Poh Hwee Ling, Sofer Zdeněk, Šimek Petr, Tomandl Ivo, Pumera Martin
Division of Chemistry and Biological Chemistry, School of Physical and Mathematical Sciences, Nanyang Technological University, Singapore 637371 (Singapore).
Department of Inorganic Chemistry, University of Chemistry and Technology Prague, Technická 5, 166 28 Prague 6 (Czech Republic).
Chemistry. 2015 May 26;21(22):8130-6. doi: 10.1002/chem.201406168. Epub 2015 Apr 15.
Covalently functionalized graphene materials with well-defined stoichiometric composition are of a very high importance in the research of 2D carbon material family due to their well-defined properties. Unfortunately, most of the contemporary graphene-functionalized materials do not have this kind of defined composition and, usually, the amount of heteroatoms bonded to graphene framework is in the range of 1-10 at. %. Herein, we show that by a well-established hydroboration reaction chain, which introduces -BH2 groups into the graphene oxide structure, followed by H2O2 or CF3COOH treatment as source of -OH or -H, we can obtain highly hydroxylated compounds of precisely defined composition with a general formula (C1O0.78H0.75)n, which we named graphol and highly hydroxylated graphane (C1(OH)0.51H0.14)n, respectively. These highly functionalized materials with an accurately defined composition are highly important for the field of graphene derivatives. The enhanced electrochemical performance towards important biomarkers as well as hydrogen evolution reaction is demonstrated.
具有明确化学计量组成的共价功能化石墨烯材料，因其明确的性质，在二维碳材料家族的研究中具有非常重要的意义。不幸的是，大多数当代石墨烯功能化材料并不具有这种明确的组成，通常，与石墨烯骨架键合的杂原子数量在1 - 10原子百分比的范围内。在此，我们表明，通过一个成熟的硼氢化反应链，将 -BH₂ 基团引入氧化石墨烯结构，随后用H₂O₂ 或CF₃COOH作为 -OH或 -H的来源进行处理，我们可以获得具有精确确定组成的高羟基化化合物，其通式分别为 (C₁O₀.₇₈H₀.₇₅)ₙ 和 (C₁(OH)₀.₅₁H₀.₁₄)ₙ，我们分别将其命名为石墨醇和高羟基化石墨烷。这些具有精确确定组成的高度功能化材料，对于石墨烯衍生物领域非常重要。展示了其对重要生物标志物以及析氢反应增强的电化学性能。
