4.8 Article

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

期刊

ADVANCED ENERGY MATERIALS
卷 9, 期 6, 页码 -

出版社

WILEY-V C H VERLAG GMBH
DOI: 10.1002/aenm.201802816

关键词

hierarchical spheres; in situ analysis; nanoarchitecture; porous structures; radial orientation

资金

  1. National Research Foundation (NRF) - Ministry of Science, ICT and Future Planning [2018M3D1A1058624]
  2. R&D Convergence Program of the National Research Council of Science & Technology, Republic of Korea [CAP-15-02-KBSI]
  3. U.S. Department of Energy, Office of Vehicle Technologies, through the Advanced Battery Materials Research (BMR) Program [DE-SC0012704]
  4. National Science Foundation Engineering Research Center for Power Optimization of Electro Thermal Systems (POETS) [EEC-1449548]
  5. National Research Council of Science & Technology (NST), Republic of Korea [CAP-15-02-KBSI] Funding Source: Korea Institute of Science & Technology Information (KISTI), National Science & Technology Information Service (NTIS)
  6. National Research Foundation of Korea [2018M3D1A1058744] Funding Source: Korea Institute of Science & Technology Information (KISTI), National Science & Technology Information Service (NTIS)

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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 Fe3O4 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 Fe3O4/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 FexOy. The reduced capacity fade relative to other conversion systems is due to the good electrical contact between the pulverized FexOy particles and rGO, the overall structural integrity of the hpMSs, and the interconnected open porosity.

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