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型中发挥着关键作用。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。 近年来，由于其安全风险低、元素资源丰富、成本低、环境友好等优点，水基锌离子电池引起了人们极大的研究兴趣。然而，与最先进的锂离子电池相比，由于其较低的能量密度和有限的循环寿命，它们的广泛使用受到限制。该项目旨在通过设计新型的“膨胀粘土中的水”电解质来开发高电压，耐用和具有成本效益的水性锌离子电池，以解决这些问题。从该项目中获得的知识将对缓解有效电网规模储能的电力供应问题产生直接影响，并加速独特材料设计在其他能源和环境工程领域的潜在应用，如粘附和吸收。该项目包括综合外展活动，如为当地K-12学生和教师开展的研究项目，这些项目可以帮助学生获得相关知识和技能。该项目还将使研究生和本科生，包括那些来自代表性不足的群体，在材料和电化学储能领域的教育和培训。该项目旨在建立一个新的，低成本的准固态“膨胀粘土中的水”电解质的结构-性能相关性的基本理解，以实现高电压，高能量，以及用于电网规模能量存储的水性锌离子电池的长循环寿命。通过化学改性调整膨胀粘土的原子结构和界面化学的合理电解质设计策略预计将有效抑制水活性（例如，分解），导致电池单元的电化学性能增强。该提案的目的是：（1）通过多尺度建模揭示基本机制，以理解和控制水分子，粘土和离子之间的相互作用，从而导致高工作电压和增强的能量密度和基于“膨胀粘土中的水”的锌离子电池的循环寿命，以及（2）通过开发这种高电压，耐用的水性电池来验证建模结果。研究方法是整合先进准固态电解质的第一性原理计算，分子动力学模拟，相场建模和实验验证，然后是高性能电池的演示。获得的基础知识有望加速水溶液锌离子电池作为锂离子电池的竞争性替代品的商业化，并解决燃料电池和超锂电池等其他水溶液电化学储能系统中的紧迫问题。该奖项反映了NSF的法定使命，并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，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.