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Completely suppressed high-voltage phase transition of P2/O3-Na0.7Li0.1Ni0.1Fe0.2Mn0.6O2 via Li/Ni co-doping for sodium storage
Inorganic Chemistry Frontiers ( IF 6.1 ) Pub Date : 2022-08-18 , DOI: 10.1039/d2qi01018f Yunpeng Wang 1 , Mengmeng Yan 2 , Kang Xu 2 , Yu-Xin Chang 2, 3 , Jin Guo 1 , Qinghua Wang 4 , Bin Wang 5 , Duan Wang 1 , Ya-Xia Yin 3 , Sailong Xu 2
Inorganic Chemistry Frontiers ( IF 6.1 ) Pub Date : 2022-08-18 , DOI: 10.1039/d2qi01018f Yunpeng Wang 1 , Mengmeng Yan 2 , Kang Xu 2 , Yu-Xin Chang 2, 3 , Jin Guo 1 , Qinghua Wang 4 , Bin Wang 5 , Duan Wang 1 , Ya-Xia Yin 3 , Sailong Xu 2
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P2-type Fe, Mn-based layered oxides have been potential cathode materials for sodium-ion batteries (SIBs), yet suffer from their intrinsic sluggish kinetics and structural instability due to the adverse P2–Z high-voltage phase transition. An improvement strategy by either single-cation doping or co-doping is used, but typically with either a lowered reversible capacity or partially suppressed high-voltage phase transition. In this study, a novel biphasic P2/O3-Na0.7Li0.1Ni0.1Fe0.2Mn0.6O2 cathode was prepared, with the high-voltage phase transition completely suppressed via Li/Ni co-doping. Inactive Li+ stabilizes the structure and active Ni2+ improves the electrical conductivity, while the P2/O3 intergrown structure induced by co-doping further limits the lattice stress during cycling. The resulting cathode exhibits an outstanding rate capability (102.2 mA h g−1 at 0.1C and 59.8 mA h g−1 at 10C), and an excellent cyclic stability (74.6% capacity retention after 500 cycles at 10C). The reaction kinetics and structural evolution demonstrate high Na+ diffusion coefficient and the complete suppression of the Z phase transition, respectively, both of which underpin the enhancement. The results highlight that the synergistic effect between Li/Ni co-doping and accompanying biphasic structure promises an effective improvement strategy to develop high-performance Fe, Mn-based and Co-free layered cathode materials for SIBs.
中文翻译：
通过 Li/Ni 共掺杂完全抑制 P2/O3-Na0.7Li0.1Ni0.1Fe0.2Mn0.6O2 的高压相变用于钠存储
P2 型 Fe、Mn 基层状氧化物一直是钠离子电池 (SIB) 的潜在正极材料，但由于不利的 P2-Z 高压相变，其固有的动力学迟缓和结构不稳定。使用单阳离子掺杂或共掺杂的改进策略，但通常具有降低的可逆容量或部分抑制高压相变。在这项研究中，制备了一种新型双相 P2/O3-Na 0.7 Li 0.1 Ni 0.1 Fe 0.2 Mn 0.6 O 2正极，通过Li/Ni 共掺杂完全抑制了高压相变。不活跃的李+稳定结构和活性Ni 2+提高了导电性，而由共掺杂引起的P2/O3共生结构进一步限制了循环过程中的晶格应力。所得正极表现出出色的倍率性能（0.1C 时为 102.2 mA hg -1和 10C 时为 59.8 mA hg -1）和优异的循环稳定性（在 10C 下 500 次循环后容量保持率为 74.6%）。反应动力学和结构演化显示出高 Na +扩散系数和 Z 相变的完全抑制分别是增强的基础。结果表明，Li/Ni 共掺杂和伴随的双相结构之间的协同效应为开发用于 SIB 的高性能 Fe、Mn 基和无 Co 层状正极材料提供了一种有效的改进策略。
更新日期：2022-08-18
中文翻译：
通过 Li/Ni 共掺杂完全抑制 P2/O3-Na0.7Li0.1Ni0.1Fe0.2Mn0.6O2 的高压相变用于钠存储
P2 型 Fe、Mn 基层状氧化物一直是钠离子电池 (SIB) 的潜在正极材料，但由于不利的 P2-Z 高压相变，其固有的动力学迟缓和结构不稳定。使用单阳离子掺杂或共掺杂的改进策略，但通常具有降低的可逆容量或部分抑制高压相变。在这项研究中，制备了一种新型双相 P2/O3-Na 0.7 Li 0.1 Ni 0.1 Fe 0.2 Mn 0.6 O 2正极，通过Li/Ni 共掺杂完全抑制了高压相变。不活跃的李+稳定结构和活性Ni 2+提高了导电性，而由共掺杂引起的P2/O3共生结构进一步限制了循环过程中的晶格应力。所得正极表现出出色的倍率性能（0.1C 时为 102.2 mA hg -1和 10C 时为 59.8 mA hg -1）和优异的循环稳定性（在 10C 下 500 次循环后容量保持率为 74.6%）。反应动力学和结构演化显示出高 Na +扩散系数和 Z 相变的完全抑制分别是增强的基础。结果表明，Li/Ni 共掺杂和伴随的双相结构之间的协同效应为开发用于 SIB 的高性能 Fe、Mn 基和无 Co 层状正极材料提供了一种有效的改进策略。
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