Effectively suppressing dissolution of manganese from spinel lithium manganate via a nanoscale surface-doping approach

Journal Article · Tue Dec 16 00:00:00 EST 2014 · Nature Communications

DOI:https://doi.org/10.1038/ncomms6693· OSTI ID:1210455

Lu, Jun ^[1]; Zhan, Chun ^[2]; Wu, Tianpin ^[3]; Wen, Jianguo ^[4]; Lei, Yu ^[5]; Kropf, A. Jeremy ^[2]; Wu, Huiming ^[2]; Miller, Dean J. ^[4]; Elam, Jeffrey W. ^[6]; Sun, Yang-Kook ^[7]; Qiu, Xinping ^[8]; Amine, Khalil ^[2]

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1. Argonne National Lab. (ANL), Argonne, IL (United States). Chemical Sciences and Engineering Division; Tsinghua Univ., Beijing (China). Key Lab. of Organic Optoelectronics and Molecular Engineering, Dept. of Chemistry
2. Argonne National Lab. (ANL), Argonne, IL (United States). Chemical Sciences and Engineering Division
3. Argonne National Lab. (ANL), Argonne, IL (United States). X-Ray Science Division
4. Argonne National Lab. (ANL), Argonne, IL (United States). Electron Microscopy Center
5. Univ. of Alabama, Huntsville, AL (United States). Dept. of Chemical and Materials Engineering
6. Argonne National Lab. (ANL), Argonne, IL (United States). Energy System Division
7. Hanyang Univ., Seoule (Republic of Korea). Dept. of Energy Engineering
8. Tsinghua Univ., Beijing (China). Key Lab. of Organic Optoelectronics and Molecular Engineering, Dept. of Chemistry

The capacity fade of lithium manganate-based cells is associated with the dissolution of Mn from cathode/electrolyte interface due to the disproportionation reaction of Mn(III), and the subsequent deposition of Mn(II) on the anode. Suppressing the dissolution of Mn from the cathode is critical to reducing capacity fade of LiMn₂O₄-based cells. Here we report a nanoscale surface-doping approach that minimizes Mn dissolution from lithium manganate. This approach exploits advantages of both bulk doping and surface-coating methods by stabilizing surface crystal structure of lithium manganate through cationic doping while maintaining bulk lithium manganate structure, and protecting bulk lithium manganate from electrolyte corrosion while maintaining ion and charge transport channels on the surface through the electrochemically active doping layer. Consequently, the surface-doped lithium manganate demonstrates enhanced electrochemical performance. This study provides encouraging evidence that surface doping could be a promising alternative to improve the cycling performance of lithium-ion batteries.

• Research Organization: Energy Frontier Research Centers (EFRC) (United States). Center for Electrical Energy Storage (CEES)
• Sponsoring Organization: USDOE Office of Science (SC), Basic Energy Sciences (BES)
• DOE Contract Number: AC02-06CH11357
• OSTI ID: 1210455
• Journal Information: Nature Communications, Vol. 5; Related Information: CEES partners with Argonne National Laboratory (lead); University of Illinois, Urbana-Champaign; Northwest University; ISSN 2041-1723
• Publisher: Nature Publishing Group
• Country of Publication: United States
• Language: English

Related Subjects

energy storage (including batteries and capacitors)
charge transport
materials and chemistry by design
synthesis (novel materials)