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Conformal PEDOT Coating Enables Ultra-High-Voltage and High-Temperature Operation for Single-Crystal Ni-Rich Cathodes
ACS Nano ( IF 15.8 ) Pub Date : 2022-09-13 , DOI: 10.1021/acsnano.2c04959 Qiang Liu 1, 2 , Yu-Tong Liu 1 , Chen Zhao 2 , Qing-Song Weng 1, 3 , Junjing Deng 4 , Inhui Hwang 4 , Yi Jiang 4 , Chengjun Sun 4 , Tianyi Li 4 , Wenqian Xu 4 , Ke Du 5 , Amine Daali 2 , Gui-Liang Xu 2 , Khalil Amine 2, 6, 7 , Guohua Chen 1
ACS Nano ( IF 15.8 ) Pub Date : 2022-09-13 , DOI: 10.1021/acsnano.2c04959 Qiang Liu 1, 2 , Yu-Tong Liu 1 , Chen Zhao 2 , Qing-Song Weng 1, 3 , Junjing Deng 4 , Inhui Hwang 4 , Yi Jiang 4 , Chengjun Sun 4 , Tianyi Li 4 , Wenqian Xu 4 , Ke Du 5 , Amine Daali 2 , Gui-Liang Xu 2 , Khalil Amine 2, 6, 7 , Guohua Chen 1
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Single-crystal Ni-rich Li[NixMnyCo1–x–y]O2 (SC-NMC) cathodes represent a promising approach to mitigate the cracking issue of conventional polycrystalline cathodes. However, many reported SC-NMC cathodes still suffer from unsatisfactory cycling stability, particularly under high charge cutoff voltage and/or elevated temperature. Herein, we report an ultraconformal and durable poly(3,4-ethylenedioxythiophene) (PEDOT) coating for SC-NMC cathodes using an oxidative chemical vapor deposition (oCVD) technique, which significantly improves their high-voltage (4.6 V) and high-temperature operation resiliency. The PEDOT coated SC LiNi0.83Mn0.1Co0.07O2 (SC-NMC83) delivers an impressive capacity retention rate of 96.7% and 89.5% after 100 and 200 cycles, respectively. Significantly, even after calendar aging at 45 °C and 4.6 V, the coated cathode can still retain 85.3% (in comparison with 59.6% for the bare one) of the initial capacity after 100 cycles at a 0.5 C rate. Synchrotron X-ray experiments and interface characterization collectively reveal that the conformal PEDOT coating not only effectively stabilizes the crystallographic structure and maintains the integrity of the particles but also significantly suppresses the electrolyte’s corrosion, resulting in improved electrochemical/thermal stability. Our findings highlight the promise of an oCVD PEDOT coating for single-crystal Ni-rich cathodes to meet the grand challenge of high-energy batteries under extreme conditions.
中文翻译：
保形 PEDOT 涂层可实现单晶富镍阴极的超高压和高温操作
单晶富镍 Li[Ni x Mn y Co 1–x– y ]O 2 (SC-NMC) 正极代表了一种有希望的方法来缓解传统多晶正极的开裂问题。然而，许多报道的 SC-NMC 正极仍然存在不令人满意的循环稳定性，特别是在高充电截止电压和/或高温下。在此，我们报告了一种用于 SC-NMC 阴极的超保形耐用聚 (3,4-乙烯二氧噻吩) (PEDOT) 涂层，该涂层采用氧化化学气相沉积 (oCVD) 技术，显着提高了其高电压 (4.6 V) 和高电压。温度操作弹性。PEDOT 涂层 SC LiNi 0.83 Mn 0.1 Co 0.07 O2(SC-NMC83) 在 100 次和 200 次循环后分别提供了 96.7% 和 89.5% 的令人印象深刻的容量保持率。值得注意的是，即使在 45 °C 和 4.6 V 的日历老化后，涂层正极在 0.5 C 速率下循环 100 次后仍可保持 85.3%（与裸正极相比为 59.6%）的初始容量。同步加速器 X 射线实验和界面表征共同表明，保形 PEDOT 涂层不仅有效地稳定了晶体结构并保持了颗粒的完整性，而且显着抑制了电解质的腐蚀，从而提高了电化学/热稳定性。我们的研究结果强调了用于单晶富镍阴极的 oCVD PEDOT 涂层有望在极端条件下应对高能电池的巨大挑战。
更新日期：2022-09-13
中文翻译：
保形 PEDOT 涂层可实现单晶富镍阴极的超高压和高温操作
单晶富镍 Li[Ni x Mn y Co 1–x– y ]O 2 (SC-NMC) 正极代表了一种有希望的方法来缓解传统多晶正极的开裂问题。然而，许多报道的 SC-NMC 正极仍然存在不令人满意的循环稳定性，特别是在高充电截止电压和/或高温下。在此，我们报告了一种用于 SC-NMC 阴极的超保形耐用聚 (3,4-乙烯二氧噻吩) (PEDOT) 涂层，该涂层采用氧化化学气相沉积 (oCVD) 技术，显着提高了其高电压 (4.6 V) 和高电压。温度操作弹性。PEDOT 涂层 SC LiNi 0.83 Mn 0.1 Co 0.07 O2(SC-NMC83) 在 100 次和 200 次循环后分别提供了 96.7% 和 89.5% 的令人印象深刻的容量保持率。值得注意的是，即使在 45 °C 和 4.6 V 的日历老化后，涂层正极在 0.5 C 速率下循环 100 次后仍可保持 85.3%（与裸正极相比为 59.6%）的初始容量。同步加速器 X 射线实验和界面表征共同表明，保形 PEDOT 涂层不仅有效地稳定了晶体结构并保持了颗粒的完整性，而且显着抑制了电解质的腐蚀，从而提高了电化学/热稳定性。我们的研究结果强调了用于单晶富镍阴极的 oCVD PEDOT 涂层有望在极端条件下应对高能电池的巨大挑战。
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