Solid-Solid Interfacial Chemistry in Energy Storage and Conversion Systems

能源需求的大幅增长需要安全、大规模和可持续的未来能源转换和储存装置，这些装置通常由固体材料制成。不明确的界面化学可能是阻碍这些设备性能和寿命的根源。本提案解决了下一代能源设备——固体钠离子电池和钙钛矿太阳能电池界面的基本过程。我们将电化学与多学科光谱和微观分析相结合，以询问电极和固体电解质（或钙钛矿）界面发生的化学反应，特别是在设备操作过程中。微扰允许在设备操作的不同阶段对界面化学特性进行明确的解释。******长期目标是彻底理解固体-固体电化学界面的结构-性能关系，并最终将材料合成和加工结合起来，实现优化的界面设计，以提高器件性能。我们通过开发原位测量工具来启动这项研究计划，以实现两个短期目标。* * * * * * 1。控制全固态钠电池（ASSB）的电极/电解质界面。ASSB利用丰富的资源，提高电池的安全性。固体电解质（SE）和电极界面的降解会影响电池的循环寿命。在循环过程中，SE/电极界面的身份和转变仍然难以捉摸。我们将研究硫代磷酸钠固体钠离子导体（一种潜在的ASSBat电极表面固体电解质材料）在电池运行过程中的化学和机械稳定性。这项工作将揭示与电池短路和容量衰减相关的界面分解机制。这些启示将指导稳定的se或界面保护材料的分子设计，并阐明界面工程协议。******2了解钙钛矿太阳能电池（PSC）的滞后性。钙钛矿太阳能电池表现出卓越的能量转换效率。器件迟滞的结构根源尚不清楚。高度期望器件稳定。我们将运用我们在现场界面表征方面的专业知识，并询问器件滞后的两个潜在原因：(1)钙钛矿/氧化物相互作用和内置电位导致的界面电荷捕获，以及(2)钙钛矿结构中离子在电位下的迁移。研究结果将为具有优异稳定性的高性能psc的材料和界面设计提供见解。******该项目开发的原位界面测量方法将作为一个可移动平台，用于研究其他下一代能源设备，如高能固态电池（多价电池）、无铅psc和其他新兴的能量存储和转换系统

The substantial growth of energy demand requires safe, large scale, and sustainable future energy conversion and storage devices, which are often made of solid materials. Poorly defined interfacial chemistries are likely the origins that hinder the performance and lifetime of these devices. This proposal addresses the fundamental processes at interfaces of the next-generation energy devicesall-solid sodium-ion batteries and perovskite solar cells. We combine electrochemistry with multi-disciplinary spectroscopic and microscopic analysis to interrogate chemistry occurring at electrode and solid-electrolyte (or Perovskite) interface, particularly during device operation. Perturbations allow for explicit interpretation of interfacial chemical identity at different stages of device operation. ******The long-term objective is a thorough understanding of the structure-property relationship at the solid-solid electrochemical interfaces, and ultimately combine material synthesis and processing to enable optimized interfacial design for promoted device performances. We initiate this research program by developing in-situ measurement tools to realize two short-term objectives. ******1. Control the electrode/electrolyte interface for All-solid Sodium Battery (ASSB). ASSB utilize abundant resources and improve battery safety. Degradation at the solid electrolyte (SE) and electrode interface hinders the battery cycle life. The identity and transformation of the SE/electrode interface during cycling remain elusive. We will investigate the (chemical and mechanical) stabilities of sodium thiophosphate solid Na-ion conductor a potential solid electrolyte material for ASSBat the electrode surfaces during battery operation. This work will reveal the mechanisms of interfacial decomposition that associated with battery shorting and capacity fade. These implications will guide the molecular design of stable SEs or interfacial protection materials, and shed light on interfacial engineering protocols.******2 Understand Hysteresis of Perovskite Solar Cell (PSC). Perovskite solar cells show outstanding energy conversion efficiencies. Structural origins of device hysteresis remain unclear. Device stabilization is highly desired. We will implement our expertise in in-situ interfacial characterization and interrogate the two potential reasons for the device hysteresis: (1) interfacial charge trapping due to Perovskite/oxide interaction and built-in potentials, and (2) ion mobility in Perovskite structure under electrical potential. Results will provide insights into the material and interface design for high-performance PSCs with excellent stability.******The in-situ interfacial measurement methods developed in this program will serve as a transportable platform to study other next-generation energy devices such as high energy solid state batteries (multivalent batteries), lead-free PSCs, and other emerging energy storage and conversion systems.**