Ren Xiaojun, Sui Xiao, Karton Amir, Nishina Yuta, Lin Tongxi, Asanoma Daisuke, Owens Llewellyn, Ji Dali, Wen Xinyue, Quintano Vanesa, Tripathi Komal, Pant Kamal K, Dai Liming, Andreeva Daria V, Foller Tobias, Novoselov Kostya S, Joshi Rakesh
School of Materials Science and Engineering, University of New South Wales Sydney, NSW 2052, Australia.
School of Marine Science and Technology, Harbin Institute of Technology, Weihai 264209, China.
Proc Natl Acad Sci U S A. 2025 Jun 24;122(25):e2508208122. doi: 10.1073/pnas.2508208122. Epub 2025 Jun 20.
Water molecules at the solid-liquid interface display intricate behaviors sensitive to small changes. The presence of different interfacial components, such as cations or functional groups, shapes the physical and chemical properties of the hydrogen-bond network. Understanding such interfacial hydrogen-bond networks is essential for a large range of applications and scientific questions. To probe the interfacial hydrogen-bond network, atmospheric water capture is a powerful tool. Here, we experimentally observe that a calcium ion on a calcium-intercalated graphene oxide aerogel (Ca-GOA) surface captures 3.2 times more water molecules than in its freestanding state. From experimental Van't Hoff estimation and density functional theory (DFT) calculations, we uncover the synergistically enhanced hydrogen-bond network of the calcium ion-epoxide complex due to significantly larger polarizations and hydrogen bond enthalpies. This study reveals valuable insights into the interfacial water hydrogen-bond network on functionalized carbon-cation complexed surfaces and potential pathways for future atmospheric water generation technologies.
固液界面处的水分子表现出对微小变化敏感的复杂行为。不同界面成分（如阳离子或官能团）的存在塑造了氢键网络的物理和化学性质。理解此类界面氢键网络对于广泛的应用和科学问题至关重要。为了探测界面氢键网络，大气水捕获是一种强大的工具。在此，我们通过实验观察到，钙插层氧化石墨烯气凝胶（Ca-GOA）表面的钙离子捕获的水分子数量比其独立状态下多3.2倍。通过实验范特霍夫估计和密度泛函理论（DFT）计算，我们发现由于显著更大的极化和氢键焓，钙离子-环氧复合物的氢键网络协同增强。这项研究揭示了关于功能化碳-阳离子复合表面上的界面水氢键网络的宝贵见解以及未来大气水生成技术的潜在途径。
