd、Tb、Dy）：溶热合成、结构、磁性和光致发光特性

四种新型单核镧系配合物[Ln(TPymT)(NO3)3(H2O)2]（Ln：利用多叉 2,4,6-三(2-嘧啶基)-1,3,5-三嗪（TPymT）溶热合成了四种新型单核镧系配合物 [Ln(TPymT)(NO3)3(H2O)2]（Ln：Eu3+ (1)、Gd3+ (2)、Tb3+ (3) 和 Dy3+ (4)）。化合物 1-3 已通过元素分析、傅立叶变换红外光谱和单晶/粉末 X 射线衍射分析进行了表征。对化合物 4 进行了结构表征。1-4 中的 Ln3+ 离子是十配位的，其中 TPymT 在等结构系列中充当 N3 给体。交变电流磁性研究显示，3 的频率依赖性低于约 10 K，这表明它是一种单离子磁体。对 3 施加直流偏置场 2000 Oe 后，磁化重新定向的活化能估计为 Ueff/kB = 95(9) K。光致发光研究表明，1 和 3 表现为红色和绿色发光体，量子产率分别高达 17% 和 39%。TD-DFT 计算支持 TPymT 与参考化合物 4′-苯基-2,2':6′,2″-三吡啶的基态和激发态能级方案。本研究为将 TPymT 应用于 4f 配位化学领域提供了广阔的机会和动力。

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来源期刊

Solid State Sciences 化学-无机化学与核化学

CiteScore

6.60

自引率

2.90%

发文量

214

审稿时长

27 days

期刊介绍： Solid State Sciences is the journal for researchers from the broad solid state chemistry and physics community. It publishes key articles on all aspects of solid state synthesis, structure-property relationships, theory and functionalities, in relation with experiments. Key topics for stand-alone papers and special issues: -Novel ways of synthesis, inorganic functional materials, including porous and glassy materials, hybrid organic-inorganic compounds and nanomaterials -Physical properties, emphasizing but not limited to the electrical, magnetical and optical features -Materials related to information technology and energy and environmental sciences. The journal publishes feature articles from experts in the field upon invitation. Solid State Sciences - your gateway to energy-related materials.