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Article Abstract

Given the high energy density and eco-friendly characteristics, lithium-carbon dioxide (Li-CO) batteries have been considered to be a next-generation energy technology to promote carbon neutral and space exploration. However, Li-CO batteries suffer from sluggish reaction kinetics, causing large overpotential and poor energy efficiency. Here, we observe enhanced reaction kinetics in aprotic Li-CO batteries with unconventional phase 4H/face-centered cubic (fcc) iridium (Ir) nanostructures grown on gold template. Significantly, 4H/fcc Ir exhibits superior electrochemical performance over fcc Ir in facilitating the round-trip reaction kinetics of Li-mediated CO reduction and evolution, achieving a low charge plateau below 3.61 V and high energy efficiency of 83.8%. Ex situ/in situ studies and theoretical calculations reveal that the boosted reaction kinetics arises from the highly reversible generation of amorphous/low-crystalline discharge products on 4H/fcc Ir via the Ir-O coupling. The demonstration of flexible Li-CO pouch cells with 4H/fcc Ir suggests the feasibility of using unconventional phase nanomaterials in practical scenarios.

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http://www.ncbi.nlm.nih.gov/pmc/articles/PMC9546633PMC
http://dx.doi.org/10.1073/pnas.2204666119DOI Listing

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