2D Ni0.25Mn0.75O2: A high-performance cathode for multivalent ion batteries
2D Ni0.25Mn0.75O2: A high-performance cathode for multivalent ion batteries
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DOI：
10.1016/j.commatsci.2021.110948
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发表时间：
2022
影响因子：
3.3
通讯作者：
Diana Liepinya;R. Shepard;Manuel Smeu
中科院分区：
文献类型：
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作者：
Diana Liepinya;R. Shepard;Manuel Smeu
尽管锂离子电池在近几十年来推动了便携式能源存储，但人们越来越关注其安全性，成本和成分的丰富性。多价离子电池（MVIB）具有解决这些问题的潜力，但它们受到目前已知的MVIB阴极的限制，其不能提供一致有利的电压、能量密度和扩散动力学。我们使用密度泛函理论（DFT）来模拟Li，Na，Mg，Ca和Al离子与2D Ni0.25Mn0.75O2配对时的性能，2D Ni0.25Mn0.75O2是一种新型阴极，其使用增加的层分离来改善其3D模拟物的动力学。我们的计算得到的最大电压为3.38 V的Na和2.7 V的Ca，优于2D NaxMnO 2和NaxNiO 2。Li、Na和Ca的扩散势垒低于300 meV，与现有电池技术和终点2D阴极相当;同时，Mg和Al具有过高的扩散势垒，这意味着它们与该阴极不相容。最后，态密度计算和Bader电荷分析表明，阴极变得导电后，离子吸附，这是必要的高倍率性能。2D Ni0.25Mn0.75O2保持了其他2D过渡金属氧化物的性能，同时增加了阴极电导率，这表明它是Li，Na和Ca离子实验研究的有希望的候选者。
Although Li-ion batteries have driven portable energy storage in recent decades, there is increasing concern about their safety, cost, and abundance of constituents. Multivalent ion batteries (MVIBs) have the potential to remedy these issues, but they are limited by the currently known MVIB cathodes, which fail to deliver unanimously favorable voltage, energy density, and diffusion kinetics. We used density functional theory (DFT) to model the performance of Li, Na, Mg, Ca, and Al ions when paired with 2D Ni0.25Mn0.75O2, a novel cathode that uses increased layer separation to improve on the kinetics of its 3D analog. Our calculations yielded maximum voltages of 3.38 V for Na and 2.7 V for Ca, outperforming 2D NaxMnO2and NaxNiO2. Diffusion barriers for Li, Na, and Ca are below 300 meV, comparable to existing battery technology and the endpoint 2D cathodes; meanwhile, Mg and Al have prohibitively high diffusion barriers, implying their incompatibility with this cathode. Lastly, density of states calculations and Bader charge analysis show that the cathode becomes conducting following ion adsorption, which is necessary for high-rate performance. 2D Ni0.25Mn0.75O2maintains performance seen with other 2D transition metal oxides while increasing cathode conductivity, indicating that it is a promising candidate for experimental investigation with Li, Na, and Ca ions.