Unraveling the Catalytic Mechanism of Rutile RuO2 for the Oxygen Reduction Reaction and Oxygen Evolution Reaction in Li–O2 Batteries
Unraveling the Catalytic Mechanism of Rutile RuO2 for the Oxygen Reduction Reaction and Oxygen Evolution Reaction in Li–O2 Batteries
复制标题
DOI：
10.1021/acscatal.6b01778
复制
发表时间：
2016-08
期刊：
影响因子：
12.9
通讯作者：
Le Shi;T. Zhao;Ao Xu;Zhaohuan Wei
中科院分区：
文献类型：
--
作者：
Le Shi;T. Zhao;Ao Xu;Zhaohuan Wei
由于固态放电产物Li 2 O2的参与，催化剂如何在非水锂氧电池中起作用尚未确定，尽管这个问题已经经历了激烈的争论。本文以一种高效且广泛应用的催化剂--金红石型RuO 2为代表，通过从头算研究了其在锂氧电池中的催化机理。对于氧还原反应（ORR），发现金红石型RuO 2可以向LiO 2和Li 2 O2提供大的吸附能，从而导致高的初始放电电压。此外，表面氧的归一化不饱和度被确定为ORR催化活性的描述符。对于析氧反应（OER），我们认为，除了三相界面外，析氧反应还可能发生在Li 2 O2/RuO 2的两相界面上，即金红石型RuO 2为锂离子提供通道，而氧则从Li 2 O2的暴露表面析出。计算结果表明，我们提出的…
Because of the involvement of solid-state discharge product Li2O2, how a catalyst works in nonaqueous lithium–oxygen batteries is yet to be determined, although the question has undergone fierce debate. In this work, we take an effective and widely used catalyst, rutile RuO2, as a representative and studied its catalytic mechanism in lithium–oxygen batteries via ab initio calculations. For the oxygen reduction reaction (ORR), it is found that rutile RuO2 can provide large adsorption energies toward LiO2 and Li2O2, thus resulting in high initial discharge voltages. Moreover, the normalized degree of unsaturation of surface oxygen is identified as a descriptor for the ORR catalytic activity. For the oxygen evolution reaction (OER), we propose that, in addition to the three-phase interface, the OER may also occur at the two-phase interface of Li2O2/RuO2, where rutile RuO2 provides pathways for the lithium ions while oxygen evolves from the exposed surfaces of Li2O2. Calculation results show that our proposed...