期刊
ACS APPLIED MATERIALS & INTERFACES
卷 14, 期 11, 页码 13410-13418出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsami.2c01400
关键词
density functional theory; lithium-oxygen batteries; 1T-ZrO2 monolayer; adsorption behavior; reaction mechanism; overpotential
资金
- China Postdoctoral Science Foundation [2020M670118]
- Open Project of State Key Laboratory of Superhard Materials, Jilin University [202011]
- National Natural Science Foundation of China [11504325]
- Natural Science Foundation of Zhejiang Province [LQ15A040004]
This study explores the potential applications of experimentally synthesized ZrO2 monolayer as the cathode catalyst for nonaqueous lithium-oxygen batteries. It shows that Zr atoms in the substrate play a critical role in stabilizing the LiO2 cluster, leading to a new peroxide-like adsorption geometry as the most stable configuration. The ab initio calculations indicate that both the ORR and OER catalytic activities are most likely to adopt the four-electron mechanism with low overpotentials. Additionally, the adsorption energy of Li2O2 is found to be a good descriptor for both ORR and OER catalytic activities.
Herein, we explore the potential applications of the experimentally synthesized ZrO2 monolayer as the cathode catalyst for nonaqueous lithium-oxygen batteries. First, we show that a new peroxide-like adsorption geometry is the most stable configuration for LiO2, which is distinct from the previously known O-Li-O triangular geometry. The proposed most stable adsorption configuration is because the Zr atoms in the substrate play a critical role in stabilizing the LiO2 cluster. Second, our ab initio calculations indicate that both the ORR and OER catalytic activities are most likely to adopt the four-electron mechanism with a considerably low overpotential of only 0.44 and 0.76 V, respectively. Finally, we show that the adsorption energy of Li2O2 is a good descriptor for both ORR and OER catalytic activities, and weak Li2O2 adsorption behavior is positively related to low overpotentials and satisfactory catalytic performance.
作者
我是这篇论文的作者
点击您的名字以认领此论文并将其添加到您的个人资料中。
推荐
暂无数据