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Binuclear Cu complex catalysis enabling Li-CO₂ battery with a high discharge voltage above 3.0 V.

ABSTRACT: Li-CO₂ batteries possess exceptional advantages in using greenhouse gases to provide electrical energy. However, these batteries following Li₂CO₃-product route usually deliver low output voltage (<2.5 V) and energy efficiency. Besides, Li₂CO₃-related parasitic reactions can further degrade battery performance. Herein, we introduce a soluble binuclear copper(I) complex as the liquid catalyst to achieve Li₂C₂O₄ products in Li-CO₂ batteries. The Li-CO₂ battery using the copper(I) complex exhibits a high electromotive voltage up to 3.38 V, an increased output voltage of 3.04 V, and an enlarged discharge capacity of 5846 mAh g^-1. And it shows robust cyclability over 400 cycles with additional help of Ru catalyst. We reveal that the copper(I) complex can easily capture CO₂ to form a bridged Cu(II)-oxalate adduct. Subsequently reduction of the adduct occurs during discharge. This work innovatively increases the output voltage of Li-CO₂ batteries to higher than 3.0 V, paving a promising avenue for the design and regulation of CO₂ conversion reactions.

SUBMITTER: Sun X

PROVIDER: S-EPMC9892515 | biostudies-literature | 2023 Feb

REPOSITORIES: biostudies-literature

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Binuclear Cu complex catalysis enabling Li-CO2 battery with a high discharge voltage above 3.0 V.

Sun Xinyi X Mu Xiaowei X Zheng Wei W Wang Lei L Yang Sixie S Sheng Chuanchao C Pan Hui H Li Wei W Li Cheng-Hui CH He Ping P Zhou Haoshen H

Nature communications 20230201 1

Li-CO2 batteries possess exceptional advantages in using greenhouse gases to provide electrical energy. However, these batteries following Li2CO3-product route usually deliver low output voltage (<2.5 V) and energy efficiency. Besides, Li2CO3-related parasitic reactions can further degrade battery performance. Herein, we introduce a soluble binuclear copper(I) complex as the liquid catalyst to achieve Li2C2O4 ...[more]

PMID: 36725869

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Project description:The substitution of an organic liquid electrolyte with lithium-conducting solid materials is a promising approach to overcome the limitations associated with conventional lithium-ion batteries. These constraints include a reduced electrochemical stability window, high toxicity, flammability, and the formation of lithium dendrites. In this way, all-solid-state batteries present themselves as ideal candidates for improving energy density, environmental friendliness, and safety. In particular, all-solid-state configurations allow the introduction of compact, lightweight, high-energy-density batteries, suitable for low-power applications, known as thin-film batteries. Moreover, solid electrolytes typically offer wide electrochemical stability windows, enabling the integration of high-voltage cathodes and permitting the fabrication of higher-energy-density batteries. A high-voltage, all-solid-state lithium-ion thin-film battery composed of LiNi0.5Mn1.5O4 cathode, a LiPON solid electrolyte, and a lithium metal anode has been deposited layer by layer on low-cost stainless-steel current collector substrates. The structural and electrochemical properties of each electroactive component of the battery had been analyzed separately prior to the full cell implementation. In addition to a study of the internal solid-solid interface, comparing them was done with two similar cells assembled using conventional lithium foil, one with thin-film solid electrolyte and another one with thin-film solid electrolyte plus a droplet of LP30 liquid electrolyte. The thin-film all-solid state cell developed in this work delivered 80.5 mAh g-1 in the first cycle at C/20 and after a C-rate test of 25 cycles at C/10, C/5, C/2, and 1C and stabilized its capacity at around 70 mAh g-1 for another 12 cycles prior to the start of its degradation. This cell reached gravimetric and volumetric energy densities of 333 Wh kg-1 and 1,212 Wh l-1, respectively. Overall, this cell showed a better performance than its counterparts assembled with Li foil, highlighting the importance of the battery interface control.

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Binuclear Cu complex catalysis enabling Li-CO₂ battery with a high discharge voltage above 3.0 V.

Publications

Binuclear Cu complex catalysis enabling Li-CO<sub>2</sub> battery with a high discharge voltage above 3.0 V.

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