Hierachical modeling of self-organization and transport in proton-conducting media: from understanding to advanced functional materials

该计划探索理论化学物理和分子建模领域。长期目标是开发材料建模的分层策略，配备先进功能材料设计的预测能力以及其特性和操作的诊断。主要的动力来自迫切的能源挑战，这推动了全世界对燃料电池的研究。聚合物电解质燃料电池的独特资产的开发取决于其材料的进展。先进的材料必须保持燃料电池无与伦比的热力学效率和高能量密度，同时它们应该提高功率密度与成本的比率。材料科学前沿的一个主要目标是开发具有增强质子传输和稳定性的质子导体。常见的聚合物电解质膜通过充满水的孔隙的随机网络引导质子。这些材料的物理性质在bbbb6长度尺度上演变，从分子尺度上的质子和水的迁移，通过中尺度上的结构演变和物理过程，到宏观上的运输和操作。我们利用精心设计的物理理论模型层次来解决这些多尺度挑战。主要模块集中在聚合物自组装，界面质子传输和水合聚合物的吸水特性。在不同尺度上获得的信息将被整合成对膜结构和功能的一个有凝聚力的描述，这反过来将揭示在合成、实验和操作过程中变化的参数的影响。因此，这项研究可以显著提高组装新型分层结构膜的前景。此外，我们的研究对理解生物膜和脂质单层的过程做出了重要贡献。材料科学、软凝聚态物理和生物化学的跨学科拓展，以及物理和化学领域提供的理论和计算方法，为培养学生和博士后创造了极好的前景。

The proposed program explores the realms of theoretical chemical physics and molecular modeling. The long-term objective is to develop hierarchical strategies in materials modeling, outfitted with predictive capabilities for the design of advanced functional materials and the diagnostics of their properties and operation. The main incentive stems from the urging energy challenge that drives worldwide research on fuel cells. Exploitation of the unique assets of polymer electrolyte fuel cells hinges on progress in their materials. Advanced materials have to preserve the unrivalled thermodynamic efficiencies and high energy densities of fuel cells, while they should boost the ratio of power density to cost. A primary goal on the materials science front is to develop proton conductors with enhanced proton transport and stability. The prevalent types of polymer electrolyte membranes channel protons through random networks of water-filled pores. The physical properties of these materials evolve over > 6 length scales, from mobilities of protons and water at molecular scale via structural evolution and physical processes at the mesoscale to macroscopic transport and operation. We exploit a well-devised hierarchy of physical-theoretical models to address these multiscale challenges. Major modules focus on polymer self-assembly, interfacial proton transport, and water sorption characteristics of hydrated polymers. Information obtained at different scales will be integrated into a cohesive description of membrane structure and function, which in turn will reveal the effects of the parameters that vary during synthesis, experiment, and operation. Thereby, this research could significantly enhance the prospects of efforts in assembling novel hierarchically structured membranes. Our research, moreover, makes vital contributions to the understanding of processes at biomembranes and lipid monolayers. The interdisciplinary outreach in materials science, soft condensed matter physics, and biochemistry together with the offered spectrum of theoretical and computational methods in physics and chemistry create excellent perspectives for the training of students and postdoctoral fellows.