Tailoring Quasi-Solid-State 'Water-in-Swelling-Clay' Electrolytes for High-Voltage, Durable Aqueous Zinc-Ion Batteries

电池在可再生能源储存和能源转换中起着至关重要的作用。为了解决风能和太阳能发电的间歇性，需要高性能电池将这些基于可再生能源的发电机连接到电网。水基锌离子电池具有安全风险低、元素资源丰富、成本低、环境友好等优点，近年来引起了人们极大的研究兴趣。然而，它们的广泛使用受到限制，因为与最先进的锂离子电池相比，它们的能量密度较低，循环寿命有限。该项目旨在通过设计新型的“膨胀型粘土”电解液来解决这些问题，从而开发出高电压、耐用和低成本的锌离子水基电池。从该项目中获得的知识将对缓解电网规模高效储能的电力供应问题产生直接影响，并加速这种独特材料设计在其他能源和环境工程领域的潜在应用，如粘合和吸收。该项目包括综合外展活动，如针对当地K-12学生和教师的研究计划，这些活动可以帮助学生获得相关知识和技能。该项目还将在材料和电化学储能领域对研究生和本科生进行教育和培训，包括那些来自代表不足的群体的学生。该项目旨在建立对新型、低成本准固态膨胀型粘土电解液结构-性能关系的基本了解，以实现电网规模储能用水锌离子电池的高电压、高能量和长循环寿命。合理的电解液设计策略通过化学修饰来调节膨胀粘土的原子结构和界面化学性质，有望有效地抑制水的活性(例如分解)，从而提高电池的电化学性能。本建议的目的是：(1)通过多尺度建模来揭示基本的机理，以了解和控制水分子、粘土和离子之间的相互作用，这些相互作用导致水膨胀粘土基锌离子电池的高工作电压、更高的能量密度和循环寿命，以及(2)通过开发这种高电压、耐用的水电池来验证建模结果。研究方法是将先进的准固态电解液的第一性原理计算、分子动力学模拟、相场模拟和实验验证相结合，然后展示高性能电池单元。所获得的基础知识有望加快锌离子水性电池的商业化进程，使其成为锂离子电池的竞争性替代品，并解决燃料电池和锂电池以外的其他水性电化学储能系统中的紧迫问题。这一奖项反映了NSF的法定使命，并通过使用基金会的智力优势和更广泛的影响审查标准进行评估，被认为值得支持。

Batteries play a critical role in renewable energy storage and energy transition. To address the intermittent nature of wind and solar power generations, high-performance batteries are necessary to connect these renewable energy sources-based electricity generators to electric power grid. Aqueous zinc-ion batteries have recently attracted tremendous research interest because of their advantages such as low safety risks, abundant elemental resources, low cost, and eco-friendliness. However, their widespread use is limited due to their lower energy density and limited cycle life compared to state-of-the-art lithium-ion batteries. This project aims to develop high-voltage, durable, and cost-effective aqueous zinc-ion batteries by designing novel ‘water-in-swelling-clay’ electrolytes to address these issues. The knowledge obtained from this project will have a direct impact on alleviating power supply issues for efficient grid-scale energy storage and accelerate potential applications of the unique material design to other energy and environmental engineering fields such as adhesion and absorption. The project includes integrated outreach activities, such as research programs for local K-12 students and teachers, which can help students to acquire relevant knowledge and skills. This project will also enable the education and training of graduate and undergraduate students, including those from underrepresented groups, in the fields of materials and electrochemical energy storage.This project seeks to establish a fundamental understanding of the structure-property correlation of new, low-cost quasi-solid-state ‘water-in-swelling-clay’ electrolytes to achieve high voltage, high energy, and long cycle life of aqueous zinc-ion batteries for grid-scale energy storage. The rational electrolyte design strategy of tuning the atomic structures and interfacial chemistries of the swelling clay by chemical modifications is expected to effectively suppress water activities (e.g., decomposition), resulting in enhanced electrochemical performance of battery cells. The objectives of this proposal are to: (1) reveal fundamental mechanisms by multiscale modeling to understand and control the interactions among water molecules, clays, and ions that lead to high working voltage and enhanced energy density and cycle life of ‘water-in-swelling-clay’-based zinc-ion batteries, and (2) validate the modeling results by developing such high-voltage, durable aqueous batteries. The research approach is to integrate first-principles calculations, molecular dynamics simulations, phase-field modeling, and experimental validation of the advanced quasi-solid-state electrolytes, followed by the demonstration of high-performance battery cells. The gained fundamental knowledge promises to expedite the commercialization of aqueous zinc-ion batteries as competitive alternatives to lithium-ion batteries and address pressing issues in other aqueous electrochemical energy storage systems such as fuel cells and beyond-lithium batteries.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.