硼掺杂富勒烯储氢-从物理吸附到化学吸附的转变

Physisorption to chemisorption of hydrogen molecules on boron-doped fullerenes

本文采用密度泛函理论(DFT)中的局域密度近似(LDA)方法对硼(B)掺杂富勒烯(C_(35)B)储氢问题在前人的基础上做了进一步研究,结果表明被C_(35)B吸附的氢分子很容易解离,经历从物理吸附到化学吸附的转变,并且发现解离产物C_(34)BHCH有分子内氢转移反应发生,这时B原子仍能与氢分子有很强的相互作用,最终导致B位置以及与B最邻近的三个C原子上都有氢原子吸附.并利用过渡态理论从热力学上分析了这种反应的发生趋势.

A further study on hydrogen storage by boron-doped fullerenes （C35B） was carried out by means of the local density approximation （LDA） on the basis of predecessors＇ work. The results indicated that the hydrogen molecules adsorbed on boron-doped fullerenes can be dissociated without additional catalysts and transformed from physisorption to chemisorption. Additionally, our calculations showed that there was an intermolecular hydrogen transfer reaction in the dissociation product C34 BHCH which lead to a strong interaction between B atom and hydrogen molecule, resulting in the absorption of hydrogen atom to the B atom as well as three C atoms in the vicinity of the B site. The reaction rate constants were predicted by transition state theory.