Enabling Sulfur-Based Beyond-Lithium Metal Batteries via a Mechanistic Understanding of Advanced Hybrid Cathodes and Borate Electrolytes

使用化石燃料发电和运输是导致气候变化的人类二氧化碳排放的主要来源。利用电池来储存可再生能源，如太阳能和风能，对于减少对不可再生资源的依赖至关重要。然而，目前用于手持设备和电动汽车的锂离子电池使用昂贵且稀有的材料，这些材料不是国内生产的，这限制了负担能力和国内供应链安全。开发低成本、可持续和国产材料（如钠、镁或钙）的电池可以克服这些挑战，但需要新的化学物质来提高基于这些材料的电池的性能。这项研究旨在引领基于这些元素的下一代电池化学物质的开发，以支持低成本电池解决方案的国内生产，从而提高美国在可再生能源领域的竞争力和独立性。此外，这一努力促进了包容性，并促进了该领域未来科学家和工程师的成长。目前，由于阴极容量低和电解质稳定性差，超越锂离子电池受到限制。这使得它们在高能量密度应用中的竞争力降低。该项目的目的是通过研究这些电池的可逆电解质和高容量阴极，创造出能够在市场上竞争的负担得起的高性能锂离子电池。实现这一宏伟目标的策略是利用计算和实验相结合的方法：1）研究一组高能量密度混合阴极，其中硫与催化基底材料化学结合，2）发现基于可调硼酸盐化学的先进电解质，以及3）将基于新型阴极和电解质的各种反应机制映射到它们的宏观性能，这将为合理发现上级Na、Mg和Ca阳极化学提供信息。这一机制图将通过计算预测上级混合阴极和硼酸盐电解质，表征其性能，并修改机制的理解迭代应用和完善。该奖项反映了NSF的法定使命，并已被认为是值得通过使用基金会的智力价值和更广泛的影响审查标准进行评估的支持。

Using fossil fuels to generate electricity and power transportation is the primary source of anthropogenic carbon dioxide emissions that lead to climate change. The utilization of batteries to store renewable energy, such as solar and wind, is critical to lessen dependence on nonrenewable resources. However, lithium-ion batteries used in handheld devices and electric vehicles currently use expensive and rare materials that are not produced domestically, limiting affordability and domestic supply chain security. Developing batteries with low-cost, sustainable, and domestically-sourced materials such as sodium, magnesium, or calcium could overcome these challenges, but new chemistries are needed to increase the performance of batteries based on these materials. This research aims to lead the development of next-generation battery chemistries based on these elements to support the domestic production of low-cost battery solutions that increase the competitiveness and independence of the U.S. in the renewable energy sector. Moreover, this effort promotes inclusivity and fosters the growth of future scientists and engineers in this field.Currently, beyond Li-ion batteries have limitations due to their low-capacity cathodes and poor electrolyte stability. This makes them less competitive in high-energy density applications. The aim of this project is to create affordable and high-performance beyond Li-ion batteries that can compete in the market by researching reversible electrolytes and high-capacity cathodes for these batteries. The strategy for accomplishing this ambitious goal is to leverage a combined computational and experimental approach to: 1) investigate a set of high-energy density hybrid cathodes where sulfur is chemically bound to a catalytic substrate material, 2) discover advanced electrolytes based on the tunable borate chemistry, and 3) map the various reaction mechanisms based on novel cathodes and electrolytes to their macroscopic performance, which will inform the rational discovery of superior Na, Mg, and Ca anode chemistries. This mechanistic map will be iteratively applied and refined by computationally predicting superior hybrid cathodes and borate electrolytes, characterizing their performance, and revising the mechanistic understanding.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.