Off-stoichiometric design of a manganese-rich mixed olivine Li-ion cathode for improved specific energy

IF 9 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Materials Today Energy Pub Date : 2024-08-09 DOI:10.1016/j.mtener.2024.101658
Angel Burgos, Junteng Du, Danna Yan, Yazhou Zhou, Hannah Levy, Jeong Gi Ryu, Jae Chul Kim
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Abstract

Lithium phospho-olivine cathodes operating with iron (Fe) and manganese (Mn) redox centers are considered technologically important materials that can make the development of Li-ion batteries sustainable. Although large Mn content is desirable to achieve high specific energy at a material level, the mixed olivine cathodes require particle nanostructuring and post-synthesis treatment to demonstrate reasonable energy storage properties at an electrode level. In this work, we have investigated the effect of off-stoichiometry on the electrochemical properties of a Mn-rich mixed olivine cathode material that does not require complex optimization processing. An off-stoichiometric form of LiFeMnPO is synthesized with nominal composition of LiFeMnPO. X-ray diffraction and electron microscopy indicate that off-stoichiometry leads to phase separation into stoichiometric LiFeMnPO crystalline particles with non-crystalline surface phases. The off-stoichiometric cathode has an improved specific energy of 622 Wh/kg at C/5, outperforming the stoichiometric cathode. The off-stoichiometric cathode also exhibits improved rate capability, delivering 120 mAh/g at 20C and 78 mAh/g at 40C discharge, respectively, due to reduced interfacial and charge transfer resistances. This work highlights off-stoichiometry as an effective approach to engineer Mn-rich mixed olivine cathode materials with desirable electrochemical properties, providing a practically feasible route for materials optimization.
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改进比能量的富锰混合橄榄石锂离子阴极的非化学计量设计
具有铁(Fe)和锰(Mn)氧化还原中心的磷橄榄石锂阴极被认为是具有重要技术意义的材料,可以使锂离子电池的发展具有可持续性。虽然大锰含量是在材料层面实现高比能量的理想选择,但混合橄榄石阴极需要进行颗粒纳米结构化和合成后处理,才能在电极层面展示出合理的储能特性。在这项工作中,我们研究了非化学计量对无需复杂优化处理的富锰混合橄榄石阴极材料电化学性能的影响。在标称成分为 LiFeMnPO 的情况下,合成了一种非化学计量形式的 LiFeMnPO。X 射线衍射和电子显微镜显示,非计量导致相分离成具有非晶表面相的计量锰酸锂晶体颗粒。非计量阴极在 C/5 时的比能量提高到 622 Wh/kg,优于计量阴极。由于降低了界面电阻和电荷转移电阻,非化学计量阴极还显示出更高的速率能力,在 20C 和 40C 放电时分别可提供 120 mAh/g 和 78 mAh/g。这项工作突出表明,非化学计量是设计具有理想电化学特性的富锰混合橄榄石阴极材料的一种有效方法,为材料优化提供了一条切实可行的途径。
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来源期刊
Materials Today Energy
Materials Today Energy Materials Science-Materials Science (miscellaneous)
CiteScore
15.10
自引率
7.50%
发文量
291
审稿时长
15 days
期刊介绍: Materials Today Energy is a multi-disciplinary, rapid-publication journal focused on all aspects of materials for energy. Materials Today Energy provides a forum for the discussion of high quality research that is helping define the inclusive, growing field of energy materials. Part of the Materials Today family, Materials Today Energy offers authors rigorous peer review, rapid decisions, and high visibility. The editors welcome comprehensive articles, short communications and reviews on both theoretical and experimental work in relation to energy harvesting, conversion, storage and distribution, on topics including but not limited to: -Solar energy conversion -Hydrogen generation -Photocatalysis -Thermoelectric materials and devices -Materials for nuclear energy applications -Materials for Energy Storage -Environment protection -Sustainable and green materials
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