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Unveiling the Structural and Dynamic Characteristics of Concentrated LiNO3 Aqueous Solutions through Ultrafast Infrared Spectroscopy and Molecular Dynamics Simulations
The Journal of Physical Chemistry Letters ( IF 4.8 ) Pub Date : 2024-07-19 , DOI: 10.1021/acs.jpclett.4c01449 Miaomiao Zhang 1 , Jiahui Peng 1 , Yuting Gao 1 , Baihui Wang 1 , Jiman He 1 , Yimin Bai 1 , Jing Liu 1 , Cheng-Lung Chen 2 , Yu Fang 1 , Hongtao Bian 1
The Journal of Physical Chemistry Letters ( IF 4.8 ) Pub Date : 2024-07-19 , DOI: 10.1021/acs.jpclett.4c01449 Miaomiao Zhang 1 , Jiahui Peng 1 , Yuting Gao 1 , Baihui Wang 1 , Jiman He 1 , Yimin Bai 1 , Jing Liu 1 , Cheng-Lung Chen 2 , Yu Fang 1 , Hongtao Bian 1
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Highly concentrated aqueous electrolytes have attracted a significant amount of attention for their potential applications in lithium-ion batteries. Nevertheless, a comprehensive understanding of the Li+ solvation structure and its migration within electrolyte solutions remains elusive. This study employs linear vibrational spectroscopy, ultrafast infrared spectroscopy, and molecular dynamics (MD) simulations to elucidate the structural dynamics in LiNO3 solutions by using intrinsic and extrinsic vibrational probes. The N–O stretching vibrations of NO3– exhibit a distinct spectral splitting, attributed to its asymmetric interaction with the surrounding solvation structure. Analysis of the vibrational relaxation dynamics of intrinsic and extrinsic probes, in combination with MD simulations, reveals cage-like networks formed through electrostatic interactions between Li+ and NO3–. This microscopic heterogeneity is reflected in the intertwined arrangement of ions and water molecules. Furthermore, both vehicular transport and structural diffusion assisted by solvent rearrangement for Li+ were analyzed, which are closely linked with the bulk concentration.
中文翻译：
通过超快红外光谱和分子动力学模拟揭示浓 LiNO3 水溶液的结构和动态特性
高浓度水性电解质因其在锂离子电池中的潜在应用而引起了广泛关注。然而，对Li +溶剂化结构及其在电解质溶液中迁移的全面了解仍然难以实现。本研究采用线性振动光谱、超快红外光谱和分子动力学 (MD) 模拟，通过使用内在和外在振动探针来阐明 LiNO 3溶液中的结构动力学。 NO 3的 N-O 伸缩振动表现出明显的光谱分裂，这归因于其与周围溶剂化结构的不对称相互作用。对内在和外在探针的振动弛豫动力学的分析，结合MD模拟，揭示了通过Li +和NO 3 -之间的静电相互作用形成的笼状网络。这种微观异质性反映在离子和水分子的交织排列中。此外，还分析了Li +溶剂重排辅助下的车辆传输和结构扩散，这与体积浓度密切相关。
更新日期：2024-07-19
中文翻译：
通过超快红外光谱和分子动力学模拟揭示浓 LiNO3 水溶液的结构和动态特性
高浓度水性电解质因其在锂离子电池中的潜在应用而引起了广泛关注。然而，对Li +溶剂化结构及其在电解质溶液中迁移的全面了解仍然难以实现。本研究采用线性振动光谱、超快红外光谱和分子动力学 (MD) 模拟，通过使用内在和外在振动探针来阐明 LiNO 3溶液中的结构动力学。 NO 3的 N-O 伸缩振动表现出明显的光谱分裂，这归因于其与周围溶剂化结构的不对称相互作用。对内在和外在探针的振动弛豫动力学的分析，结合MD模拟，揭示了通过Li +和NO 3 -之间的静电相互作用形成的笼状网络。这种微观异质性反映在离子和水分子的交织排列中。此外，还分析了Li +溶剂重排辅助下的车辆传输和结构扩散，这与体积浓度密切相关。
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