Seenithurai Sonai, Chai Jeng-Da
Department of Physics, National Taiwan University, Taipei, 10617, Taiwan.
Center for Theoretical Physics, National Taiwan University, Taipei, 10617, Taiwan.
Sci Rep. 2018 Sep 10;8(1):13538. doi: 10.1038/s41598-018-31947-9.
It has been extremely difficult for conventional computational approaches to reliably predict the properties of multi-reference systems (i.e., systems possessing radical character) at the nanoscale. To resolve this, we employ thermally-assisted-occupation density functional theory (TAO-DFT) to predict the electronic and hydrogen storage properties of Li-terminated linear boron chains (LiB), with n boron atoms (n = 6, 8, …, and 16). From our TAO-DFT results, LiB, which possess radical character, can bind up to 4 H molecules per Li, with the binding energies in the desirable regime (between 20 and 40 kJ/mol per H). The hydrogen gravimetric storage capacities of LiB range from 7.9 to 17.0 wt%, achieving the ultimate goal of the United States Department of Energy. Accordingly, LiB could be promising media for storing and releasing H at temperatures much higher than the boiling point of liquid nitrogen.
对于传统的计算方法而言，要在纳米尺度上可靠地预测多参考系统（即具有自由基特性的系统）的性质极其困难。为了解决这个问题，我们采用热辅助占据密度泛函理论（TAO-DFT）来预测具有n个硼原子（n = 6、8、…和16）的锂端接线性硼链（LiB）的电子和储氢性质。根据我们的TAO-DFT结果，具有自由基特性的LiB每个锂原子最多可结合4个H分子，结合能处于理想范围（每个H为20至40 kJ/mol）。LiB的氢重量储存容量在7.9至17.0 wt%之间，达到了美国能源部的最终目标。因此，LiB有望成为在远高于液氮沸点的温度下储存和释放H的介质。
