Ru Single Atoms on N-Doped Carbon by Spatial Confinement and Ionic Substitution Strategies for High-Performance Li-O2 Batteries

Xiaolin Hu; Gan Luo; Qiannan Zhao; Dan Wu; Tongxin Yang; Jie Wen; Ronghua Wang; Chaohe Xu; Ning Hu

doi:10.1021/jacs.0c07317

Ru Single Atoms on N-Doped Carbon by Spatial Confinement and Ionic Substitution Strategies for High-Performance Li-O₂ Batteries

J Am Chem Soc. 2020 Sep 30;142(39):16776-16786. doi: 10.1021/jacs.0c07317. Epub 2020 Sep 17.

Authors

Xiaolin Hu¹, Gan Luo¹, Qiannan Zhao¹, Dan Wu¹, Tongxin Yang¹, Jie Wen¹, Ronghua Wang², Chaohe Xu¹, Ning Hu^{1

3}

Affiliations

¹ College of Aerospace Engineering, Chongqing University, Chongqing 400044, China.
² College of Materials Science and Engineering, Chongqing University, Chongqing 400044, China.
³ School of Mechanical Engineering, Hebei University of Technology, Tianjin 300401, China.

PMID: 32876448
DOI: 10.1021/jacs.0c07317

Abstract

Nonaqueous rechargeable lithium-oxygen batteries (LOBs) are one of the most promising candidates for future electric vehicles and wearable/flexible electronics. However, their development is severely hindered by the sluggish kinetics of the ORR and OER during the discharge and charge processes. Here, we employ MOF-assisted spatial confinement and ionic substitution strategies to synthesize Ru single atoms riveted with nitrogen-doped porous carbon (Ru SAs-NC) as the electrocatalytic material. By using the optimized Ru_0.3 SAs-NC as electrocatalyst in the oxygen-breathing electrodes, the developed LOB can deliver the lowest overpotential of only 0.55 V at 0.02 mA cm^-2. Moreover, in-situ DEMS results quantify that the e^-/O₂ ratio of LOBs in a full cycle is only 2.14, indicating a superior electrocatalytic performance in LOB applications. Theoretical calculations reveal that the Ru-N₄ serves as the driving force center, and the amount of this configuration can significantly affect the internal affinity of intermediate species. The rate-limiting step of the ORR on the catalyst surface is the occurrence of 2e^- reactions to generate Li₂O₂, while that of the OER pathway is the oxidation of Li₂O₂. This work broadens the field of vision for the design of single-site high-efficiency catalysts with maximum atomic utilization efficiency for LOBs.