d-Electrons of Platinum Alloy Steering CO Pathway for Low-Charge Potential Li-CO 2 Batteries

• Published in: Angewandte Chemie International Edition 2024-11, p.e202415728
• Main Authors: Liu, Limin, Shen, Shenyu, Li, Jiatian, Zhao, Ning, Yin, Xiangkai, Zhao, Hongyang, Yu, Wei, Su, Yaqiong, Xia, Bao Yu, Ding, Shujiang
• Format: Article
• Language: English
• ISSN: 1433-7851; 1521-3773
• DOI: 10.1002/anie.202415728

Aprotic Li-CO batteries suffer from sluggish solid-solid co-oxidation kinetics of C and Li CO , requiring extremely high charging potentials and leading to serious side reactions and poor energy efficiency. Herein, we introduce a novel approach to address these challenges by modulating the reaction pathway with tailored Pt d-electrons and develop an aprotic Li-CO battery with CO and Li CO as the main discharge products. Note that the gas-solid co-oxidation reaction between CO and Li CO is both kinetically and thermodynamically more favorable. Consequently, the Li-CO batteries with CoPt alloy-supported on nitrogen-doped carbon nanofiber (CoPt@NCNF) cathode exhibit a charging potential of 2.89 V at 50 μA cm , which is the lowest charging potential to date. Moreover, the CoPt@NCNF cathode also shows exceptional cycling stability (218 cycles at 50 μA cm ) and high energy efficiency up to 74.6 %. Comprehensive experiments and theoretical calculations reveal that the lowered d-band center of CoPt alloy effectively promotes CO desorption and inhibits further CO reduction to C. This work provides promising insights into developing efficient and CO-selective Li-CO batteries.