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Title: Enhancing the Electrode Gravimetric Capacity of Li1.2Mn0.4Ti0.4O2 Cathode Using Interfacial Carbon Deposition and Carbon Nanotube-Mediated Electrical Percolation

Journal Article · · ACS Applied Materials and Interfaces
 [1];  [2];  [3]; ORCiD logo [1];  [1]; ORCiD logo [3]; ORCiD logo [1];  [4]; ORCiD logo [1]
  1. Rice University, Houston, TX (United States)
  2. University of Tennessee, Knoxville, TN (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
  3. Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
  4. Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Mn-based cation disordered rocksalt oxides (Mn-DRX) are emerging as promising cathode materials for next-generation Li-ion batteries due to their high specific capacities and cobalt and nickel free characteristic. However, to reach the theoretical capacity, solid-state method synthesized Mn-DRX materials require activation via post-synthetic ball milling, typically incorporating more than 20 wt.% conductive carbon that adversely reduces the electrode level gravimetric capacity. To solve this issue, we firstly deposit amorphous carbon on the surface of the Li1.2Mn0.4Ti0.4O2 (LMTO) particles to increase the electrical conductivity by a five order of magnitude. Although the cathode material gravimetric first charge capacity reaches 180 mAh/g, its highly irreversible behavior leads to a 70 mAh/g first discharge capacity. Subsequently, to ensure a good electrical percolation network, the LMTO material is ball milled with multi-wall carbon nanotube (CNT) to obtain a 78.7 wt.% LMTO active material loading in the cathode electrode (LMTO-CNT). As a result, a 210 mAh/g cathode electrode gravimetric first charge and 165 mAh/g first discharge capacity are obtained, compared to the respective capacity values of 222 mAh/g and 155 mAh/g for the LMTO ball milled with 20 wt.% SuperP C65 electrode (LMTO-SP). After 50 cycles, the LMTO-CNT delivers a 121 mAh/g electrode gravimetric discharge capacity, largely outperforming the 44 mAh/g value of the LMTO-SP. In conclusion, our study demonstrates that while ball milling is necessary to achieve the theoretical capacity of LMTO, a careful selection of the additive, such as CNT, effectively reduces the required carbon quantity to achieve a higher electrode gravimetric discharge capacity.

Research Organization:
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
Sponsoring Organization:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO); USDOE Office of Science (SC), Biological and Environmental Research (BER); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)
Grant/Contract Number:
AC05-76RL01830; AC05-00OR22725; LC-000 L053
OSTI ID:
2000452
Report Number(s):
PNNL-SA-181894
Journal Information:
ACS Applied Materials and Interfaces, Vol. 15, Issue 26; ISSN 1944-8244
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English

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