Cost-Effective Scalable Synthesis of Mesoporous Germanium Particles via a Redox-Transmetalation Reaction for High-Performance Energy Storage Devices
Cost-Effective Scalable Synthesis of Mesoporous Germanium Particles via a Redox-Transmetalation Reaction for High-Performance Energy Storage Devices
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DOI：
10.1021/acsnano.5b00389
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发表时间：
2015-02-01
期刊：
影响因子：
17.1
通讯作者：
Park, Soojin
中科院分区：
文献类型：
--
作者：
Choi, Sinho;Kim, Jieun;Park, Soojin
纳米结构锗是一种有前途的高性能储能器件材料。然而，以经济有效且简单的方式大规模合成它仍然是一个重大挑战。在此，我们报告了一种基于氧化还原-金属转移反应的路线，用于在 420600 摄氏度的温度下从氧化锗大规模合成介孔锗颗粒。我们可以利用温度依赖性原位 X 射线吸收精细结构分析，确认在大约 420 摄氏度下 Zn0 和 Ge4+ 之间发生独特的氧化还原-金属转移反应。该反应具有几个优点，其中包括（i）在低温（类似于 450 摄氏度）下成功合成锗颗粒，（ii）由于锗颗粒的介孔结构，可适应大的体积变化，以及（iii）由于使用廉价的金属氧化物作为起始材料，因此能够以经济有效且可扩展的方式合成颗粒。优化的介孔锗阳极在 0.5 C 倍率下循环 300 次后表现出类似于 1400 mA h g(1) 的可逆容量（相当于 99.5% 的容量保持率），并且在包含高能量密度 LiCoO2 阴极的全电池中表现出稳定的循环（充电容量 = 286.62 mA h cm(3)）。
Nanostructured germanium is a promising material for high-performance energy storage devices. However, synthesizing it in a cost-effective and simple manner on a large scale remains a significant challenge. Herein, we report a redox-transmetalation reaction-based route for the large-scale synthesis of mesoporous germanium particles from germanium oxide at temperatures of 420600 degrees C. We could confirm that a unique redox-transmetalation reaction occurs between Zn0 and Ge4+ at approximately 420 degrees C using temperature-dependent in situ X-ray absorption fine structure analysis. This reaction has several advantages, which include (i) the successful synthesis of germanium particles at a low temperature (similar to 450 degrees C), (ii) the accommodation of large volume changes, owing to the mesoporous structure of the germanium particles, and (iii) the ability to synthesize the particles in a cost-effective and scalable manner, as inexpensive metal oxides are used as the starting materials. The optimized mesoporous germanium anode exhibits a reversible capacity of similar to 1400 mA h g(1) after 300 cycles at a rate of 0.5 C (corresponding to the capacity retention of 99.5%), as well as stable cycling in a full cell containing a LiCoO2 cathode with a high energy density (charge capacity = 286.62 mA h cm(3)).