Engineering principles for sustainable organic electrode materials

可持续有机电极材料的工程原理

• 批准号: 2124604
• 负责人: Shiyu Zhang
• 金额: $ 43.73万
• 依托单位: Ohio State University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2021
• 资助国家: 美国
• 起止时间: 2021-09-01 至 2024-08-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2124604&HistoricalAwards=false
• 关键词: Engineering; principles; sustainable; organic; electrode

Lithium-ion batteries have become one of the leading electrochemical energy storage systems driving the progress of modern electronic technologies. However, the production of conventional lithium-ion batteries relies on finite and unsustainably sourced transition metals, such as lithium and cobalt, which will inevitably restrict their application in the long term. In this research project, the investigators seek to develop new organic electrode materials as alternative energy storage media in batteries. These new battery materials are made of abundant elements, such as carbon, nitrogen, oxygen, and sulfur, and can provide a more economical and sustainable route to renewable energy storage. These research activities are integrated with the training of graduate and undergraduate students in addressing scientific challenges at the interface of electrochemistry, synthetic chemistry, and machine learning. The educational aims include developing a laboratory exercise for an undergraduate general chemistry course that will introduce students to connections between electrochemistry and environmental water quality testing and a mentoring program for these students which connects them with peer tutors. Organic electrode materials (OEM) are promising alternatives to unsustainably sourced transition metals as energy storage media in lithium-ion batteries. Current OEMs (primarily redox organic polymers), however, suffer from (a) poor conductivity (30% carbon loading required), (b) poor cycling stability (ca. 100 cycles), and (c) sloping/multiple-stage voltage profiles. The overall goal of the research project is to discover, elucidate, and apply engineering principles to improve the rechargeability of OEMs. First, a wide array of novel small-molecule OEMs featuring strong intermolecular interactions are prepared. In-situ and ex-situ spectroscopic studies are performed to understand how the intermolecular interactions between charge storage units change as a function of state-of-charge. These tasks will explore the hypotheses that complementary hydrogen bonding and pi-pi stacking improve the stability of quinone-fused aza-phenazine OEM materials. It is predicted that additional intermolecular disulfide bonds between sulfur-rich thiazyl charge storage units can improve conductivity and facilitate high-rate cycling of OEMs. These results and new fundamental understanding will be used to develop new design principles for optimizing the conductivity, stability, voltage profile of OEMs through modification of molecular structure. In the second part of the proposal, the research project seeks to develop machine learning-based models that can (a) predict the long-term cycling life of OEMs using data collected from short-term high-throughput tests and (b) recommend new highly stable OEMs based on physical organic descriptors. This systematic study will ultimately reveal unintuitive design principles that enable more focused research efforts in place of extensive trial-and-error screening.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.

锂离子电池已成为推动现代电子技术进步的领先电化学能源存储系统之一。但是，常规锂离子电池的生产依赖于有限的和不可能的过渡金属，例如锂和钴，从长远来看，这将不可避免地限制其应用。在该研究项目中，研究人员试图开发新的有机电极材料作为电池中的替代储能介质。这些新的电池材料由丰富的元素制成，例如碳，氮，氧气和硫，并且可以提供更经济和可持续的途径以可再生能源存储。这些研究活动与研究生和本科生的培训相结合，以应对电化学，合成化学和机器学习界面的科学挑战。教育目的包​​括为大学一般化学课程开发实验室练习，该课程将向学生介绍电化学与环境水质测试之间的联系，以及针对这些学生与同伴导师相关的这些学生的指导计划。有机电极材料（OEM）是在锂离子电池中作为储能介质的不可持续的过渡金属的有希望的替代品。然而，当前的OEM（主要是氧化还原有机聚合物）遭受（a）的电导率较差（需要30％的碳负载），（b）循环稳定性不佳（CA。100个循环）和（c）倾斜/多阶段电压曲线。研究项目的总体目标是发现，阐明和应用工程原则，以提高OEM的可再生能力。首先，准备了各种具有强分子间相互作用的新型小分子OEM。进行原位和原位光谱研究，以了解电荷存储单元之间的分子间相互作用如何随着电荷的函数而变化。这些任务将探讨互补的氢键键合和PI-PI堆叠的假设可改善喹酮融合的偶氮苯唑OEM材料的稳定性。可以预测，富含硫的硫嗪电荷存储单元之间的其他分子间二硫键可以提高电导率并促进OEM的高速循环。这些结果和新的基本理解将用于开发新的设计原理，以通过修饰分子结构来优化OEM的电导率，稳定性，电压谱。在提案的第二部分中，该研究项目试图开发基于机器学习的模型，以（a）使用从短期高通量测试中收集的数据预测OEM的长期循环寿命，并且（b）建议基于物理有机描述符的新高度稳定的OEM。这项系统的研究最终将揭示不直觉的设计原则，该原则能够实现更加集中的研究工作，以替代广泛的反复试验筛查。该奖项反映了NSF的法定任务，并被认为是值得通过基金会的智力优点和更广泛的影响来通过评估来支持的。

项目成果

Gaseous Nitrogen Oxides Catholyte for Rechargeable Redox Flow Batteries

用于可充电氧化还原液流电池的气态氮氧化物阴极电解液

• DOI: 10.1002/anie.202216889
• 发表时间: 2023
• 期刊: Angewandte Chemie International Edition
• 作者: Zhang, Weiyao;Yang, Xin;Zhang, Shiyu
• 通讯作者: Zhang, Shiyu