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[材料资讯] 邓鹤翔:基于MOF分子钳的快速尿检纳米试纸

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发表于 2018-7-6 08:12:06 | 显示全部楼层 |阅读模式
国际权威期刊Angewandte Chemie International Edition (《德国应用化学》) 在线发表化学与分子科学学院邓鹤翔教授团队在MOF(Metal-organic framework,金属有机框架材料)结构中创造分子钳的研究新成果。基于该分子钳的纳米试纸可用于快速尿检。
在传统的配位化学中,金属配合物的空间几何构型往往会随着有机配体的改变而发生配位键长和键角的变化。研究团队人员根据MOF材料晶态及多孔性的特性,将萤石拓扑结构材料中四连接的有机配体用一个三连接和一个单连接的有机配体替换。由于MOF净体重中金属构筑单元位置的固定,三连接的有机配体和单连接的配体实现一一对应,如钳子一样,能够对进入其空穴的金属进行精确配位。三连接的配体用来配位引入到MOF中的活性金属,类似钳子的固定部分;而单连接的配体长度和官能团可以很方便的改变,从而通过位阻效应和弱的分子作用力来影响引入的活性金属的配位能力,就像钳的的活动部分一样。以此,首次实现了在不改变金属配位空间几何的情况下,对配位键长的精确调节。基于此方法,研究人员通过尝试不同的合成条件,改变三连接和四连接配体不同的比例以及选用不同的单连接的配体,合成出了一系列带有不同配位环境的分子钳MOF材料。这些分子钳能够和多种金属离子发生配位,包括Mg2+、Al3+、Cr3+、Mn2+、Fe3+、Co2+、Ni2+、Cu2+、Zn2+、Ag+、Cd2+和Pb2+等,并且能在较大范围内调节配位常数(Kobs从1.56×102到1.70×104 Lmol-1)。
这类含有分子钳的MOF可以用来精确的检测半胱氨酸、高半胱氨酸和谷胱甘肽这类和人体健康息息相关的巯基氨基酸,检出限低达22.4纳摩尔。值得注意的是,这类高度定制的分子钳具有较好的识别性能,其高效的检测不受水或体液(如尿液)的干扰。通过对此类MOF材料纳米化,团队成功开了成本较低的用于尿液检测的试纸并申请了相专利。这些试纸便于携带和保存,能够瞬间判定巯基氨基酸是否超标,且能够通过酒精淋洗后多次重复使用,非常适合于用于边远及穷困地区的健康检测。
该论文的题目为Molecular Vise Approach to Create Metal-Binding Sites in MOFs and Detection of Biomarkers,doi.org/10.1002/anie.201803201。通讯作者邓鹤翔为武汉大学化学院教授,博士生汪洋和博士后刘琦为该论文的共同第一作者,其他作者包括2014级本科生张勤和2013级本科生彭博思。该研究得到中组部计划、基金委重大研究计划重点项目、培育项目、基金委面上项目、湖北省重点项目和武汉大学创新团队以及武汉大学重点博后项目的支持。

基于MOF分子钳的快速尿检纳米试纸

基于MOF分子钳的快速尿检纳米试纸

Molecular Vise Approach to Coordinate Metals
(Research breakthrough reported by Deng’s groups)
Scientists in Wuhan University found a new way to bind metals in a controllable manner using metal-organic frameworks, reported on the recent issue of Angew. Chem. Int. Ed., and these nano-materials are good for the fast detection of biomarkers in urine without the use of sophisticated instruments.
Molecular constructs are highly desirable in various applications such as nanomachines, nanorobots, drug delivery, catalysis and biomolecule detection. However, molecular constructs were usually synthesized in solution phase rather than solid-state phase. In this report, a research group led by Hexiang Deng at Wuhan university show that a “molecular vise” can be created inside metal-organic frameworks to provide customized binding site for metal ions, and forming the so called “MV-MOFs”. This was achieve by replacing a tetra-topic organic linker with a pair of mono-topic and tri-topic linker, where the length of the mono-topic linker can be precisely adjusted, thus provide a controlled coordination environment for metals with the amine on the tri-topic linker. The mono-topic linker resembles the moving part of the vise, while the tri-topic linker fixed by three secondary building units (SBUs) in MOFs resembles the stationary part.
This “molecular vise” was taking the advantage of ordered arrangement of SBUs in MOFs, thus the coordination environment can be adjusted without affecting the geometry of coordinating linkers. This unique feature cannot be found in any other systems. A large variety of organic linkers, functional groups and metals can be introduces to customize the metal binding site. These MV-MOFs can also been made in the form of nanocrystals, where the diffusion of chemicals was favored. One of these nano-MV-MOFs was successfully used in the detection of biomarkers such as cysteine with extremely high sensitivity, by simply using UV lamp to observe the fluorescent decay. These MOFs were also prepared into test papers that are easy to store and transfer for remote areas, wheresophisticated instruments are lack.
This work was conducted in College of Chmistry & Molecular Sciences of Wuhan University, led by Prof. Hexiang Deng. Yang Wang and Qi Liu are the co-first authors of this publications. Qin Zhang and Bosi Peng also made significant contributions. This research was supported by the 1000 Talent Plan of China, National Natural Science Foundation of China (21471118, 91545205, 91622103), National Science Foundation of Jiangsu Province of China (ZXG201446, BK20140410), National Key Basic Research Program of China (2014CB239203), Key Program of Hubei Provence (2015CFA126) and Innovation Team of Wuhan University (2042017kf0232).

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