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Title: Excess Li-Ion Storage on Reconstructed Surfaces of Nanocrystals To Boost Battery Performance

Because of their enhanced kinetic properties, nanocrystallites have received much attention as potential electrode materials for energy storage. However, because of the large specific surface areas of nanocrystallites, they usually suffer from decreased energy density, cycling stability, and effective electrode capacity. Here, in this work, we report a size-dependent excess capacity beyond theoretical value (170 mA h g -1) by introducing extra lithium storage at the reconstructed surface in nanosized LiFePO 4 (LFP) cathode materials (186 and 207 mA h g -1 in samples with mean particle sizes of 83 and 42 nm, respectively). Moreover, this LFP composite also shows excellent cycling stability and high rate performance. Our multimodal experimental characterizations and ab initio calculations reveal that the surface extra lithium storage is mainly attributed to the charge passivation of Fe by the surface C–O–Fe bonds, which can enhance binding energy for surface lithium by compensating surface Fe truncated symmetry to create two types of extra positions for Li-ion storage at the reconstructed surfaces. Such surface reconstruction nanotechnology for excess Li-ion storage makes full use of the large specific surface area of the nanocrystallites, which can maintain the fast Li-ion transport and greatly enhance the capacity. Finally, this discovery andmore » nanotechnology can be used for the design of high-capacity and efficient lithium ion batteries.« less
Authors:
 [1] ;  [1] ;  [1] ;  [1] ;  [2] ;  [2] ;  [3] ;  [1] ;  [1] ;  [1] ;  [1] ;  [4] ;  [1] ;  [1] ;  [1] ; ORCiD logo [2] ;  [5] ;  [1] ;  [6] ; ORCiD logo [3] more »;  [7] ; ORCiD logo [2] ; ORCiD logo [2] ; ORCiD logo [1] « less
  1. Peking University, Shenzhen Graduate School (China). School of Advanced Materials
  2. Argonne National Lab. (ANL), Argonne, IL (United States). Center for Nanoscale Materials
  3. Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Environmental Molecular Sciences Laboratory
  4. Peking University, Shenzhen Graduate School (China). School of Advanced Materials; Argonne National Lab. (ANL), Argonne, IL (United States). X-ray Science Division
  5. Argonne National Lab. (ANL), Argonne, IL (United States). X-ray Science Division
  6. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source
  7. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Science Division
Publication Date:
Grant/Contract Number:
AC02-06CH11357; AC02-05CH11231
Type:
Accepted Manuscript
Journal Name:
Nano Letters
Additional Journal Information:
Journal Volume: 17; Journal Issue: 10; Journal ID: ISSN 1530-6984
Publisher:
American Chemical Society
Research Org:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); USDOE Office of Energy Efficiency and Renewable Energy (EERE); National Natural Science Foundation of China (NNSFC)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 25 ENERGY STORAGE; Cathode materials; excess capacity; lithium-ion batteries; reconstructed surface; size-dependent
OSTI Identifier:
1414428