4.8 Article

Mesocrystallizing Nanograins for Enhanced Li+ Storage

Journal

ADVANCED ENERGY MATERIALS
Volume 11, Issue 26, Pages -

Publisher

WILEY-V C H VERLAG GMBH
DOI: 10.1002/aenm.202100503

Keywords

Li-ion storage; mesocrystalline; metal oxides; transmission electron microscopy

Funding

  1. National Nature Science Foundation of China [51922008, 51872075]
  2. 111 project [D17007]
  3. Henan Center for Outstanding Overseas Scientists [GZS2018003]
  4. U.S. Department of Energy (DOE), Office of Energy Efficiency and Renewable Energy, Vehicle Technologies Office under Clean Vehicles, US-China Clean Energy Research Centre (CERC-CVC2)
  5. DOE Office of Science [DE-AC02-06CH11357]
  6. National Science Foundation [CBET-1805938]

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The morphology and crystallinity of electrode materials play a crucial role in their charge carrier storage properties in rechargeable batteries. By designing electrode particles consisting of numerous nanograins with uniform crystalline orientation, both high surface area and high structural integrity can be achieved, significantly improving Li+ storage kinetics and performance. The mesocrystalline NiCo2O4 electrode exhibits a high specific capacity of 1403 mAh g(-1) after 200 cycles at 1.6 A g(-1) (a rate of 1.8 C), demonstrating the effectiveness of this strategy in enhancing battery performance.
The morphology and crystallinity of electrode materials have a major effect on their charge carrier storage properties when applied in rechargeable batteries. While nanosizing electrode particles (with larger surface area) and maintaining electrode integrity are both good for performance enhancement, they seem to contradict each other and are challenging to balanced. Herein, electrode particles consisting of numerous nanograins with uniform crystalline orientation are designed to guarantee both high surface area and high structural integrity, allowing the significant improvement of Li+ storage kinetics and performance. Applying this mesocrystallizing strategy to an NiCo2O4-based anode, results in various degrees of pseudocapacitance response, the long-term cyclability and rate performance of this material are also significantly enhanced. Impressively, the mesocrystalline NiCo2O4 electrode exhibits a high specific capacity of 1403 mAh g(-1) after 200 cycles at 1.6 A g(-1) (a rate of 1.8 C). The growth mechanism of mesocrystalline materials with different morphologies is identified to be a topotactic structural transition process featuring a gradual edge-to-core corrosion process. This work presents an important synthetic clue to balance the morphology and crystallinity of battery electrode materials for their performance optimization and is expected to inspire future structural design for battery materials beyond the one prototyped here.

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