New progress made in the research of metal organic nano-tubular materials of Fujian Institute of Materials

Nano-tubular one-dimensional materials are the focus of attention in the field of modern chemistry and physics. How to efficiently and controllably prepare new materials with nano-tubular structures is a subject that chemists have been continuously exploring for a long time. The study of supramolecular coordination self-assembly chemistry provides a powerful means for synthesizing and preparing novel molecular-based functional materials through the "bottom-up" approach. However, the use of solution coordination self-assembly methods to prepare nanotubular one-dimensional Material has always been a big challenge.

Under the support of the “Youth Thousand Talents Program” of the Central Organization Department and the National Natural Science Foundation of China, the National Key Laboratory of Structural Chemistry of the Institute of Physical Structure Research of the Chinese Academy of Sciences, Sun Qingfu’s group of researchers in mesoporous materials “bottom up” supramolecular In the field of coordination self-assembly research, a breakthrough has been made. For the first time, a new idea of ​​preparing metal-organic supramolecular nanotubes with mesoporous pore diameters has been proposed through a "bottom-up" solution-graded self-assembly method. It was found that the "molecular clamp" module 1 containing a bimetallic center and the pyridine pyrazole bridged ligand 2 can first be deprotonated and self-assembled in-situ to form a binuclear orthogonal secondary structural unit (SBU) having a metal-metal bond. 3; due to the presence of uncoordinated pyridine groups, 3 can also undergo secondary self-assembly with PdII ions to form discrete nanotube units 4 of the formula Pd30L124L224.

It is understood that this 78-component discrete tubular supramolecules are the most abundant supramolecular assemblies reported in the literature. More interestingly, three levels of self-assembly occur during crystallization: discrete nanotube units are cross-linked by spontaneous removal of capped ligands and further converted to one-dimensional infinite nanotubes 5, which is a discrete type. It is also the first time that the special phenomenon that the tube unit transforms into infinite nanotubes by spontaneous cross-linking self-assembly has also been discovered. In addition, the results of the catalytic experiments show that with the participation of as low as 0.45% molar equivalents, these nano-tubular materials have excellent catalytic performance for the Suzuki–Miyaura carbon-carbon coupling reaction and enable the efficient use of noble metal Pd catalysts. In the future, a new approach will be provided for the controlled preparation of novel metal-organic nano-tubular materials and their applications. The above research work was published in the German Journal of Applied Chemistry (DOI: 10.1002/anie.201503295).

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