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Modulation of Si–O Structure in Uniformly Ultrasmall Silicon Oxycarbide for Superior Lifespan of Lithium Metal Anodes
ACS Nano ( IF 15.8 ) Pub Date : 2023-11-17 , DOI: 10.1021/acsnano.3c08561 Zhijie Jiang 1 , Ang Li 1 , Zipeng Jiang 1 , Jiapeng Zhang 1 , Mohammad Tabish 1 , Xiaohong Chen 1 , Huaihe Song 1
ACS Nano ( IF 15.8 ) Pub Date : 2023-11-17 , DOI: 10.1021/acsnano.3c08561 Zhijie Jiang 1 , Ang Li 1 , Zipeng Jiang 1 , Jiapeng Zhang 1 , Mohammad Tabish 1 , Xiaohong Chen 1 , Huaihe Song 1
Affiliation
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Utilizing nanoseeds guiding homogeneous deposition of lithium is an effective strategy to inhibit disorderly growth of lithium, where silicon oxide has been attracting attention as a transform seed. However, the research on silicon-oxide-based seeds has concentrated more on utilizing their lithiophilicity but less on their Si–O structures, which could result in different failure mechanisms. In this study, various Si–O structures of silicon oxycarbide carbon nanofibers are prepared by adjusting the content of octa(aminopropylsilsesquioxane). According to XANES and experimental observations, the C-rich SiOC has an active Si–O–C structure but generates a larger volume variation during lithiation, while in the O-rich phase, the silica–oxygen tetrahedral structure can contribute to alleviate the volume expansion but has poor electrochemical activity. SiOC, which is dominated by SiO3C, has a suitable Si–O and silica–oxygen tetrahedral-structure distribution, which balances the electrochemical activity and volume expansion. This allows the host to demonstrate an excellent lifespan over 3740 h with a tiny voltage hysteresis (22 mV) at 2 mA cm–2, and it retains a favorable capacity of 97 mA h g–1 after 630 cycles with a high Coulombic efficiency of 99.7% in full cells. This study experiences the influence of various Si–O structures on lithium metal anodes.
中文翻译：
均匀超小型碳氧化硅中 Si-O 结构的调制可提高锂金属阳极的使用寿命
利用纳米种子引导锂的均匀沉积是抑制锂无序生长的有效策略，其中氧化硅作为转化种子已引起人们的关注。然而，对氧化硅基晶种的研究更多地集中在利用其亲锂性，而较少关注其 Si-O 结构，这可能导致不同的失效机制。本研究通过调节八氨基丙基倍半硅氧烷的含量制备了各种Si-O结构的碳氧化硅碳纳米纤维。根据XANES和实验观察，富C的SiOC具有活跃的Si-O-C结构，但在锂化过程中产生较大的体积变化，而在富O相中，硅氧四面体结构有助于减轻体积变化。膨胀，但电化学活性较差。 SiOC以SiO 3 C为主，具有合适的Si-O和硅-氧四面体结构分布，平衡了电化学活性和体积膨胀。这使得主机能够表现出超过 3740 小时的优异寿命，在 2 mA cm –2下具有微小的电压迟滞 (22 mV)，并且在 630 个循环后保持 97 mA hg –1的良好容量，库仑效率高达 99.7占完整细胞的百分比。本研究体验了各种 Si-O 结构对锂金属负极的影响。
更新日期：2023-11-17
中文翻译：
均匀超小型碳氧化硅中 Si-O 结构的调制可提高锂金属阳极的使用寿命
利用纳米种子引导锂的均匀沉积是抑制锂无序生长的有效策略，其中氧化硅作为转化种子已引起人们的关注。然而，对氧化硅基晶种的研究更多地集中在利用其亲锂性，而较少关注其 Si-O 结构，这可能导致不同的失效机制。本研究通过调节八氨基丙基倍半硅氧烷的含量制备了各种Si-O结构的碳氧化硅碳纳米纤维。根据XANES和实验观察，富C的SiOC具有活跃的Si-O-C结构，但在锂化过程中产生较大的体积变化，而在富O相中，硅氧四面体结构有助于减轻体积变化。膨胀，但电化学活性较差。 SiOC以SiO 3 C为主，具有合适的Si-O和硅-氧四面体结构分布，平衡了电化学活性和体积膨胀。这使得主机能够表现出超过 3740 小时的优异寿命，在 2 mA cm –2下具有微小的电压迟滞 (22 mV)，并且在 630 个循环后保持 97 mA hg –1的良好容量，库仑效率高达 99.7占完整细胞的百分比。本研究体验了各种 Si-O 结构对锂金属负极的影响。
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