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A mineralogically-inspired silver–bismuth hybrid material: an efficient heterogeneous catalyst for the direct synthesis of nitriles from terminal alkynes
Green Chemistry ( IF 9.8 ) Pub Date : 2018-01-08 00:00:00 , DOI: 10.1039/c7gc02487h
Sándor B. Ötvös 1, 2, 3, 4, 5 , Rebeka Mészáros 1, 2, 3, 4 , Gábor Varga 2, 3, 4, 6, 7 , Marianna Kocsis 1, 2, 3, 4, 6 , Zoltán Kónya 3, 4, 8, 9, 10 , Ákos Kukovecz 2, 3, 4, 10 , Péter Pusztai 2, 3, 4, 10 , Pál Sipos 2, 3, 4, 7, 11 , István Pálinkó 2, 3, 4, 6, 7 , Ferenc Fülöp 1, 2, 3, 4, 5
Affiliation  

The synthesis and characterization of a silver-containing hybrid material is reported as a novel heterogeneous noble metal catalyst. In order to eliminate the need for traditional immobilization techniques, and to create a solid material with structurally-bound silver catalytic centers, the layered structure of a naturally occurring mineral served as the basis of the initial catalyst design. The novel material was prepared by means of the urea-mediated homogeneous precipitation of the corresponding metal nitrates, and was fully characterized by means of diverse instrumental techniques (X-ray diffractometry, Raman, IR, UV-Vis, EPR, X-ray photoelectron spectroscopies, thermal methods as well as atomic force, scanning and transmission electron microscopies). The as-prepared material exhibited outstanding activity in silver-catalyzed C[triple bond, length as m-dash]C bond activation to yield organic nitriles directly from terminal alkynes with less environmental concerns as compared to the classical synthesis methods. The effects of the reaction time, the temperature, as well as the role of various solvents, nitrogen sources and additives were carefully scrutinized in order to achieve high-yielding and selective nitrile formation. The heterogeneous nature of the reaction was verified and the solid catalyst was recycled and reused numerous times without loss of its activity or degradation of its structure, thereby offering a sustainable synthetic methodology.

中文翻译:

矿物学启发的银-铋杂化材料:从末端炔烃直接合成腈的有效多相催化剂

据报道,含银杂化材料的合成和表征是一种新型的非均相贵金属催化剂。为了消除对传统固定化技术的需求,并创建具有结构绑定的银催化中心的固体材料,天然矿物的层状结构用作初始催化剂设计的基础。通过脲介导的相应金属硝酸盐的均相沉淀制备了这种新型材料,并通过多种仪器技术(X射线衍射仪,拉曼光谱,IR,UV-Vis,EPR,X射线光电子)对其进行了全面表征。光谱,热方法以及原子力,扫描和透射电子显微镜)。所制备的材料在银催化的C中表现出优异的活性。[三重键,长度为m-破折号]与传统的合成方法相比,C键活化可直接从末端炔烃生产有机腈,而对环境的关注较小。仔细研究了反应时间,温度以及各种溶剂,氮源和添加剂的作用,以实现高产率和选择性腈的形成。验证了反应的非均质性质,并且将固体催化剂再循环并重复使用了许多次,而不会损失其活性或降低其结构,从而提供了一种可持续的合成方法。
更新日期:2018-03-06
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