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Title: Rational Design of Hierarchically Open-Porous Spherical Hybrid Architectures for Lithium Ion Batteries

Journal Article · · Advanced Energy Materials
 [1]; ORCiD logo [2];  [3];  [1];  [4];  [5];  [6];  [1]
  1. Sungkyunkwan Univ. (SKKU), Jangangu, Suwon (Korea). School of Chemical Engineering
  2. Sungkyunkwan Univ. (SKKU), Jangangu, Suwon (Korea). School of Chemical Engineering; Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Division
  3. Univ. of Illinois, Urbana-Champaign, IL (United States). Frederick Seitz Materials Research Lab., Beckman Inst. for Advanced Science and Technology, Dept. of Materials Science and Engineering
  4. Pohang Accelerator Lab., Pohang (Republic of Korea). Beamline Research Division
  5. Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Division
  6. Univ. of Illinois, Urbana-Champaign, IL (United States). Frederick Seitz Materials Research Lab., Beckman Inst. for Advanced Science and Technology, Dept. of Materials Science and Engineering

Abstract Controlling the internal microstructure and overall morphology of building blocks used to form hybrid materials is crucial for the realization of deterministically designed architectures with desirable properties. Here, integrative spray‐frozen (SF) assembly is demonstrated for forming hierarchically structured open‐porous microspheres (hpMSs) composed of Fe 3 O 4 and reduced graphene oxide (rGO). The SF process drives the formation of a radially aligned microstructure within the sprayed colloidal droplets and also controls the overall microsphere morphology. The spherical Fe 3 O 4 /rGO hpMSs contain interconnected open pores, which, when used as a lithium‐ion battery anode, enables them to provide gravimetric and volumetric capacities of 1069.7 mAh g −1 and 686.7 mAh cm −3 , much greater than those of samples with similar composition and different morphologies. The hpMSs have good rate and cycling performance, retaining 78.5% capacity from 100 to 1000 mA g −1 and 74.6% capacity over 300 cycles. Using in situ synchrotron X‐ray absorption spectroscopy, the reaction pathway and phase evolution of the hpMSs are monitored enabling observation of the very small domain size and highly disordered nature of Fe x O y . The reduced capacity fade relative to other conversion systems is due to the good electrical contact between the pulverized Fe x O y particles and rGO, the overall structural integrity of the hpMSs, and the interconnected open porosity.

Research Organization:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Organization:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V); USDOE
Grant/Contract Number:
SC0012704; DE‐SC0012704
OSTI ID:
1485779
Alternate ID(s):
OSTI ID: 1488623
Report Number(s):
BNL-209738-2018-JAAM
Journal Information:
Advanced Energy Materials, Vol. 9, Issue 6; ISSN 1614-6832
Publisher:
WileyCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 42 works
Citation information provided by
Web of Science

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Cited By (3)

Recent Progress of In Situ Transmission Electron Microscopy for Energy Materials journal September 2019
Facile construction of hierarchical ellipsoid-shaped TiO 2 porous nanostructures with enhanced photocatalytic activity journal January 2019
A multi-shelled V 2 O 3 /C composite with an overall coupled carbon scaffold enabling ultrafast and stable lithium/sodium storage journal January 2019