高容量质子电池中氢化非晶硅薄膜电化学储氢行为的第一性原理分析,International Journal of Hydrogen Energy

当前位置： X-MOL 学术 › Int. J. Hydrogen Energy › 论文详情

Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)

高容量质子电池中氢化非晶硅薄膜电化学储氢行为的第一性原理分析
International Journal of Hydrogen Energy ( IF 8.1 ) Pub Date : 2023-03-21 , DOI: 10.1016/j.ijhydene.2023.03.034
Haimin Zhang , Yongchun Luo , Yujie Xiang , Fuling Tang , Qiankun Zhang , Boyang Lin , Chen Wu , Xinhui Liu , Boshi Su

硅材料电极作为高容量质子电池的质子载体仅在很短的时间内被提出，以至于它们在充电和放电过程中的物理化学性质和电化学储氢行为几乎仍然是未知领域。在此，氢化非晶硅 (a-Si:H)薄膜电极是通过射频溅射然后异位氢化制备的。电化学性质对a-Si:H电极的电化学储氢行为进行了实验测试，并通过第一性原理计算分析了a-Si:H电极的电化学储氢行为。结果表明，氢化过程显着提高了电极的电化学容量，降低了电极结构的带隙。电极在初始充电过程中表现出较弱的导电性，但在后期充电过程中电极电子结构的不稳定导致电化学充电过程略有波动。a-Si:H电极具有更好的电化学储氢/释放可逆性比非氢化电极，但这种可逆性被电极表面覆盖的氧原子削弱。对于a-Si:H电极，电化学储氢过程比析氢反应的电化学解吸过程更容易完成。a-Si:H薄膜电极在Ni(111)衬底表面更稳定，电极/衬底界面良好的导电性为电化学充放电过程中电子的自由传输提供了便利条件。我们相信这些结果完美地解释了负责a-Si:H电极在该类质子电池中的电极反应和电化学行为，对了解应用于其他类型电池的硅材料电极在充放电过程中的理化性质和电化学储氢行为具有一定的参考价值.

"点击查看英文标题和摘要"

First-principles analysis of electrochemical hydrogen storage behavior for hydrogenated amorphous silicon thin film in high-capacity proton battery

Silicon material electrodes as proton carriers for high-capacity proton battery have only been proposed for such a short period of time that their physicochemical properties and electrochemical hydrogen storage behavior during charge and discharge processes remain nearly uncharted territory. Herein, the hydrogenated amorphous silicon (a-Si:H) thin film electrodes are prepared by radio frequency sputtering followed by ex-situ hydrogenation. The electrochemical properties of a-Si:H electrodes are tested experimentally, and the electrochemical hydrogen storage behaviors of a-Si:H electrodes are analyzed by first-principles calculations. The results show that the hydrogenation process significantly increases the electrochemical capacity of the electrodes and reduces the band gap of the electrode structure. The electrode exhibits weak conductivity during the initial charging, but the instability of the electrode electronic structure during the later charging results in a slight fluctuation of the electrochemical charging process. The a-Si:H electrode have better electrochemical hydrogen storage/release reversibility than non-hydrogenated electrodes, but this reversibility is weakened by oxygen atoms covered on the electrode surface. The electrochemical hydrogen storage process is easier to accomplish than the electrochemical desorption process of hydrogen evolution reaction for the a-Si:H electrodes. The a-Si:H thin film electrode is more stable on the Ni(111) substrate surface and the good conductivity of the electrode/substrate interface provides convenient conditions for the free transport of electrons in the electrochemical charge/discharge processes. We believe that these results perfectly explain the microscopic mechanisms responsible for the electrode reaction and electrochemical behavior of a-Si:H electrodes in this type of proton battery, and have a certain reference value in understanding the physicochemical properties and electrochemical hydrogen storage behavior of silicon material electrodes applied to other types of batteries during charge/discharge processes.

更新日期：2023-03-21

点击分享查看原文

点击收藏

阅读更多本刊最新论文本刊介绍/投稿指南11