Department of Chemical Engineering, University of Michigan, Ann Arbor, Michigan 48109, USA.
Langmuir. 2010 Oct 5;26(19):15394-8. doi: 10.1021/la100172b.
Recent studies have shown that using the hydrogen spillover phenomena is a promising approach for developing new materials for hydrogen storage at ambient temperature. However, the rates need to be improved. Significant catalytic effects on both spillover (i.e., adsorption) and reverse spillover (i.e., desorption) on Pt-doped carbon by TiF(3) were found. By doping 2 wt % TiF(3) on the Pt-doped Maxsorb (a superactivated carbon), both adsorption and desorption rates were significantly increased while the storage capacity decreased only slightly due to decreased surface areas. The effect of the heat treatment temperature (473 K vs 673 K) of the doped TiF(3) on its catalytic effects was also studied. XPS analyses showed that C-F bonds were formed upon heat treatment and that the amount of C-F bonds increased with the heat treatment temperature. The catalytic effects also increased with the heat treatment temperature, indicating that the catalytic mechanism possibly involved the formation of C-F bonds on the carbon edge sites. In addition, the issue of proper sample preparation of Pt/carbon was briefly addressed; missteps in metal doping and consequently poor metal dispersion will result in significantly diminished spillover enhancements (Stadie et al.).
最近的研究表明,利用氢溢出现象是开发常温下储氢新材料的一种很有前途的方法。然而,其转化速度仍需进一步提高。在 Pt 掺杂 Maxsorb(一种超级活性炭)中掺杂 2wt%TiF3 时,发现对 Pt 掺杂 Maxsorb 的溢出(即吸附)和反向溢出(即解吸)具有显著的催化效应。通过掺杂 2wt%TiF3,吸附和解吸速率都得到了显著提高,而由于表面积的减小,储氢容量仅略有下降。还研究了掺杂 TiF3 的热处理温度(473K 与 673K)对其催化效应的影响。XPS 分析表明,热处理时形成了 C-F 键,并且 C-F 键的数量随热处理温度的升高而增加。催化效应也随热处理温度的升高而增加,表明催化机制可能涉及在碳边缘位点形成 C-F 键。此外,简要讨论了 Pt/碳的适当样品制备问题;金属掺杂过程中的失误以及由此导致的金属分散不良将导致溢出增强显著减弱(Stadie 等人)。