The ubiquity of aqueous solutions in contact with charged surfaces and the realization that the molecular-level details of water–surface interactions often determine interfacial functions and properties relevant in many natural processes have led to intensive research. Even so, many open questions remain regarding the molecular picture of the interfacial organization and preferential alignment of water molecules, as well as the structure of water molecules and ion distributions at different charged interfaces. While water, solutes and charge are present in each of these systems, the substrate can range from living tissues to metals. This diversity in substrates has led to different communities considering each of these types of aqueous interface. In this Review, by considering water in contact with metals, oxides and biomembranes, we show the essential similarity of these disparate systems. While in each case the classical mean-field theories can explain many macroscopic and mesoscopic observations, it soon becomes apparent that such theories fail to explain phenomena for which molecular properties are relevant, such as interfacial chemical conversion. We highlight the current knowledge and limitations in our understanding and end with a view towards future opportunities in the field.

与带电表面接触的水溶液无处不在，以及水与表面相互作用的分子水平细节通常决定许多自然过程中相关的界面功能和特性的认识导致了深入的研究。即便如此，关于界面组织的分子图和水分子的优先排列，以及水分子的结构和不同带电界面的离子分布，仍然存在许多悬而未决的问题。虽然这些系统中的每一个都存在水、溶质和电荷，但底物的范围可以从活组织到金属。底物的这种多样性导致不同的社区考虑这些类型的水界面中的每一种。在这篇评论中，通过考虑与金属、氧化物和生物膜接触的水，我们展示了这些不同系统的本质相似性。虽然在每种情况下，经典平均场理论都可以解释许多宏观和介观观察结果，但很快就会发现，这些理论无法解释与分子特性相关的现象，例如界面化学转化。我们强调当前的知识和我们理解的局限性，并以对该领域未来机会的看法结束。