journal article·2022-05-10

High-Rate Lithium Cycling and Structure Evolution in Mo4O11

Rebecca C. Vincent, Yunkai Luo, Jessica L. Andrews, Arava Zohar, Yucheng Zhou, Qizhang Yan, Eve M. Mozur, Molleigh B. Preefer, Johanna Nelson Weker, Anthony K. Cheetham, Jian Luo, Laurent Pilon, Brent C. Melot, Bruce Dunn, Ram Seshadri

Chemistry of Materials· Volume 34· Issue 9
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Abstract

Shear-phase early transition metal oxides, mostly of Nb, and comprising edge- and corner-shared metal–oxygen octahedra have seen a resurgence in recent years as fast-charging, low-voltage electrodes for Li+-ion batteries. Mo oxides, broadly, have been less well studied as fast-charging electrodes. Here we examine a reduced Mo oxide, Mo4O11, that has a structure comprising only corner-connected MoO4 tetrahedra and MoO6 octahedra. We show that an electrode formed using micrometer-sized particles of Mo4O11 as the active material can function as a high-rate Li+-ion electrode against Li metal, with a stable capacity of over 200 mAh g–1 at the high rate of 5C. Operando X-ray diffraction (XRD), entropic potential measurements, and ex situ Raman spectroscopy are employed to understand the nature of the charge storage. The crystal structure dramatically changes upon the first lithiation, and subsequent cycling is completely reversible with low capacity fade. It is the newly formed and potentially more layered structure that demonstrates high-rate cycling and small voltage polarization. A space group and unit cell for the new structure is proposed. This finding expands the scope of candidate high-rate electrode materials to those beyond the expected Nb-containing shear-phase oxide materials.
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Research context

OpenAlex topics: Advancements in Battery Materials · Semiconductor materials and devices · Supercapacitor Materials and Fabrication

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Materials Department and Materials Research Laboratory, University of California, Santa Barbara, California 93106, United States

Department of Materials Science and Engineering, University of California, Los Angeles, California 90095, United States

Department of Chemistry, University of Southern California, Los Angeles, California 90089, United States

Mechanical and Aerospace Engineering Department, University of California, Los Angeles, California 90095, United States

Department of Nanoengineering, University of California San Diego, La Jolla, California 92093, United States

Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, Menlo Park, California 94025, United States

Program of Materials Science and Engineering, University of California San Diego, La Jolla, California 92093, United States

Department of Chemical Engineering and Materials Science, University of Southern California, Los Angeles, California 90089, United States

Funding

Basic Energy Sciences · Division of Graduate Education

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