Issue 1, 2023

Pre-zeolite framework super-MIEC anodes for high-rate lithium-ion batteries


Zeolites, Prussian blue analogues (PBAs), and metal–organic frameworks (MOFs) rely on surface-like internal pore diffusions, which have generically low activation barriers to enable the rapid uptake of chemical species. Here we show that Wadsley–Roth oxides (WROs) with pore diameters of 2.5 Å < d < 2.8 Å, while excluding molecules, enable very rapid diffusion of Li+ in single-crystal particles >10 μm size. This supports full charge cycles at high rates of 30C, which would rival the filling up of gasoline vehicles, while reducing the contact and side reactions with the electrolyte and enhancing the cycle life up to 10000 cycles. Pore diffusion in WRO mixed ionic and electronic conductors (MIECs) differs from that in lithium intercalation compounds in the off-centered Li storage and low-coordination saddle points for migration. The reduced topological constraints per atom and large free volume in the host also lead to abnormally low or even negative thermal expansion and soft phonons, similar to other open frameworks such as zeolites, PBAs, and MOFs. Based on these guidelines, we have synthesized new composition (Nb9W4Ti4O42.5) and crystal size-coarsened H-Nb2O5 (>20 μm single crystals) with unprecedented performance.

Graphical abstract: Pre-zeolite framework super-MIEC anodes for high-rate lithium-ion batteries

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Article information

Article type
08 Sep 2022
23 Nov 2022
First published
14 Dec 2022
This article is Open Access
Creative Commons BY license

Energy Environ. Sci., 2023,16, 241-251

Pre-zeolite framework super-MIEC anodes for high-rate lithium-ion batteries

S. Wang, L. Zhao, Y. Dong, H. Zhu, Y. Yang, H. Xu, B. Wang, Y. Yuan, Y. Ren, X. Huang, W. Quan, Y. Li, Y. Huang, C. M. Settens, Q. He, Y. Sun, H. Wang, Z. Xiao, W. Liu, X. Xiao, R. Fu, Q. Li, Y. S. Chu, Z. Zhang, Q. Liu, A. M. Minor, J. Zhang, Z. Tang and J. Li, Energy Environ. Sci., 2023, 16, 241 DOI: 10.1039/D2EE02918A

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