A novel P3-type Na2/3Mg1/3Mn2/3O2 as high capacity sodium-ion cathode using reversible oxygen redox†,Journal of Materials Chemistry A

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A novel P3-type Na2/3Mg1/3Mn2/3O2 as high capacity sodium-ion cathode using reversible oxygen redox†
Journal of Materials Chemistry A ( IF 10.7 ) Pub Date : 2018-12-10 00:00:00 , DOI: 10.1039/c8ta09422e
Bohang Song _{1,

2,

3,

4} , Enyuan Hu _{4,

5,

6,

7} , Jue Liu _{1,

2,

3,

4} , Yiman Zhang _{2,

3,

4,

8} , Xiao-Qing Yang _{4,

5,

6,

7} , Jagjit Nanda _{2,

3,

4,

8} , Ashfia Huq _{1,

2,

3,

4} , Katharine Page _{1,

2,

3,

4}

Affiliation

There is great interest in the discovery of Li/Na-ion cathode materials with capacity exceeding the limitation of conventional intercalation-based oxide cathodes. One plausible but challenging path is to reversibly use the charge compensation of both lattice oxygen redox and transition metal (TM) redox. Here, we report that lattice oxygen redox alone contributes over 190 mA h g⁻¹ charge capacity (cut-off at 4.65 V vs. Na⁺/Na) for the newly synthesized P3-type Na_2/3Mg_1/3Mn(IV)_2/3O₂. Similar amounts of discharge capacity are reversibly achieved. The discharge capacity exceeds 220 mA h g⁻¹ when Mn³⁺/Mn⁴⁺ redox is partially used in addition to the oxygen redox reaction. This represents one of the highest energy density sodium-ion cathodes with superior low-cost. Our results reveal that cations with strong ionic bonding nature with oxygen (such as Mg²⁺) are very effective in inducing the reversible oxygen redox reaction. We also identified the origin of voltage hysteresis to be a P3-to-O3 phase transition in concomitance with Mg²⁺ migration, suggesting further structure design that reduces the structure transition induced cation migration is critical for increasing the energy efficiency of the oxygen redox reactions.

中文翻译：

新型P3型Na _2/3 Mg _1/3 Mn _2/3 O ₂作为可逆氧氧化还原的高容量钠离子阴极†

人们对锂/钠离子阴极材料的发现非常感兴趣，这些材料的容量超过了传统的基于嵌入的氧化物阴极的极限。一个可行但有挑战性的途径是可逆地使用晶格氧氧化还原和过渡金属（TM）氧化还原的电荷补偿。在这里，我们报道晶格氧氧化还原对新合成的P3型Na _2/3 Mg _1/3 Mn（IV的贡献超过190 mA hg ^-1（在4.65 V vs. Na ⁺ / Na时截止））_2/3 O ₂。可逆地实现了类似的放电容量。Mn时的放电容量超过220 mA hg ^-1除氧氧化还原反应外，还部分使用³⁺ / Mn⁴⁺氧化还原。这代表了具有优异低成本的最高能量密度钠离子阴极之一。我们的结果表明，与氧具有强离子键合性质的阳离子（例如Mg²⁺）在诱导可逆的氧氧化还原反应中非常有效。我们还确定了电压迟滞的起源是与Mg²⁺迁移同时发生的P3-O3相变，这表明进一步的结构设计可减少结构转变引起的阳离子迁移，这对于提高氧氧化还原反应的能效至关重要。。

更新日期：2018-12-10

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