Air Products and Chemicals, Inc., 7201 Hamilton Boulevard, Allentown, Pennsylvania 18195, USA.
J Am Chem Soc. 2009 Dec 16;131(49):17732-3. doi: 10.1021/ja907232y.
We present a combined theoretical and experimental study on H(2) physisorption in partially fluorinated graphite. This material, first predicted computationally using ab initio molecular dynamics simulation and subsequently synthesized and characterized experimentally, represents a novel class of "acceptor type" graphite intercalated compounds that exhibit significantly higher isosteric heat of adsorption for H(2) at near ambient temperatures than previously demonstrated for commonly available porous carbon-based materials. The unusually strong interaction arises from the semi-ionic nature of the C-F bonds. Although a high H(2) storage capacity (>4 wt %) at room temperature is predicted not to be feasible due to the low heat of adsorption, enhanced storage properties can be envisaged by doping the graphitic host with appropriate species to promote higher levels of charge transfer from graphene to F(-) anions.
我们提出了一个关于部分氟化石墨中 H(2)物理吸附的理论和实验综合研究。这种材料最初是通过从头算分子动力学模拟预测的，随后通过实验合成和表征，代表了一类新型的“受体型”石墨插层化合物，它们在接近环境温度下对 H(2)的等容热吸附比以前证明的常用多孔碳基材料高得多。这种不寻常的强相互作用源于 C-F 键的半离子性质。尽管由于吸附热低，预测在室温下不可能实现高的 H(2)存储容量（>4wt%），但通过用适当的物质掺杂石墨主体来促进从石墨烯到 F(-)阴离子的更高水平的电荷转移，可以设想增强存储性能。
