Synergetic hydrogen-bond network of functionalized graphene and cations for enhanced atmospheric water capture

• 成果类型: Article
• 署名作者: 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
• 署名单位: University of New South Wales Sydney; Harbin Institute of Technology; University of New England; Okayama University; Institute for Functional Intelligent Materials (I-FIM); National University of Singapore; Consejo Superior de Investigaciones Cientificas (CSIC); Barcelona Institute of Science & Technology; Catalan Institute of Nanoscience & Nanotechnology (ICN2); Barcelona Institute of Science & Technology; Indian Institute of Technology System (IIT System); Indian Institute of Technology (IIT) - Roorkee; University of New South Wales Sydney; National University of Singapore
• 刊物名称: PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
• ISSN/ISSBN: 0027-14769
• DOI: 10.1073/pnas.2508208122
• 发表日期: 2025-06-24
• 关键词: hydration behavior; free-energies; oxide; adsorption; ions; interfaces; molecules; membrane; DYNAMICS; systems

摘要

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.