This paper reports a multiscale controlled three‐dimensional (3D) electrode structure to boost the battery performance for thick electrode batteries with LiMn1.5Ni0.5O4 as cathode material, which exhibits a high areal capacity (3.5 mAh/cm2) along with a high specific capacity (130 mAh/g). This excellent battery performance is achieved by a new concept of cell electrode fabrication, which simultaneously controls the electrode structure in a multiscale manner to address the key challenges of the material. Particles with ultrathin conformal coating layers are prepared through atomic layer deposition followed by a nanoscale‐controlled, thermal diffusion doping. The particles are organized into a macroscale‐controlled 3D hybrid‐structure. This synergistic control of nano‐/macro‐structures is a promising concept for enhancing battery performance and its cycle life. The nanoscale coating/doping provides enhanced fundamental properties, including transport and structural properties, while the mesoscale control can provide a better network of the nanostructured elements by decreasing the diffusion path between. Electrochemical tests have shown that the synergistically controlled electrode exhibits the best performance among non‐controlled and selectively‐controlled samples, in terms of specific capacity, areal capacity, and cycle life.


Chemical and Biochemical Engineering

Second Department

Mechanical and Aerospace Engineering

Research Center/Lab(s)

Intelligent Systems Center

Second Research Center/Lab

Center for High Performance Computing Research


The authors gratefully acknowledge the financial support from National Science Foundation Awards (CMMI‐1563029, CBET‐1510085)

Keywords and Phrases

Atomic Layer Deposition; Lithium-Ion Batteries; Materials Science; Multiscale Controlled Structure; Thick Electrode

International Standard Serial Number (ISSN)


Document Type

Article - Journal

Document Version

Final Version

File Type





© 2019 Wiley-VCH Verlag, All rights reserved.

Publication Date

01 Oct 2018