Exploiting anion and cation redox chemistry in lithium-rich perovskite oxalate: a novel next-generation Li/Na-ion battery electrode
Exploiting anion and cation redox chemistry in lithium-rich perovskite oxalate: a novel next-generation Li/Na-ion battery electrode
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DOI：
10.1039/d2dt01447e
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发表时间：
2022-07-25
影响因子：
4
通讯作者：
Armstrong, A. Robert
中科院分区：
文献类型：
--
作者：
Pramanik, Atin;Manche, Alexis G.;Armstrong, A. Robert
对锂/钠离子电池（LIBs & NIBs）电化学反应动力学的基本理解是推进新一代电极材料的重要标准。在此，我们展示了一种新型富锂钙钛矿草酸盐KLi3Fe(C2O4)(3) （KLFC）阴极，具有阳离子和阴离子氧化还原的组合，在LIB和NIB中分别提供了100次循环后的86和99 mA h g（-1）的放电容量，具有良好的可循环性。实验拉曼光谱分析结合DFT计算的充电/放电样品说明草酸阴离子氧化还原活性。此外，态偏密度的第一性原理计算和Bader电荷分析也表征了钾提取过程中的氧化还原行为和电荷转移。
The fundamental understanding of electrochemical reaction kinetics for lithium/sodium-ion batteries (LIBs & NIBs) is a significant criterion for advancing new-generation electrode materials. Herein, we demonstrate a novel lithium-rich perovskite oxalate KLi3Fe(C2O4)(3) (KLFC) cathode with the combination of cation and anion redox delivering discharge capacities of 86 and 99 mA h g(-1) after 100 cycles for a LIB and NIB, respectively, with good cyclability. Experimental Raman spectroscopy analysis combined with DFT calculations of charged/discharged samples illustrate the oxalate anion redox activity. Further, first-principles calculations of the partial density of states and Bader charges analysis have also characterised the redox behaviour and charge transfer during the potassium extraction processes.