Materials for Electrochemical Energy Conversion: From Fundamental Physics to Advanced Design

此应用程序支持“用于能源应用的电化学材料：从基础物理到高级设计”的研究计划。它探索了理论化学物理和电化学材料建模的领域。长期目标是开发材料建模的分层方法，配备创新设计和诊断的预测能力。社会动因是全球能源挑战。日益增长的能源需求、低效的能源利用以及以化石燃料为基础的能源经济对环境和气候的致命影响，推动着全球能源研究的努力。奥斯特瓦尔德（Ostwald）在1894年指出，电化学材料和器件的卓越多功能性，以及它们无与伦比的热力学效率和减少的环境影响，刺激了电化学技术的发展。软质子材料和多孔电极是此类技术的通用组成部分。我们在这两个领域进行深入的研究项目，涵盖从原子尺度到宏观器件水平的现象。本文主要研究质子导电聚合物电解质膜的理论和模型。它努力发展对这些材料的结构和组成如何决定其物理化学性质和操作的深刻理论理解。电解质研究的首要目标是开发高输运选择性材料，促进质子输运，抑制所有其他物质的输运，包括电子、溶剂分子和反应物气体。鉴于这一目标，关键的科学挑战是阐明溶剂、离子的带电荷表面基团和多孔宿主材料对质子传输的结构和动力学影响。我们将追求的理论膜研究的主要方向包括离聚体束形成和束弹性理论；水的吸附和侵入理论；束断裂与裂缝形成理论；利用分子模型和孤子理论研究酸功能化界面上的质子运动。这个程序将有助于解释具有不同化学结构和组成的膜的性质。结果将指导在组装新的层次结构材料的努力。此外，我们的见解将对聚合物电解质膜以外的重要现象和材料类别具有价值，仅举几例：弹性多孔介质中的结构形成、水侵入和裂缝形成；质子在聚电解质刷、生物膜和脂质单层中的传输。在所有这些方面，我们将与实验小组密切互动，以便系统地审查理论发现并探索其实际用途。从长远来看，我们在电解质和电极方面的综合研究将为纳米质子材料和器件的设计和集成提供理论框架。未来能源技术和基础设施的可行性取决于基础材料科学方面持续努力的成功。该计划的跨学科推广及其在物理和化学方面的理论和计算研究的特殊带宽，为学生提供了良好的学习和职业前景。学生将掌握现代材料科学的发展方向、电化学系统的要求和现代实验技术。在他们自己的研究领域，他们将有机会学习、发展和应用一套理论化学物理和计算材料科学的现代方法。

This application supports a research program in "Electrochemical Materials for Energy Applications: From Fundamental Physics to Advanced Design". It explores the realms of theoretical chemical physics and electrochemical materials modeling. The long-term objective is to develop hierarchical approaches in materials modeling, outfitted with predictive capabilities for innovative design and diagnostics. The societal incentive is the global energy challenge. Ever-increasing energy demand, inefficient energy use, and fatal impacts of the fossil fuel-based energy economy on environment and climate drive worldwide efforts in energy research. The sublime versatility of electrochemical materials and devices as well as their unmatched thermodynamic efficiency and reduced environmental impact, famously noted by Ostwald in 1894, spur the development of electrochemical technologies. Soft protonic materials and porous electrodes are generic components of such technologies. We pursue profound research programs in both areas, encompassing phenomena from atomistic scale to the macroscopic device level. This proposal focuses on theory and modeling of proton-conducting polymer electrolyte membranes. It strives to develop a deep theoretical understanding of how structure and composition of these materials dictate their physicochemical properties and operation. The foremost objective of electrolyte research is to develop highly transport-selective materials that facilitate proton transport and suppress the transport of all other species, including electrons, solvent molecules and reactant gases. Critical scientific challenges in view of this objective are to elucidate structural and dynamic effects of solvent, charge-bearing surface groups of the ionomer, and porous host material on proton transport. The main directions in theoretical membrane research that we will pursue involve a theory of ionomer bundle formation and bundle elasticity; a theory of water sorption and invasion; a theory of bundle breakage and fracture formation; and studies of proton motion at acid-functionalized interfaces using molecular modeling and soliton theory. This program will help explaining the properties of membranes with different chemical architecture and composition. Results will guide efforts in the assembly of novel hierarchically structured materials. Moreover, our insights will be of value for important classes of phenomena and materials beyond polymer electrolyte membranes, to name a few: structure formation, water invasion and fracture formation in elastic porous media; proton transport at polyelectrolyte brushes, biomembranes, and lipid monolayers. On all of these aspects, we will interact closely with experimental groups in order to systematically scrutinize theoretical findings and explore their practical utility. As a long-term perspective, our comprehensive programs in electrolyte and electrode research will furnish the theoretical framework for the design and integration of nanoprotonic materials and devices. The viability of future energy technologies and infrastructures hinges on the success of sustained efforts in fundamental materials science. The interdisciplinary outreach of this program and its exceptional bandwidth of theoretical and computational research in physics and chemistry, offer excellent learning and career perspectives for students. Students will gain a firm grasp of modern directions in materials science, requirements on electrochemical systems, and modern experimental techniques. In the realm of their own research, they will have opportunities to learn, develop, and apply a suite of modern methods in theoretical chemical physics and computational materials science.