Operando neutron imaging-guided gradient design of Li-ion solid conductor for high-mass-loading cathodes

Tongtai Ji; Yuxuan Zhang; James Torres; Aleksandar S. Mijailovic; Ya Tang; Xianhui Zhao; Jean Christophe Bilheux; Jiwei Wang; Brian W. Sheldon; Oluwafemi Oyedeji; Hongli Zhu

doi:10.1038/s41467-025-62518-y

Operando neutron imaging-guided gradient design of Li-ion solid conductor for high-mass-loading cathodes

Tongtai Ji
, Yuxuan Zhang
, James Torres
, Aleksandar S. Mijailovic
, Ya Tang
, Xianhui Zhao
, Jean Christophe Bilheux
, Jiwei Wang
, Brian W. Sheldon
, Oluwafemi Oyedeji
, Hongli Zhu

Research output: Contribution to journal › Article › peer-review

11 Scopus citations

Abstract

High-mass-loading cathodes are crucial for achieving high energy density in all-solid-state batteries from the lab scale to industry. However, as mass-loading increases, electrochemical performance is significantly compromised due to sluggish kinetics. In this work, operando neutron imaging is deployed on a high-mass-loading NMC 811 cathode of 33 mg/cm² (5.0 mAh/cm²) and directly visualizes the lithiation prioritization of the cathode active material (CAM) from the solid electrolyte membrane side to the current collector side. In addition to the tortuosity, another key limitation on ion transfer in the cathode arises from the mismatch between the uniform distribution of the solid electrolyte (catholyte) in the conventional composite cathode and the non-uniform Li⁺ flux generated by the faradaic reaction of CAMs. Therefore, we engineer a gradient in the catholyte concentration to match the Li⁺ flux distribution as a means of eliminating the ion transfer obstacle. This approach demonstrates enhanced rate performance, even with high-mass-loading cathodes. A LiCoO₂ composite cathode with 100 mg/cm² high-mass-loading exhibits an areal capacity of 10.4 mAh/cm² at a current density of 2.25 mA/cm². This work provides insight into the ion-transport limitation in thick cathodes and demonstrates an effective gradient design to overcome the kinetic barrier and achieve high battery performance.

Original language	English
Article number	7667
Journal	Nature Communications
Volume	16
Issue number	1
DOIs	https://doi.org/10.1038/s41467-025-62518-y
State	Published - Dec 2025

Funding

This research used resources at the High Flux Isotope Reactor, a DOE Office of Science User Facility operated by the Oak Ridge National Laboratory. H.Z. acknowledges the primary support of the US Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences under award number DESC0024528. The authors would like to acknowledge support from the US Department of Energy (DOE) Bioenergy Technologies Office (BETO) Projects under contract with UT-Battelle LLC. This manuscript was partially authored by UT-Battelle LLC under contract DE-AC05-00OR22725 with DOE. The US government retains and the publisher, by accepting the article for publication, acknowledges that the US government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript, or allow others to do so, for US government purposes. DOE will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan ( http://energy.gov/downloads/doe-public-access-plan ).

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title = "Operando neutron imaging-guided gradient design of Li-ion solid conductor for high-mass-loading cathodes",

abstract = "High-mass-loading cathodes are crucial for achieving high energy density in all-solid-state batteries from the lab scale to industry. However, as mass-loading increases, electrochemical performance is significantly compromised due to sluggish kinetics. In this work, operando neutron imaging is deployed on a high-mass-loading NMC 811 cathode of 33 mg/cm2 (5.0 mAh/cm2) and directly visualizes the lithiation prioritization of the cathode active material (CAM) from the solid electrolyte membrane side to the current collector side. In addition to the tortuosity, another key limitation on ion transfer in the cathode arises from the mismatch between the uniform distribution of the solid electrolyte (catholyte) in the conventional composite cathode and the non-uniform Li+ flux generated by the faradaic reaction of CAMs. Therefore, we engineer a gradient in the catholyte concentration to match the Li+ flux distribution as a means of eliminating the ion transfer obstacle. This approach demonstrates enhanced rate performance, even with high-mass-loading cathodes. A LiCoO2 composite cathode with 100 mg/cm2 high-mass-loading exhibits an areal capacity of 10.4 mAh/cm2 at a current density of 2.25 mA/cm2. This work provides insight into the ion-transport limitation in thick cathodes and demonstrates an effective gradient design to overcome the kinetic barrier and achieve high battery performance.",

author = "Tongtai Ji and Yuxuan Zhang and James Torres and Mijailovic, \{Aleksandar S.\} and Ya Tang and Xianhui Zhao and Bilheux, \{Jean Christophe\} and Jiwei Wang and Sheldon, \{Brian W.\} and Oluwafemi Oyedeji and Hongli Zhu",

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AU - Ji, Tongtai

AU - Zhang, Yuxuan

AU - Torres, James

AU - Mijailovic, Aleksandar S.

AU - Tang, Ya

AU - Zhao, Xianhui

AU - Bilheux, Jean Christophe

AU - Wang, Jiwei

AU - Sheldon, Brian W.

AU - Oyedeji, Oluwafemi

AU - Zhu, Hongli

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AB - High-mass-loading cathodes are crucial for achieving high energy density in all-solid-state batteries from the lab scale to industry. However, as mass-loading increases, electrochemical performance is significantly compromised due to sluggish kinetics. In this work, operando neutron imaging is deployed on a high-mass-loading NMC 811 cathode of 33 mg/cm2 (5.0 mAh/cm2) and directly visualizes the lithiation prioritization of the cathode active material (CAM) from the solid electrolyte membrane side to the current collector side. In addition to the tortuosity, another key limitation on ion transfer in the cathode arises from the mismatch between the uniform distribution of the solid electrolyte (catholyte) in the conventional composite cathode and the non-uniform Li+ flux generated by the faradaic reaction of CAMs. Therefore, we engineer a gradient in the catholyte concentration to match the Li+ flux distribution as a means of eliminating the ion transfer obstacle. This approach demonstrates enhanced rate performance, even with high-mass-loading cathodes. A LiCoO2 composite cathode with 100 mg/cm2 high-mass-loading exhibits an areal capacity of 10.4 mAh/cm2 at a current density of 2.25 mA/cm2. This work provides insight into the ion-transport limitation in thick cathodes and demonstrates an effective gradient design to overcome the kinetic barrier and achieve high battery performance.

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Operando neutron imaging-guided gradient design of Li-ion solid conductor for high-mass-loading cathodes

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