Enhanced Cycle Performance of Rechargeable Li-CO2 Batteries Using Nanostructured AMn2O4 (A = Ni, Zn, Co) Electrocatalysts

ACS Appl Mater Interfaces. 2025 Jan 1. doi: 10.1021/acsami.4c10764. Online ahead of print.

Abstract

Rechargeable Li-CO2 batteries face challenges of sluggish reaction kinetics and poor rechargeability. Highly efficient electrocatalysts are urgently needed to decompose the discharge product, Li2CO3. Mn-based transition metal oxides are regarded as promising candidates for improving the cycle performance and reaction kinetics of Li-CO2 batteries. Notably, morphology engineering plays a vital role in enhancing electrocatalytic performance by tuning the structure of the electrode. Herein, we adopted a morphology engineering strategy to develop nanostructured Mn-based electrocatalysts with high surface area and rich active sites. The nanostructured electrocatalysts were synthesized using a facile anodic electrodeposition method by depositing Mn-based hydroxides directly onto a carbon cloth electrode, followed by a calcination process. The electrochemical characterization showed that the Li-CO2 battery with Mn-based transition metal oxides AMn2O4 (A = Ni, Zn, Co) achieves impressive cycle performance (over 150 cycles at 100 mA/g). This work not only exhibits the excellent electrocatalytic performance of Mn-based transition metal oxide but also demonstrates a general selection principle for next-generation electrocatalysts for metal-CO2 batteries.

Keywords: CO2 conversion; Li-CO2 batteries; NiMn2O4; electrocatalysts; nanomaterials; transition metal oxide.