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Barnes, Pete; Zuo, Yunxing; Dixon, Kiev; Hou, Dewen; Lee, Sungsik; Ma, Zhiyuan; Connell, Justin G.; Zhou, Hua; Deng, Changjian; Smith, Kassiopeia; et al (, Nature Materials)
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Smith, Kassiopeia A.; Savva, Andreas I.; Mao, Keyou S.; Wang, Yongqiang; Tenne, Dmitri A.; Chen, Di; Liu, Yuzi; Barnes, Pete; Deng, Changjian; Butt, Darryl P.; et al (, Journal of Materials Science)
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Deng, Changjian; Lau, Miu Lun; Ma, Chunrong; Skinner, Paige; Liu, Yuzi; Xu, Wenqian; Zhou, Hua; Zhang, Xianghui; Wu, Di; Yin, Yadong; et al (, Journal of Materials Chemistry A)Nanoscale oxide-based negative electrodes are of great interest for lithium ion batteries due to their high energy density, power density and enhanced safety. In this work, we conducted a case study on mesoporous TiO 2 nanoparticle negative electrodes with uniform size and varying crystallinity in order to investigate the trend in the electrochemical properties of oxide-based nanoscale negative electrodes with varying crystallinity. Mesoporous solid spherical TiO 2 nanoparticles with a uniform particle size and varying crystallinity, i.e. , amorphous TiO 2 (A-TiO 2 ), partially crystalline TiO 2 (PC-TiO 2 ) and fully crystalline TiO 2 (FC-TiO 2 ) nanoparticles were studied. At low current rate (quasi steady-state), the specific capacity of the samples drops with the decrease of crystallinity. Ex situ synchrotron pair distribution function analysis reveals that the 1D zigzag Li ion diffusion pathway becomes expanded with the increase of crystallinity, which promotes ion mobility and charge storage. At high current rates (away from equilibrium states), however, the A-TiO 2 sample demonstrates slightly larger capacity than the FC-TiO 2 sample, both of which show larger capacities than that of the PC-TiO 2 sample. Both A-TiO 2 and FC-TiO 2 samples exhibit higher capacitive contribution to the charge storage and larger Li + diffusivity than those of the PC-TiO 2 sample, which explains their better rate capability. Moreover, the larger Li + diffusivity of the A-TiO 2 sample leads to the slightly larger specific capacity than the FC-TiO 2 sample at the highest current rate.more » « less
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