Nature of Proton Transfer in Water near Interfaces

当水被用于技术应用时--无论是在燃料电池、药物输送过程中，还是在电催化中--它都与界面接触。然而，水不仅仅是一种纯净的液体，而是由有限浓度的氢氧化物离子和过剩的质子组成，这取决于液体的pH值。只有从根本上了解这些溶剂化质子和氢氧化物离子在与技术相关的界面附近的行为方式，新技术的目标优化才能成为可能，以应对我们未来的一些核心社会挑战。这包括多种过程和应用，如燃料电池、沿生物通道的质子转移、海洋酸化以及酶催化，因此与未来的主要优先事项有关。为了阐明界面附近质子转移的性质，计算机模拟是补充实验的关键。直到现在，所需的模拟技术才能在高性能计算资源上准确和预测地描述这些物种在界面附近的动态和反应特性。借助于量子模拟技术，基于新的机器学习模型，我们将对质子和氢氧化物离子在界面上的结构和动力学有一个全新的认识。这包括碳基和六方氮化硼2D材料附近的质子转移机制，但也包括过多的质子或氢氧化物离子是否积累在这些界面上的问题。通过与实验工作，特别是介电显微镜和表面灵敏振动光谱的密切合作，将提供对这些现象的统一理解，作为生物过程和技术应用的坚实基础。

Whenever water is used in technological applications ― be it in fuel cells, drug delivery processes, or electro-catalysis ― it is in contact with interfaces. However, water is not just a pure liquid, but rather consists of a finite concentration of hydroxide ions and excess protons depending on the pH value of the liquid. Only if it is fundamentally understood, how such solvated protons and hydroxide ions behave near technologically relevant interfaces, the target-oriented optimization of new technologies will become possible in order to address some of our central societal challenges of the future. This includes diverse processes and applications such as fuel cells, the proton transfer along biological channels, the acidification of our oceans, as well as enzyme catalysis and is, thus, linked to major priorities of the future.In order to elucidate the nature of proton transfer near interfaces, computer simulations are key to complement experiment. Only now the required simulation techniques have become available to accurately and predictively describe the dynamical and reactive character of these species near interfaces on high performance computing resources. By means of quantum simulation techniques, based on new machine learning models, we will obtain a fundamental new understanding of the structure and dynamics of protons and hydroxide ions at interfaces. This includes the mechanism of proton transfer near carbon-based and hexagonal boron nitride 2D materials, but also the question whether excess protons or rather hydroxide ions accumulate at such interfaces. In close collaboration with experimental work, in particular dielectric microscopy and surface sensitive vibrational spectroscopy, a united understanding of these phenomena will be provided as solid foundation for biological processes and technical applications.