NSF-BSF: Physical-Chemical Stabilization of Electrodeposition through Fundamental Interfacial Studies

电化学存储系统（电池）无处不在，从商业电子产品到电动汽车，应有尽有。在电池中，物理化学过程驱动界面上复杂的耦合现象，如电沉积。电沉积是金属离子（溶解在电解质中）在电场存在下沉积到导电表面（电极）上的过程。电池电极上不稳定（即不均匀）的电沉积会导致性能下降和失效。这是限制下一代电池的主要挑战之一，下一代电池具有远程电动汽车和可再生能源电网规模储能的潜力。在本项目中，研究人员将采用综合计算-实验方法来研究电沉积过程中界面区域物理-化学过程的复杂耦合，从而导致不稳定的沉积。然后，该团队将利用这些知识来定义电沉积的物理化学稳定（或不稳定）区域。这项研究将为设计出更稳定、寿命更长、容量更高的电池奠定基础。该项目是美国和以色列研究人员之间的合作，将为学生提供机会，不仅了解最先进的研究，而且与不同的文化互动和学习。该项目将在美国波士顿大学（Boston University）和以色列耶路撒冷希伯来大学（The Hebrew University of Jerusalem）培训研究生，并将通过在两国开展外展活动吸引k-12学生。不稳定电沉积是由非均匀性引起的，包括非均匀输运、反应性、应力等，并导致性能损失和失效。虽然均匀材料/界面/系统的理想发展将解决这些问题，但不可能制造完美的系统。在本项目中，研究人员将采用综合计算-实验方法来研究电沉积过程中界面区域物理-化学过程的复杂耦合，从而导致不稳定的沉积。然后，该团队将利用这些知识来定义电沉积的物理化学稳定（或不稳定）区域。利用计算和实验模型系统，我们将研究几种金属系统（即银、铜、锌等）的物理和化学性质对电沉积的影响，目的是全面了解稳定电沉积的驱动力，从而绘制电沉积稳定和不稳定的图谱。该项目将测试电极表面电沉积的位置和速率可以通过调整材料系统的物理化学性质来控制的假设。为了实现研究目标，介面区域的中尺度计算模型将与电沉积的受控实验研究相结合。电极界面的受控实验研究将为参数化和模型验证提供数据；而计算模型将指导实验研究，并进一步深入了解导致观察到的实验行为的基本物理现象。通过整合实验和计算研究，该项目将发展对驱动不稳定或稳定电沉积的物理化学过程的基本理解，包括界面传输，表面特征，如工程表面粗糙度，通过掺杂剂改变表面反应性，以及结构界面。该奖项反映了美国国家科学基金会的法定使命，并通过使用基金会的知识价值和更广泛的影响审查标准进行评估，被认为值得支持。

Electrochemical storage systems (batteries) are ubiquitous, found in everything from commercial electronics to electric vehicles. In batteries, physical-chemical processes drive complex, coupled phenomena at the interfaces, such as electrodeposition. Electrodeposition is the deposition of metallic ions (dissolved in an electrolyte) onto an electrically conductive surface (the electrode) in the presence of an electric field. Unstable (i.e. non-uniform) electrodeposition on the electrodes of batteries leads to performance degradation and failure. This is one of the main challenges limiting next generation batteries, which hold potential for longer range electric vehicle and grid scale energy storage for renewable energy. In this project, the investigators will use an integrated computational-experimental approach to study the complex coupling of physical-chemical processes in the interface region during electrodeposition that lead to unstable deposition. The team will then use that knowledge to define regions of physical-chemical stabilization (or destabilization) of electrodeposition. This research will lay the foundation for engineering more stable batteries with longer lifetimes and higher capacities. This project is a collaboration between researchers in the United States and Israel and will provide opportunities for students to not only learn about state-of-the-art research but also to interact with and learn about different cultures. The project will train graduate students in both the United States at Boston University and in Israel at The Hebrew University of Jerusalem, and will engage k-12 students through outreach activities in both countries.Unstable electrodeposition is caused by heterogeneities, including non-uniform transport, reactivity, stresses, etc., and leads to performance loss and failure. While ideally development of homogeneous materials/interfaces/systems would solve these issues, it is impossible to fabricate perfect systems. In this project, the investigators will use an integrated computational-experimental approach to study the complex coupling of physical-chemical processes in the interface region during electrodeposition that lead to unstable deposition. The team will then use that knowledge to define regions of physical-chemical stabilization (or destabilization) of electrodeposition. Using computational and experimental model systems we will investigate the effects of both physical and chemical properties on electrodeposition for several metal systems (i.e. silver, copper, zinc, etc.) with the goal of developing a holistic understanding of the driving forces for stable electrodeposition that will lead to the mapping of electrodeposition stabilization and destabilization regimes. This project will test the hypothesis that the location and rate of electrodeposition on the electrode surface can be controlled by tuning the physical-chemical properties of the material system. To accomplish the research objectives a meso-scale computational model of the interfacial region will be coupled with controlled experimental investigations of electrodeposition. Controlled experimental studies of the electrode interface will provide data for parameterization, and validation of the model; while the computational models will guide experimental studies and provide further insight into the fundamental physical phenomena that lead to observed experimental behavior. By integrating the experimental and computational research, the project will develop a fundamental understanding of the physical-chemical processes that drive unstable or stable electrodeposition including interfacial transport, surface features, such as engineered surface roughness, changing surface reactivity through dopants, and structured interfaces.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.