超薄二维Cu-BDC纳米片及其衍生的集成MOF纳米复合材料的制备,Advanced Functional Materials

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超薄二维Cu-BDC纳米片及其衍生的集成MOF纳米复合材料的制备
Advanced Functional Materials ( IF 18.5 ) Pub Date : 2019-01-08 , DOI: 10.1002/adfm.201806720
Guowu Zhan ₁ , Longlong Fan ₁ , Feigang Zhao ₁ , Zhongliang Huang ₁ , Bin Chen ₁ , Xin Yang ₁ , Shu-feng Zhou ₁

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具有许多空前特性的独立式2D纳米片已经在众多应用中使用。在这项工作中，通过使用Cu ₂ O纳米立方体（≈60nm）作为受限金属离子源，并通过一种简便而良性的方法成功地制造了二维含铜金属有机框架（MOF；即Cu-BDC）纳米片。1,4-苯二甲酸（H ₂ BDC）作为有机连接基。Cu ₂ O纳米立方体逐渐释放出Cu ⁺离子被溶解的氧气进一步氧化，并充当2D框架构建的养分。相比之下，使用铜盐进行的常规溶剂热合成仅产生体积为2–10 µm的块状Cu-BDC。有趣的是，所制备的Cu-BDC纳米片具有超薄的厚度，定向生长和出色的结晶度，可通过加载各种金属纳米晶体（例如Au，Ag， Pt和Ru，以3-巯基丙酸为分子键。此外，发现在表面上具有高度可及的活性位点的Cu-BDC / M复合材料在苯甲醛和伯胺之间的几次缩合反应中表现出高催化活性。

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Fabrication of Ultrathin 2D Cu‐BDC Nanosheets and the Derived Integrated MOF Nanocomposites

Freestanding 2D nanosheets with many unprecedented properties have been used in a myriad of applications. In this work, 2D copper‐bearing metal‐organic frameworks (MOFs; viz., Cu‐BDC) nanosheets are successfully fabricated via a facile and benign methodology through using Cu₂O nanocubes (≈60 nm) as a confined metal ion source and 1,4‐benzenedicarboxylic acid (H₂BDC) as an organic linker. The Cu₂O nanocubes gradually release Cu⁺ ions which are further oxidized by the dissolved oxygen and serve as nutrients for construction of 2D frameworks. In contrast, the conventional solvothermal synthesis with copper salt exclusively yields bulk Cu‐BDC with edge dimensions of 2–10 µm. Interestingly, the as‐prepared Cu‐BDC nanosheets show ultrathin thickness, oriented growth, and excellent crystallinity, which can be exploited as a platform for the design of a series of 2D‐integrated nanocatalysts by loading various metal nanocrystals such as Au, Ag, Pt, and Ru, with 3‐mercaptopropionic acid as molecular link. In addition, it is found that Cu‐BDC/M composites with highly accessible active sites on the surface exhibit high catalytic activity in several condensation reactions between benzaldehyde and primary amines. The findings offer an alternative strategy for rational design and synthesis of 2D MOF nanosheets and the derived 2D nanocomposites for catalytic applications.

更新日期：2019-01-08

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