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    Silicon carbide-free graphene growth on silicon for lithium-ion battery with high volumetric energy density
    (London : Nature Publishing Group, 2015) Son, In Hyuk; Park, Jong Hwan; Kwon, Soonchul; Park, Seongyong; Rümmeli, Mark H.; Bachmatiuk, Alicja; Song, Hyun Jae; Ku, Junhwan; Choi, Jang Wook; Choi, Jae-man; Doo, Seok-Gwang; Chang, Hyuk
    Silicon is receiving discernable attention as an active material for next generation lithium-ion battery anodes because of its unparalleled gravimetric capacity. However, the large volume change of silicon over charge–discharge cycles weakens its competitiveness in the volumetric energy density and cycle life. Here we report direct graphene growth over silicon nanoparticles without silicon carbide formation. The graphene layers anchored onto the silicon surface accommodate the volume expansion of silicon via a sliding process between adjacent graphene layers. When paired with a commercial lithium cobalt oxide cathode, the silicon carbide-free graphene coating allows the full cell to reach volumetric energy densities of 972 and 700 Wh l−1 at first and 200th cycle, respectively, 1.8 and 1.5 times higher than those of current commercial lithium-ion batteries. This observation suggests that two-dimensional layered structure of graphene and its silicon carbide-free integration with silicon can serve as a prototype in advancing silicon anodes to commercially viable technology.
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    Hierarchical hollow Fe2O3@MIL-101(Fe)/C derived from metal-organic frameworks for superior sodium storage
    (London : Nature Publishing Group, 2016) Li, Chengping; Hu, Qian; Li, Yan; Zhou, Hang; Lv, Zhaolin; Yang, Xiangjun; Liu, Lixiang; Guo, Hong
    A facile generic template-free strategy is employed to prepare hierarchical hollow hybrid Fe2O3@MIL-101(Fe)/C materials derived from metal-organic frameworks as anode materials for Na-ion batteries. The intrinsic hollow nanostructure can shorten the lengths for both electronic and ionic transport, enlarge the surface areas of electrodes, and improve accommodation of the volume change during Na+ insertion/extraction cycling. Therefore, The stable reversible capacity of Fe2O3@MIL-101(Fe)/C electrode is 710 mAhg−1, and can be retained at 662 mAhg−1 after 200 cycles with the retention of 93.2%. Especially, its overall rate performance data confirm again the importance of the hierarchical hollow structures and multi-elements characteristics toward high capacities in both low and high current rates. This general strategy may shed light on a new avenue for fast synthesis of hierarchic hollow functional materials for energy storage, catalyst, sensor and other new applications.
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    High area capacity lithium-sulfur full-cell battery with prelitiathed silicon nanowire-carbon anodes for long cycling stability
    (London : Nature Publishing Group, 2016) Krause, Andreas; Dörfler, Susanne; Piwko, Markus; Wisser, Florian M.; Jaumann, Tony; Ahrens, Eike; Giebeler, Lars; Althues, Holger; Schädlich, Stefan; Grothe, Julia; Jeffery, Andrea; Grube, Matthias; Brückner, Jan; Martin, Jan; Eckert, Jürgen; Kaskel, Stefan; Mikolajick, Thomas; Weber, Walter M.
    We show full Li/S cells with the use of balanced and high capacity electrodes to address high power electro-mobile applications. The anode is made of an assembly comprising of silicon nanowires as active material densely and conformally grown on a 3D carbon mesh as a light-weight current collector, offering extremely high areal capacity for reversible Li storage of up to 9 mAh/cm2. The dense growth is guaranteed by a versatile Au precursor developed for homogenous Au layer deposition on 3D substrates. In contrast to metallic Li, the presented system exhibits superior characteristics as an anode in Li/S batteries such as safe operation, long cycle life and easy handling. These anodes are combined with high area density S/C composite cathodes into a Li/S full-cell with an ether- and lithium triflate-based electrolyte for high ionic conductivity. The result is a highly cyclable full-cell with an areal capacity of 2.3 mAh/cm2, a cyclability surpassing 450 cycles and capacity retention of 80% after 150 cycles (capacity loss <0.4% per cycle). A detailed physical and electrochemical investigation of the SiNW Li/S full-cell including in-operando synchrotron X-ray diffraction measurements reveals that the lower degradation is due to a lower self-reduction of polysulfides after continuous charging/discharging.