Towards an ultra-long lifespan Li-CO2: electron structure and charge transfer pathway regulation on hierarchical architecture. [Dataset]

Abstract

Energy shortage and environmental pollution are severe challenges for achieving sustainable development of human society. Li-CO2 batteries offer particularly attractive merits in combination with CO2 fixation and energy storage, in which it shows a coming win–win blueprint by utilizing greenhouse gas (CO2) as fuel, to alleviate energy shortage and global warming issues. In addition, it is also considered to be one of the most promising beyond Li-ion technologies, with a theoretical energy density of 1876 Wh kg−1, far exceeding that of Li-ion batteries (≈265 Wh kg−1). Evidently, the most common reaction mechanism of Li-CO2 batteries is associated with the formation of lithium carbonate (Li2CO3) through a four-electron reaction: 4Li+ + 3CO2 + 4e- ↔ 2Li2CO3 + C, (Eo = 2.80 V vs Li/Li+), during the CO2 reduction reaction/CO2 evolution reaction (CRR/CER) process. Unfortunately, Li2CO3 is a wide band gap insulator, leading to sluggish kinetics for its decomposition during the CER process (a high charge voltage up to 4.30 V vs Li/Li+). Such a high charge potential accelerates both electrode oxidation and electrolyte decompositions. The accumulation of solid carbonate species on the cathode surface, relative to incomplete decomposition or irreversible formation of Li2CO3, results in a distinct decrease of space and active sites, further leading to problems such as high polarization gap, poor cycle stability and "sudden death". It is therefore highly urgent to develop compatible electrode materials to boost their lifespan and reduce polarization voltage by facilitating the reversible formation/decomposition of Li2CO3 during the discharge/charge processes. There are several pathways to tailor the decomposition behavior of Li2CO3 in the past decade. Firstly, the decomposition of Li2CO3 can be promoted by chemically bonding the catalysts or changing the stable triangular structure of the carbonate. Secondary, to promote decomposition, the discharge product Li2CO3 with small particle size or thin-film morphology is also desirable. Thirdly, highly stable amorphous intermediate discharge product Li2C2O4 on Li2CO3 can enhance battery cycle efficiency. Finally, the increment of the specific surface area of the cathode catalyst would induce uniform nucleation or decomposition of discharge products. Although the electrochemical properties of Li-CO2 batteries are improved greatly, the cyclability is still far beneath the industrial threshold.

Citation

WANG, Y., WANG, J., WANG, J., YANG, M., ZOU, G., LI, L., TSE, J.S., FERNANDEZ, C. and PENG, Q. 2022. Towards an ultra-long lifespan Li-CO2: electron structure and charge transfer pathway regulation on hierarchical architecture. [Dataset]. Chemical engineering journal [online], 451(Part 3), article 138953. Available from: https://www.sciencedirect.com/science/article/pii/S1385894722044321#s0075

• Acceptance Date: Aug 29, 2022
• Online Publication Date: Sep 3, 2022
• Publication Date: Jan 1, 2023
• Deposit Date: Sep 9, 2022
• Publicly Available Date: Sep 4, 2023
• Publisher: Elsevier
• DOI: https://doi.org/10.1016/j.cej.2022.138953
• Keywords: MXene; Li-CO2 batteries; Catalyst; Ultra-long lifespan; Low overpotential
• Public URL: https://rgu-repository.worktribe.com/output/1745268
• Publisher URL: https://www.sciencedirect.com/science/article/pii/S1385894722044321?via%3Dihub#s0075
• Related Public URLs: https://rgu-repository.worktribe.com/output/1745237
• Type of Data: MP4 video, DOCX file and accompanying TXT file.
• Collection Date: Aug 20, 2022
• Collection Method: The full experimental methods, results and discussion is described in a published journal article: WANG, Y., WANG, J., WANG, J., YANG, M., ZOU, G., LI, L., TSE, J.S., FERNANDEZ, C. and PENG, Q. 2022. Towards an ultra-long lifespan Li-CO2: electron structure and charge transfer pathway regulation on hierarchical architecture. Chemical engineering journal [online], 451(Part 3), article 138953. Available from: https://doi.org/10.1016/j.cej.2022.138953