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Bonding the Terminal Isocyanate-Related Functional Group to the Surface Manganese Ions to Enhance Li-Rich Cathode’s Cycling Stability
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2021-04-07 , DOI: 10.1021/acsami.1c01726 Chaochao Fu 1 , Linglong Meng 1 , Jinfeng Wang 1 , Qi Wang 2 , Kun Yang 1 , Wenming Zhang 3 , Liping Li 2
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2021-04-07 , DOI: 10.1021/acsami.1c01726 Chaochao Fu 1 , Linglong Meng 1 , Jinfeng Wang 1 , Qi Wang 2 , Kun Yang 1 , Wenming Zhang 3 , Liping Li 2
Affiliation
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Capacity fading of Li-rich cathodes in the cycling process is mainly caused by the irreversible side reactions at the interface of electrode and electrolyte by reason of the lack of a corrosion resistant surface. In this work, isocyanate-related functional groups (−N═C═O groups and polyamide-like groups) were tightly bonded on the surface of Li-rich oxides through a urea decomposition gas heat-treatment. The surface isocyanate functionalization inhibits the side reaction of PF5 hydrolysis to give LixPFyOz and HF species at the surface of Li-rich materials in the cycle process. As compared to the untreated Li-rich sample U0, the samples with the spinel-like layer and isocyanate functionalized surface exhibited an enhanced cycle stability. The capacity retention of the treated sample U3 reached as high as 92.6% after 100 cycles at the current density of 100 mA/g, larger than 66.8% for the untreated sample. Even at a higher current density of 1000 mA/g, sample U3 gives a capacity retention of 81.7% after 300 cycles. The findings of this work reveal the importance of surface isocyanate functionalization in restraining the surface side reactions and also suggest an effective method to design Li-rich cathode materials with better electrochemistry performance.
中文翻译：
将末端异氰酸酯相关的官能团键合到表面锰离子上，以提高富锂阴极的循环稳定性
循环过程中富锂阴极的容量衰减主要是由于缺乏耐腐蚀表面，导致电极和电解质界面发生不可逆的副反应。在这项工作中，通过尿素分解气体热处理，异氰酸酯相关的官能团（-N═C= O基团和类聚酰胺基团）紧密结合在富锂氧化物的表面上。表面异氰酸酯官能化抑制了PF 5水解的副反应，从而生成Li x PF y O z循环过程中富锂材料表面的氢和氢氟酸类物质。与未处理的富含Li的样品U0相比，具有尖晶石样层和异氰酸酯官能化表面的样品显示出增强的循环稳定性。经过100次循环后，在100 mA / g的电流密度下，处理过的样品U3的容量保持率高达92.6％，大于未处理样品的66.8％。即使在1000 mA / g的较高电流密度下，样品U3在300次循环后仍可保持81.7％的容量。这项工作的发现揭示了表面异氰酸酯官能化在抑制表面副反应中的重要性，并且还提出了一种设计具有更好的电化学性能的富锂阴极材料的有效方法。
更新日期：2021-04-21
中文翻译：
将末端异氰酸酯相关的官能团键合到表面锰离子上，以提高富锂阴极的循环稳定性
循环过程中富锂阴极的容量衰减主要是由于缺乏耐腐蚀表面，导致电极和电解质界面发生不可逆的副反应。在这项工作中，通过尿素分解气体热处理，异氰酸酯相关的官能团（-N═C= O基团和类聚酰胺基团）紧密结合在富锂氧化物的表面上。表面异氰酸酯官能化抑制了PF 5水解的副反应，从而生成Li x PF y O z循环过程中富锂材料表面的氢和氢氟酸类物质。与未处理的富含Li的样品U0相比，具有尖晶石样层和异氰酸酯官能化表面的样品显示出增强的循环稳定性。经过100次循环后，在100 mA / g的电流密度下，处理过的样品U3的容量保持率高达92.6％，大于未处理样品的66.8％。即使在1000 mA / g的较高电流密度下，样品U3在300次循环后仍可保持81.7％的容量。这项工作的发现揭示了表面异氰酸酯官能化在抑制表面副反应中的重要性，并且还提出了一种设计具有更好的电化学性能的富锂阴极材料的有效方法。
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