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Formation of LiF Surface Layer During Direct Fluorination of High-Capacity Co-Free Disordered Rocksalt Cathodes
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2021-08-04 , DOI: 10.1021/acsami.1c07882 Yiman Zhang 1 , Ethan C Self 1 , Bishnu P Thapaliya 2 , Raynald Giovine 3 , Harry M Meyer 1 , Linze Li 4 , Yuan Yue 5 , Dongchang Chen 5 , Wei Tong 5 , Guoying Chen 5 , Chongmin Wang 5 , Raphaële Clément 3 , Sheng Dai 1, 2 , Jagjit Nanda 1
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2021-08-04 , DOI: 10.1021/acsami.1c07882 Yiman Zhang 1 , Ethan C Self 1 , Bishnu P Thapaliya 2 , Raynald Giovine 3 , Harry M Meyer 1 , Linze Li 4 , Yuan Yue 5 , Dongchang Chen 5 , Wei Tong 5 , Guoying Chen 5 , Chongmin Wang 5 , Raphaële Clément 3 , Sheng Dai 1, 2 , Jagjit Nanda 1
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Disordered rocksalt (DRX) cathodes have attracted interest due to their high capacity and compositional flexibility (e.g., Co-free chemistries). However, the sloping voltage profile and gradual capacity fade during cycling have hindered the widespread adoption of these materials. Simulations predict that fluorine substitution in DRX cathodes will improve their capacity, rate performance, and cyclability. In this study, we use a fluidized bed reactor to fluorinate a model Li-rich DRX composition (Li1.15Ni0.375Ti0.375Mo0.1O2, NTMO) to investigate how fluorine content impacts the cathode’s structure and electrochemical performance. Instead of substituting O with F to form oxyfluoride phases, direct fluorination of DRX cathodes leads to the formation of LiF surface films, which improves the specific energy and capacity retention. This study demonstrates the feasibility of direct fluorination to improve the electrochemical performance of high-voltage cathodes by tuning the material’s surface chemistry.
中文翻译：
高容量无钴无序岩盐阴极直接氟化过程中 LiF 表面层的形成
无序岩盐 (DRX) 阴极由于其高容量和组成灵活性（例如，无 Co 化学）而引起了人们的兴趣。然而，在循环过程中倾斜的电压曲线和逐渐的容量衰减阻碍了这些材料的广泛采用。模拟预测，DRX 正极中的氟取代将提高其容量、倍率性能和循环性能。在本研究中，我们使用流化床反应器对模型富锂 DRX 组合物 (Li 1.15 Ni 0.375 Ti 0.375 Mo 0.1 O 2, NTMO) 来研究氟含量如何影响阴极的结构和电化学性能。DRX 正极的直接氟化不是用 F 取代 O 形成氟氧化物相，而是导致形成 LiF 表面膜，从而提高了比能量和容量保持率。这项研究证明了直接氟化通过调整材料的表面化学来改善高压阴极电化学性能的可行性。
更新日期：2021-08-19
中文翻译：
高容量无钴无序岩盐阴极直接氟化过程中 LiF 表面层的形成
无序岩盐 (DRX) 阴极由于其高容量和组成灵活性（例如，无 Co 化学）而引起了人们的兴趣。然而，在循环过程中倾斜的电压曲线和逐渐的容量衰减阻碍了这些材料的广泛采用。模拟预测，DRX 正极中的氟取代将提高其容量、倍率性能和循环性能。在本研究中，我们使用流化床反应器对模型富锂 DRX 组合物 (Li 1.15 Ni 0.375 Ti 0.375 Mo 0.1 O 2, NTMO) 来研究氟含量如何影响阴极的结构和电化学性能。DRX 正极的直接氟化不是用 F 取代 O 形成氟氧化物相，而是导致形成 LiF 表面膜，从而提高了比能量和容量保持率。这项研究证明了直接氟化通过调整材料的表面化学来改善高压阴极电化学性能的可行性。
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