Chua Chun Kiang, Ambrosi Adriano, Sofer Zdeněk, Macková Anna, Havránek Vladimír, Tomandl Ivo, Pumera Martin
Division of Chemistry & Biological Chemistry, School of Physical and Mathematical Sciences, Nanyang Technological University, 21, Nanyang Link, Singapore 637371.
Chemistry. 2014 Nov 24;20(48):15760-7. doi: 10.1002/chem.201404205. Epub 2014 Oct 5.
Chemical synthesis of graphene relies on the usage of various chemical reagents. The initial synthesis step, in which graphite is oxidized to graphite oxide, is achieved by a combination of chemical oxidants and acids. A subsequent chemical reduction step eliminates/reduces most oxygen functionalities to yield graphene. We demonstrate here that these chemical treatments significantly contaminate graphene with heteroatoms/metals, depending on the procedures followed. Contaminations with heteroatoms (N, B, Cl, S) or metals (Mn, Al) were present at relatively high concentrations (up to 3 at%), with their chemical states dependent on the procedures. Such unintentional contaminations (unwanted doping) during chemical synthesis are rarely anticipated and reported, although the heteroatoms/metals may alter the electronic and catalytic properties of graphene. In fact, the levels of unintentionally introduced contaminants on graphene are often higher than typical levels found on intentionally doped graphene. Our findings are important for scientists applying chemical methods to prepare graphene.
石墨烯的化学合成依赖于各种化学试剂的使用。最初的合成步骤是将石墨氧化为氧化石墨,这是通过化学氧化剂和酸的组合来实现的。随后的化学还原步骤消除/减少了大部分含氧官能团,从而得到石墨烯。我们在此证明,根据所采用的程序,这些化学处理会使石墨烯被杂原子/金属严重污染。杂原子(N、B、Cl、S)或金属(Mn、Al)的污染以相对较高的浓度存在(高达3原子%),其化学状态取决于程序。尽管杂原子/金属可能会改变石墨烯的电子和催化性能,但在化学合成过程中这种无意的污染(不必要的掺杂)很少被预料到和报道。事实上,石墨烯上无意引入的污染物水平通常高于有意掺杂的石墨烯上的典型水平。我们的发现对应用化学方法制备石墨烯的科学家来说很重要。