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Title: Lithiation Mechanism of Tunnel-Structured MnO 2 Electrode Investigated by In Situ Transmission Electron Microscopy

Journal Article · · Advanced Materials
 [1];  [2];  [2];  [3];  [3];  [3];  [4];  [5];  [2]
  1. Brookhaven National Lab. (BNL), Upton, NY (United States); Seoul National Univ. (Korea, Republic of)
  2. Brookhaven National Lab. (BNL), Upton, NY (United States)
  3. Stony Brook Univ., NY (United States)
  4. Brookhaven National Lab. (BNL), Upton, NY (United States); Stony Brook Univ., NY (United States)
  5. Seoul National Univ. (Korea, Republic of)
+ Show Author Affiliations

Abstract Manganese oxide (α‐MnO 2 ) has been considered a promising energy material, including as a lithium‐based battery electrode candidate, due to its environmental friendliness. Thanks to its unique 1D [2 × 2] tunnel structure, α‐MnO 2 can be applied to a cathode by insertion reaction and to an anode by conversion reaction in corresponding voltage ranges, in a lithium‐based battery. Numerous reports have attributed its remarkable performance to its unique tunnel structure; however, the precise electrochemical reaction mechanism remains unknown. In this study, finding of the lithiation mechanism of α‐MnO 2 nanowire by in situ transmission electron microscopy (TEM) is reported. By elaborately modifying the existing in situ TEM experimental technique, rapid lithium‐ion diffusion through the tunnels is verified. Furthermore, by tracing the full lithiation procedure, the evolution of the MnO intermediate phase and the development of the MnO and Li 2 O phases with preferred orientations is demonstrated, which explains how the conversion reaction occurs in α‐MnO 2 material. This study provides a comprehensive understanding of the electrochemical lithiation process and mechanism of α‐MnO 2 material, in addition to the introduction of an improved in situ TEM biasing technique.

Research Organization:
Brookhaven National Laboratory (BNL), Upton, NY (United States); Energy Frontier Research Centers (EFRC) (United States). Center for Mesoscale Transport Properties (m2M)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
SC0012704; DESC0012704
OSTI ID:
1425056
Alternate ID(s):
OSTI ID: 1398290
Report Number(s):
BNL-200057-2018-JAAM; TRN: US1802020
Journal Information:
Advanced Materials, Vol. 29, Issue 43; ISSN 0935-9648
Publisher:
WileyCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 53 works
Citation information provided by
Web of Science

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Cited By (6)

Nanowires in Energy Storage Devices: Structures, Synthesis, and Applications journal October 2018
Reversible Intercalation of Multivalent Al 3+ Ions into Potassium‐Rich Cryptomelane Nanowires for Aqueous Rechargeable Al‐Ion Batteries journal June 2019
Flexible Graphene-Wrapped Carbon Nanotube/Graphene@MnO 2 3D Multilevel Porous Film for High-Performance Lithium-Ion Batteries journal July 2018
In situ TEM study of lithiation into a PPy coated α-MnO 2 /graphene foam freestanding electrode journal January 2018
Highly effective fabrication of two dimensional metal oxides as high performance lithium storage anodes journal January 2019
Reversible Intercalation of Multivalent Al 3+ Ions into Potassium‐Rich Cryptomelane Nanowires for Aqueous Rechargeable Al‐Ion Batteries journal July 2019

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