Zhu Z H, Lu G Q, Hatori H
ARC Centre for Functional Nanomaterials, University of Queensland, Brisbane 4072, Australia.
J Phys Chem B. 2006 Jan 26;110(3):1249-55. doi: 10.1021/jp0516590.
Boron substitution in carbon materials has been comprehensively investigated using the density functional theory method. It was found that there is a correlation between the stability of the graphene sheet, the distribution of pi electrons, the electrostatic potential, and the capability for hydrogen-atom adsorption. Boron substitution destabilizes the graphene structure, increases the density of the electron wave around the substitutional boron atoms, and lowers the electrostatic potential, thus improving the hydrogen adsorption energy on carbon. However, this improvement is only ca. 10-20% instead of a factor of 4 or 5. Our calculations also show that two substitutional boron atoms provide consistent and reliable results, but one substitutional boron results in contradictory conclusions. This is a warning to other computational chemists who work on boron substitution that the conclusion from one substitutional boron might not be reliable.
利用密度泛函理论方法对碳材料中的硼取代进行了全面研究。研究发现，石墨烯片的稳定性、π电子分布、静电势以及氢原子吸附能力之间存在关联。硼取代会使石墨烯结构不稳定，增加取代硼原子周围的电子波密度，并降低静电势，从而提高碳对氢的吸附能。然而，这种提高仅约为10 - 20%，而非4倍或5倍。我们的计算还表明，两个取代硼原子能提供一致且可靠的结果，但一个取代硼原子会导致相互矛盾的结论。这对其他从事硼取代研究的计算化学家是一个警示，即一个取代硼原子得出的结论可能不可靠。
