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Stabilized Co‐Free Li‐Rich Oxide Cathode Particles with An Artificial Surface Prereconstruction
Advanced Energy Materials ( IF 24.4 ) Pub Date : 2020-08-06 , DOI: 10.1002/aenm.202001120 Zhi Zhu 1 , Rui Gao 1 , Iradwikanari Waluyo 2 , Yanhao Dong 1 , Adrian Hunt 2 , Jinhyuk Lee 1 , Ju Li 1
Advanced Energy Materials ( IF 24.4 ) Pub Date : 2020-08-06 , DOI: 10.1002/aenm.202001120 Zhi Zhu 1 , Rui Gao 1 , Iradwikanari Waluyo 2 , Yanhao Dong 1 , Adrian Hunt 2 , Jinhyuk Lee 1 , Ju Li 1
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Li‐rich metal oxide (LXMO) cathodes have attracted intense interest for rechargeable batteries because of their high capacity above 250 mAh g−1. However, the side effects of hybrid anion and cation redox (HACR) reactions, such as oxygen release and phase collapse that result from global oxygen migration (GOM), have prohibited the commercialization of LXMO. GOM not only destabilizes the oxygen sublattice in cycling, aggravating the well‐known voltage fading, but also intensifies electrolyte decomposition and Mn dissolution, causing severe full‐cell performance degradation. Herein, an artificial surface prereconstruction (ASR) for Li1.2Mn0.6Ni0.2O2 particles with a molten‐molybdate leaching is conducted, which creates a crystal‐dense anion‐redox‐free LiMn1.5Ni0.5O4 shell that completely encloses the LXMO lattice (ASR‐LXMO). Differential electrochemical mass spectroscopy and soft X‐ray absorption spectroscopy analyses demonstrate that GOM is shut down in cycling, which not only stabilizes HACR in ASR‐LXMO, but also mitigates the electrolyte decomposition and Mn dissolution. ASR‐LXMO displays greatly stabilized cycling performance as it retains 237.4 mAh g−1 with an average discharge voltage of 3.30 V after 200 cycles. More crucially, while the pristine LXMO cycling cannot survive 90 cycles in a pouch full‐cell matched with a commercial graphite anode and lean (2 g A−1 h−1) electrolyte, ASR‐LXMO shows high capacity retention of 76% after 125 cycles in full‐cell cycling.
中文翻译：
具有人造表面预重构的稳定的无钴氧化锂正极颗粒
富锂金属氧化物（LXMO）阴极因其在250 mAh g -1以上的高容量而引起了可再充电电池的强烈兴趣。但是，混合阴离子和阳离子氧化还原（HACR）反应的副作用，例如由于整体氧气迁移（GOM）导致的氧气释放和相塌陷，已禁止了LXMO的商业化。GOM不仅使循环中的氧亚晶格不稳定，加剧了众所周知的电压衰减，还加剧了电解质的分解和Mn的溶解，从而导致严重的全电池性能下降。本文中，对Li 1.2 Mn 0.6 Ni 0.2 O 2进行了人工表面预处理（ASR）进行了具有熔融钼酸盐浸出的颗粒，从而形成了无晶体致密的阴离子-氧化还原-的LiMn 1.5 Ni 0.5 O 4壳，该壳完全包围了LXMO晶格（ASR-LXMO）。差示电化学质谱和软X射线吸收光谱分析表明，GOM在循环中关闭，这不仅稳定了ASR-LXMO中的HACR，而且减轻了电解质的分解和Mn的溶解。ASR-LXMO表现出极大的稳定的循环性能，在200个循环后，它保持237.4 mAh g -1的平均放电电压为3.30V 。更重要的是，原始LXMO循环在装有商用石墨阳极和稀薄（2 g A-1 h -1）电解质，ASR-LXMO在全电池循环中经过125个循环后显示出76％的高容量保持率。
更新日期：2020-09-15
中文翻译：
具有人造表面预重构的稳定的无钴氧化锂正极颗粒
富锂金属氧化物（LXMO）阴极因其在250 mAh g -1以上的高容量而引起了可再充电电池的强烈兴趣。但是，混合阴离子和阳离子氧化还原（HACR）反应的副作用，例如由于整体氧气迁移（GOM）导致的氧气释放和相塌陷，已禁止了LXMO的商业化。GOM不仅使循环中的氧亚晶格不稳定，加剧了众所周知的电压衰减，还加剧了电解质的分解和Mn的溶解，从而导致严重的全电池性能下降。本文中，对Li 1.2 Mn 0.6 Ni 0.2 O 2进行了人工表面预处理（ASR）进行了具有熔融钼酸盐浸出的颗粒，从而形成了无晶体致密的阴离子-氧化还原-的LiMn 1.5 Ni 0.5 O 4壳，该壳完全包围了LXMO晶格（ASR-LXMO）。差示电化学质谱和软X射线吸收光谱分析表明，GOM在循环中关闭，这不仅稳定了ASR-LXMO中的HACR，而且减轻了电解质的分解和Mn的溶解。ASR-LXMO表现出极大的稳定的循环性能，在200个循环后，它保持237.4 mAh g -1的平均放电电压为3.30V 。更重要的是，原始LXMO循环在装有商用石墨阳极和稀薄（2 g A-1 h -1）电解质，ASR-LXMO在全电池循环中经过125个循环后显示出76％的高容量保持率。
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