Boosting a practical Li-CO2 battery through dimerization reaction based on solid redox mediator

Abstract Li-CO2 batteries offer a promising avenue for converting greenhouse gases into electricity. However, the inherent challenge of direct electrocatalytic reduction of inert CO2 often results in the formation of Li2CO3, causing a dip in output voltage and energy efficiency. Our innovative appro...

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Main Authors: Wei Li, Menghang Zhang, Xinyi Sun, Chuanchao Sheng, Xiaowei Mu, Lei Wang, Ping He, Haoshen Zhou
Format: Article
Language:English
Published: Nature Portfolio 2024-01-01
Series:Nature Communications
Online Access:https://doi.org/10.1038/s41467-024-45087-4
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author Wei Li
Menghang Zhang
Xinyi Sun
Chuanchao Sheng
Xiaowei Mu
Lei Wang
Ping He
Haoshen Zhou
author_facet Wei Li
Menghang Zhang
Xinyi Sun
Chuanchao Sheng
Xiaowei Mu
Lei Wang
Ping He
Haoshen Zhou
author_sort Wei Li
collection DOAJ
description Abstract Li-CO2 batteries offer a promising avenue for converting greenhouse gases into electricity. However, the inherent challenge of direct electrocatalytic reduction of inert CO2 often results in the formation of Li2CO3, causing a dip in output voltage and energy efficiency. Our innovative approach involves solid redox mediators, affixed to the cathode via a Cu(II) coordination compound of benzene-1,3,5-tricarboxylic acid. This technique effectively circumvents the shuttle effect and sluggish kinetics associated with soluble redox mediators. Results show that the electrochemically reduced Cu(I) solid redox mediator efficiently captures CO2, facilitating Li2C2O4 formation through a dimerization reaction involving a dimeric oxalate intermediate. The Li-CO2 battery employing the Cu(II) solid redox mediator boasts a higher discharge voltage of 2.8 V, a lower charge potential of 3.7 V, and superior cycling performance over 400 cycles. Simultaneously, the successful development of a Li-CO2 pouch battery propels metal-CO2 batteries closer to practical application.
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spelling doaj.art-f950e21dcae84c1bb2757274bbf10bf92024-03-05T16:34:40ZengNature PortfolioNature Communications2041-17232024-01-0115111110.1038/s41467-024-45087-4Boosting a practical Li-CO2 battery through dimerization reaction based on solid redox mediatorWei Li0Menghang Zhang1Xinyi Sun2Chuanchao Sheng3Xiaowei Mu4Lei Wang5Ping He6Haoshen Zhou7Center of Energy Storage Materials & Technology, College of Engineering and Applied Sciences, Jiangsu Key Laboratory of Artificial Functional Materials, National Laboratory of Solid-State Microstructures and Collaborative Innovation Center of Advanced Microstructures, Nanjing UniversityCenter of Energy Storage Materials & Technology, College of Engineering and Applied Sciences, Jiangsu Key Laboratory of Artificial Functional Materials, National Laboratory of Solid-State Microstructures and Collaborative Innovation Center of Advanced Microstructures, Nanjing UniversityCenter of Energy Storage Materials & Technology, College of Engineering and Applied Sciences, Jiangsu Key Laboratory of Artificial Functional Materials, National Laboratory of Solid-State Microstructures and Collaborative Innovation Center of Advanced Microstructures, Nanjing UniversityCenter of Energy Storage Materials & Technology, College of Engineering and Applied Sciences, Jiangsu Key Laboratory of Artificial Functional Materials, National Laboratory of Solid-State Microstructures and Collaborative Innovation Center of Advanced Microstructures, Nanjing UniversityCenter of Energy Storage Materials & Technology, College of Engineering and Applied Sciences, Jiangsu Key Laboratory of Artificial Functional Materials, National Laboratory of Solid-State Microstructures and Collaborative Innovation Center of Advanced Microstructures, Nanjing UniversityCenter of Energy Storage Materials & Technology, College of Engineering and Applied Sciences, Jiangsu Key Laboratory of Artificial Functional Materials, National Laboratory of Solid-State Microstructures and Collaborative Innovation Center of Advanced Microstructures, Nanjing UniversityCenter of Energy Storage Materials & Technology, College of Engineering and Applied Sciences, Jiangsu Key Laboratory of Artificial Functional Materials, National Laboratory of Solid-State Microstructures and Collaborative Innovation Center of Advanced Microstructures, Nanjing UniversityCenter of Energy Storage Materials & Technology, College of Engineering and Applied Sciences, Jiangsu Key Laboratory of Artificial Functional Materials, National Laboratory of Solid-State Microstructures and Collaborative Innovation Center of Advanced Microstructures, Nanjing UniversityAbstract Li-CO2 batteries offer a promising avenue for converting greenhouse gases into electricity. However, the inherent challenge of direct electrocatalytic reduction of inert CO2 often results in the formation of Li2CO3, causing a dip in output voltage and energy efficiency. Our innovative approach involves solid redox mediators, affixed to the cathode via a Cu(II) coordination compound of benzene-1,3,5-tricarboxylic acid. This technique effectively circumvents the shuttle effect and sluggish kinetics associated with soluble redox mediators. Results show that the electrochemically reduced Cu(I) solid redox mediator efficiently captures CO2, facilitating Li2C2O4 formation through a dimerization reaction involving a dimeric oxalate intermediate. The Li-CO2 battery employing the Cu(II) solid redox mediator boasts a higher discharge voltage of 2.8 V, a lower charge potential of 3.7 V, and superior cycling performance over 400 cycles. Simultaneously, the successful development of a Li-CO2 pouch battery propels metal-CO2 batteries closer to practical application.https://doi.org/10.1038/s41467-024-45087-4
spellingShingle Wei Li
Menghang Zhang
Xinyi Sun
Chuanchao Sheng
Xiaowei Mu
Lei Wang
Ping He
Haoshen Zhou
Boosting a practical Li-CO2 battery through dimerization reaction based on solid redox mediator
Nature Communications
title Boosting a practical Li-CO2 battery through dimerization reaction based on solid redox mediator
title_full Boosting a practical Li-CO2 battery through dimerization reaction based on solid redox mediator
title_fullStr Boosting a practical Li-CO2 battery through dimerization reaction based on solid redox mediator
title_full_unstemmed Boosting a practical Li-CO2 battery through dimerization reaction based on solid redox mediator
title_short Boosting a practical Li-CO2 battery through dimerization reaction based on solid redox mediator
title_sort boosting a practical li co2 battery through dimerization reaction based on solid redox mediator
url https://doi.org/10.1038/s41467-024-45087-4
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