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首页> 外文期刊>Dalton transactions: An international journal of inorganic chemistry >Alkaline earth imidazolate coordination polymers by solvent free melt synthesis as potential host lattices for rare earth photoluminescence: ~X _∞[AE(Im) _2(ImH) _(2-3)], Mg, Ca, Sr, Ba, x = 1-2
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Alkaline earth imidazolate coordination polymers by solvent free melt synthesis as potential host lattices for rare earth photoluminescence: ~X _∞[AE(Im) _2(ImH) _(2-3)], Mg, Ca, Sr, Ba, x = 1-2

机译：碱土金属咪唑基配位聚合物通过无溶剂熔融合成作为稀土光致发光的潜在主体晶格：〜X_∞[AE（Im）_2（ImH）_（2-3）]，Mg，Ca，Sr，Ba，x = 1-2

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摘要

The series of alkaline earth elements magnesium, calcium, strontium and barium yields single crystalline imidazolate coordination polymers by reactions of the metals with a melt of 1H-imidazole: 1~∞[Mg(Im) _2(ImH) _3] (1), 2~∞[AE(Im) _2(ImH) _2], AE = Ca (2), Sr (3), and 1~∞[Ba(Im) _2(ImH) _2] (4). No additional solvents were used for the reactions. Co-doping experiments by addition of the rare earth elements cerium, europium and terbium were carried out. They indicate 2~∞[Sr(Im) _2(ImH) _2] as a possible host lattice for cerium(iii) photoluminescence showing a blue emission and thus a novel blue emitting hybrid material phosphor 3:Ce ~(3+). Co-doping with europium and terbium is also possible but resulted in formation of 3~∞[Sr(Im) _2]:Ln, Ln = Eu and Tb (5), with both exhibiting green emission of either Eu ~(2+) or Tb ~(3+). The other alkaline earth elements do not show acceptance of the rare earth ions investigated and a different structural chemistry. For magnesium and barium one-dimensional strand structures are observed whereas calcium and strontium give two-dimensional network structures. Combined with an increase of the ionic radii of AE ~(2+) the coordinative demand is also increasing from Mg ~(2+) to Ba ~(2+), reflected by four different crystal structures for the four elements Mg, Ca, Sr, Ba in 1-4. Different linkages of the imidazolate ligands result in a change from complete σ-N coordination in 1 to additional η ~5-π coordination in 4. The success of co-doping with different lanthanide ions is based on a match in the chemical behaviour and cationic radii. The use of strontium for host lattices with imidazole is a rare example in coordination chemistry of co-doping with small amounts of luminescence centers and successfully reduces the amount of high price rare earth elements in hybrid materials while maintaining the properties. All compounds are examples of pure N-coordinated coordination polymers of the alkaline earth metals and were identified by single crystal X-ray analysis and powder diffraction. The degree of co-doping was determined by SEM/EDX. Mid IR, Far IR and Raman spectroscopy and micro analyses as well as simultaneous DTA/TG were also carried out to characterize the products in addition to the photoluminescence studies of the co-doped samples.
机译：一系列碱土元素镁，钙，锶和钡通过金属与1H-咪唑熔体的反应生成单晶咪唑酸酯配位聚合物：1〜∞[Mg（Im）_2（ImH）_3]（1）， 2〜∞[AE（Im）_2（ImH）_2]，AE = Ca（2），Sr（3）和1〜∞[Ba（Im）_2（ImH）_2]（4）。反应中不使用其他溶剂。通过添加稀土元素铈，euro和ter进行共掺杂实验。他们指出2〜∞[Sr（Im）_2（ImH）_2]是铈（iii）光致发光的可能的主晶格，显示出蓝色发光，因此是新型的蓝色发光杂化材料磷光体3：Ce〜（3+）。也可以与euro和ter共掺杂，但会导致形成3〜∞[Sr（Im）_2]：Ln，Ln = Eu和Tb（5），并且都显示Eu〜（2+）的绿色发射。或Tb〜（3+）。其他碱土金属元素未显示出对所研究的稀土离子和不同的化学结构的接受。对于镁和钡，观察到一维链结构，而钙和锶给出二维网络结构。结合AE〜（2+）离子半径的增加，配位需求也从Mg〜（2+）增至Ba〜（2+），反映出四种元素Mg，Ca， Sr，Ba在1-4中。咪唑化物配体的不同键合导致从1中的完整σ-N配位变为4中的附加η〜5-π配位。用不同镧系元素离子共掺杂的成功是基于化学行为和阳离子的匹配半径在咪唑与少量发光中心共掺杂的配位化学中，将锶与咪唑一起用于主晶格是一个罕见的例子，它可以在保持性能的同时，成功地减少混合材料中高价稀土元素的含量。所有化合物均为碱土金属的纯N配位聚合物的实例，并通过单晶X射线分析和粉末衍射鉴定。共掺杂程度通过SEM / EDX确定。除了对共掺杂样品进行光致发光研究以外，还进行了中红外，远红外和拉曼光谱分析，显微分析以及同时的DTA / TG表征产品。

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