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Two-Dimensional Nanosheets from Redox-Active Superatoms
ACS Central Science ( IF 12.7 ) Pub Date : 2017-08-30 00:00:00 , DOI: 10.1021/acscentsci.7b00328
Anouck M Champsaur 1 , Jaeeun Yu 1 , Xavier Roy 1 , Daniel W Paley 1, 1 , Michael L Steigerwald 1 , Colin Nuckolls 1 , Christopher M Bejger 2
Affiliation  

We describe a new approach to synthesize two-dimensional (2D) nanosheets from the bottom-up. We functionalize redox-active superatoms with groups that can direct their assembly into multidimensional solids. We synthesized Co6Se8[PEt2(4-C6H4COOH)]6 and found that it forms a crystalline assembly. The solid-state structure is a three-dimensional (3D) network in which the carboxylic acids form intercluster hydrogen bonds. We modify the self-assembly by replacing the reversible hydrogen bonds that hold the superatoms together with zinc carboxylate bonds via the solvothermal reaction of Co6Se8[PEt2(4-C6H4COOH)]6 with Zn(NO3)2. We obtain two types of crystalline materials using this approach: one is a 3D solid and the other consists of stacked layers of 2D sheets. The dimensionality is controlled by subtle changes in reaction conditions. These 2D sheets can be chemically exfoliated, and the exfoliated, ultrathin 2D layers are soluble. After they are deposited on a substrate, they can be imaged. We cast them onto an electrode surface and show that they retain the redox activity of the superatom building blocks due to the porosity in the sheets.

中文翻译:


来自氧化还原活性超级原子的二维纳米片



我们描述了一种自下而上合成二维(2D)纳米片的新方法。我们用可以引导其组装成多维固体的基团对氧化还原活性超原子进行功能化。我们合成了Co 6 Se 8 [PEt 2 (4-C 6 H 4 COOH)] 6并发现它形成了晶体组装体。固态结构是三维(3D)网络,其中羧酸形成簇间氢键。我们通过 Co 6 Se 8 [PEt 2 (4-C 6 H 4 COOH)] 6与 Zn(NO 3 ) 的溶剂热反应,用羧酸锌键取代将超原子结合在一起的可逆氢键,从而修改自组装过程2 .我们使用这种方法获得了两种类型的晶体材料:一种是 3D 固体,另一种由 2D 片材的堆叠层组成。维数是通过反应条件的细微变化来控制的。这些 2D 片材可以进行化学剥离,并且剥离后的超薄 2D 层是可溶的。将它们沉积在基底上后,就可以对其进行成像。我们将它们浇铸到电极表面上,并表明由于片材中的孔隙率,它们保留了超原子构建块的氧化还原活性。
更新日期:2017-08-30
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