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

Shitong Wang; Lijiang Zhao; Yanhao Dong; He Zhu; Yang Yang; Haowei Xu; Baoming Wang; Yakun Yuan; Yang Ren; Xiaojing Huang; Wei Quan; Yutong Li; Yimeng Huang; Charles M. Settens; Qi He; Yongwen Sun; Hua Wang; Zunqiu Xiao; Wenjun Liu; Xianghui Xiao; Riqiang Fu; Qiang Li; Yong S. Chu; Zhongtai Zhang; Qi Liu; Andrew M. Minor; Junying Zhang; Zilong Tang; Ju Li

doi:10.1039/D2EE02918A

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

Shitong Wang,‡^a Lijiang Zhao,‡^b Yanhao Dong,

*^ac He Zhu,^d Yang Yang,^ef Haowei Xu,^a Baoming Wang,^g Yakun Yuan,^hi Yang Ren,^d Xiaojing Huang,^j Wei Quan,^kl Yutong Li,^c Yimeng Huang,^g Charles M. Settens,^m Qi He,^a Yongwen Sun,^e Hua Wang,^a Zunqiu Xiao,^c Wenjun Liu,ⁿ Xianghui Xiao,^j Riqiang Fu,

^o Qiang Li,^p Yong S. Chu,^j Zhongtai Zhang,^c Qi Liu,

^d Andrew M. Minor,^fq Junying Zhang,

*^b Zilong Tang

*^c and Ju Li

*^ag

Author affiliations

* Corresponding authors

^a Department of Nuclear Science and Engineering, Massachusetts Institute of Technology, Cambridge, MA 02139, USA
E-mail: dongyh@mit.edu, liju@mit.edu

^b School of Physics, Beihang University, Beijing 100191, China
E-mail: zjy@buaa.edu.cn

^c State Key Lab of New Ceramics and Fine Processing, School of Materials Science and Engineering, Tsinghua University, Beijing 100084, China
E-mail: tzl@tsinghua.edu.cn

^d Department of Physics, City University of Hong Kong, Kowloon, Hong Kong, China

^e Department of Engineering Science and Mechanics and Materials Research Institute, The Pennsylvania State University, University Park, PA 16802, USA

^f National Center for Electron Microscopy, Molecular Foundry, Lawrence Berkeley National Laboratory, Berkeley, CA 94702, USA

^g Department of Materials Science and Engineering, Massachusetts Institute of Technology, Cambridge, MA 02139, USA

^h School of Mechanical Engineering, Shanghai Jiao Tong University, Shanghai 200240, China

ⁱ Zhangjiang Institute for Advanced Study, Shanghai Jiao Tong University, Shanghai 201203, China

^j National Synchrotron Light Source II, Brookhaven National Laboratory, Upton, NY 11973, USA

^k China Automotive Battery Research Institute Co., Ltd., Beijing 101407, China

^l General Research Institute for Nonferrous Metals, Beijing 100088, China

^m Materials Research Laboratory, Massachusetts Institute of Technology, Cambridge, MA 02139, USA

ⁿ Advanced Photon Source, Argonne National Laboratory, Argonne, IL 60439, USA

^o National High Magnetic Field Laboratory, Florida State University, Tallahassee, FL 32310, USA

^p Beijing Advanced Innovation Center for Materials Genome Engineering, Institute of Solid State Chemistry, University of Science and Technology Beijing, Beijing 100083, China

^q Department of Materials Science and Engineering, University of California, Berkeley, CA 94702, USA

Abstract

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 10 000 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 (Nb₉W₄Ti₄O_42.5) and crystal size-coarsened H-Nb₂O₅ (>20 μm single crystals) with unprecedented performance.

Energy & Environmental Science

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

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

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