Solid-State Calcium-Ion Diffusion in Ca1.5Ba0.5Si5O3N6

被引:11
作者
Chen, Yu [1 ,2 ]
Bartel, Christopher J. [1 ,2 ]
Avdeev, Maxim [3 ,4 ]
Zhang, Ya-Qian [1 ,5 ]
Liu, Jue [6 ]
Zhong, Peichen [1 ,2 ]
Zeng, Guobo [1 ,2 ]
Cai, Zijian [1 ,2 ]
Kim, Haegyeom [2 ]
Ji, Huiwen [7 ,8 ]
Ceder, Gerbrand [1 ,2 ]
机构
[1] Univ Calif Berkeley, Dept Mat Sci & Engn, Berkeley, CA 94720 USA
[2] Lawrence Berkeley Natl Lab, Mat Sci Div, Berkeley, CA 94720 USA
[3] Australian Nucl Sci & Technol Org, Kirrawee Dc, NSW 2232, Australia
[4] Univ Sydney, Sch Chem, Sydney, NSW 2006, Australia
[5] Lawrence Berkeley Natl Lab, Mol Foundry, Berkeley, CA 94720 USA
[6] Oak Ridge Natl Lab, Neutron Scattering Div, POB 2009, Oak Ridge, TN 37831 USA
[7] Lawrence Berkeley Natl Lab, Energy Storage & Distributed Resources Div, Berkeley, CA 94720 USA
[8] Univ Utah, Dept Mat Sci & Engn, Salt Lake City, UT 84112 USA
基金
美国国家科学基金会;
关键词
TOTAL-ENERGY CALCULATIONS; CATHODE MATERIALS; 3-DIMENSIONAL VISUALIZATION; CONDUCTOR; CA; BATTERIES; MN; CO; 1ST-PRINCIPLES; INTERCALATION;
D O I
10.1021/acs.chemmater.1c02923
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Rechargeable batteries based on multivalent working ions are promising candidates for next-generation high-energy-density batteries. Development of these technologies, however, is largely limited by the low diffusion rate of multivalent ions in solid-state materials, thereby necessitating a better understanding of the design principles that control multivalent-ion mobility. Here, we report Ca1.5Ba0.5Si5O3N6 as a potential calcium solid-state conductor and investigate its Ca migration mechanism by means of ab initio computations and neutron diffraction. This compound contains partially occupied Ca sites in close proximity to each other, providing a unique mechanism for Ca migration. Nuclear density maps obtained with the maximum entropy method from neutron powder diffraction data provide strong evidence for low-energy percolating one-dimensional pathways for Ca-ion migration. Ab initio molecular dynamics simulations further support a low Ca-ion migration barrier of similar to 400 meV when Ca vacancies are present and reveal a unique "vacancy-adjacent" concerted ion migration mechanism. This work provides a new understanding of solid-state Ca-ion diffusion and insights into the future design of novel cation configurations that utilize the interactions between mobile ions to enable fast multivalent-ion conduction in solid-state materials.
引用
收藏
页码:128 / 139
页数:12
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