Heterogeneous intercalated metal-organic framework active materials for fast-charging non-aqueous Li-ion capacitors

Nobuhiro Ogihara (), Masaki Hasegawa, Hitoshi Kumagai, Riho Mikita and Naoyuki Nagasako
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Nobuhiro Ogihara: Frontier Research Management Office, Toyota Central R&D Labs., Inc.
Masaki Hasegawa: Emerging Electrification Technology Div., Toyota Central R&D Labs., Inc.
Hitoshi Kumagai: Frontier Research Management Office, Toyota Central R&D Labs., Inc.
Riho Mikita: Emerging Electrification Technology Div., Toyota Central R&D Labs., Inc.
Naoyuki Nagasako: Frontier Research Management Office, Toyota Central R&D Labs., Inc.

Nature Communications, 2023, vol. 14, issue 1, 1-11

Abstract: Abstract Intercalated metal-organic frameworks (iMOFs) based on aromatic dicarboxylate are appealing negative electrode active materials for Li-based electrochemical energy storage devices. They store Li ions at approximately 0.8 V vs. Li/Li+ and, thus, avoid Li metal plating during cell operation. However, their fast-charging capability is limited. Here, to circumvent this issue, we propose iMOFs with multi-aromatic units selected using machine learning and synthesized via solution spray drying. A naphthalene-based multivariate material with nanometric thickness allows the reversible storage of Li-ions in non-aqueous Li metal cell configuration reaching 85% capacity retention at 400 mA g−1 (i.e., 30 min for full charge) and 20 °C compared to cycling at 20 mA g−1 (i.e., 10 h for full charge). The same material, tested in combination with an activated carbon-based positive electrode, enables a discharge capacity retention of about 91% after 1000 cycles at 0.15 mA cm−2 (i.e., 2 h for full charge) and 20 °C. We elucidate the charge storage mechanism and demonstrate that during Li intercalation, the distorted crystal structure promotes electron delocalization by controlling the frame vibration. As a result, a phase transition suppresses phase separation, thus, benefitting the electrode’s fast charging behavior.

Date: 2023
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DOI: 10.1038/s41467-023-37120-9

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