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Title: Solvent-directed Solgel Assembly of 3-dimensional Graphene-tented Metal Oxides and Strong Synergistic Disparities in Lithium Storage

Journal Article · · Journal of Materials Chemistry. A
DOI:https://doi.org/10.1039/C5TA10730J· OSTI ID:1241936
 [1];  [2];  [1];  [1];  [1];  [1];  [3];  [1];  [1];  [4];  [5];  [2]
  1. Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
  2. Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States); Arizona State Univ., Tempe, AZ (United States)
  3. Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States); National Renewable Energy Lab. (NREL), Golden, CO (United States)
  4. Arizona State Univ., Tempe, AZ (United States)
  5. Rice Univ., Houston, TX (United States)

The graphene/metal oxide (GMO) nanocomposites promise a broad range of utilities for lithium ion batteries (LIBs), pseudocapacitors, catalysts, and sensors. When applied as anodes for LIBs, GMOs often exhibit high capacity, improved rate capability and cycling performance. Numerous studies have attributed these favorable properties to the charisma of graphene in assisting various metal oxides (MOs) to achieve near-theoretical capacities, exploiting the exceptional electronic and mechanical properties of graphene. By comparison, the true lithium storage mechanisms of graphene and their correlations with MOs remain enigmatic. Via a unique two-step liquid-flow-guided solgel process, we have synthesized and investigated the electrochemical performance of several representative GMOs, namely Fe2O3/graphene, SnO2/graphene, and TiO2/graphene. We observe that MOs play an equally important role in promoting graphene to achieve large reversible lithium storage capacity. Our experiments suggest that the unexpected lithium storage heightening may arise from a unique surface coverage mechanism of MOs. The magnitude of capacity improvement is found to scale crudely with the surface coverage of MOs but depend strongly upon the storage mechanisms of MOs variety. Importantly, synergistic effect is only observed in conversion reaction GMOs (i.e., Fe2O3/graphene and SnO2/graphene) but not in intercalationbased GMOs (i.e., TiO2/graphene). Our first principles calculations suggest an alternative lithium storage sites from resultant interfaces between Li2O and graphene that agree with our experimental observations. This unusually beneficial role of MOs to graphene suggests an effective pathway for reversible lithium storage in graphene and shifts design paradigms for graphene-based electrodes.

Research Organization:
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
Sponsoring Organization:
USDOE
Grant/Contract Number:
AC52-07NA27344
OSTI ID:
1241936
Report Number(s):
LLNL-JRNL-676537
Journal Information:
Journal of Materials Chemistry. A, Vol. 4; ISSN 2050-7488
Publisher:
Royal Society of ChemistryCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 17 works
Citation information provided by
Web of Science

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