Dali Ji

Solid‐state electrolytes offer improved safety compared to liquid counterparts but suffer from inherent limitations when used as single‐component systems. Composite electrolytes, combining complementary materials, provide a promising route to overcome these issues. Among fabrication techniques, in situ polymerization stands out for its ability to construct intimately integrated composite polymer electrolytes with enhanced interfacial stability and tunable architectures. However, a systematic and comprehensive review of recent advances in in situ polymerized composite polymer electrolytes (CPEs) is still lacking. In this work, recent developments in in situ polymerized CPEs are systematically reviewed and categorized based on different polymer matrices and their specific interactions with various inorganic fillers. The fundamental reaction mechanisms governing in situ polymerization are discussed, with particular attention to the coupling between polymerization kinetics, interfacial structure evolution, and ion‐transport pathway reconstruction. Building on this mechanistic perspective, representative polymer–filler systems are analyzed to illustrate how organic–inorganic interactions regulate ionic conductivity, mechanical integrity, and electrochemical stability. Key challenges in current systems are critically assessed, and finally, future perspectives, guidelines, and strategies toward the resolution of these challenges are analyzed and discussed.

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.

Water molecules at the solid-liquid interface display intricate behaviours sensitive to small changes. The presence of different interfacial components, such as cations or functional groups, shape 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.

Bottom‐up electrochemical synthesis of atomically thin materials is desirable yet challenging, especially for non‐van der Waals (non‐vdW) materials. Thicknesses below a few nanometers have not been reported yet, posing the question how thin can non‐vdW materials be electrochemically synthesized. This is important as materials with (sub‐)unit‐cell thickness often show remarkably different properties compared to their bulk form or thin films of several nanometers thickness. Here, a straightforward electrochemical method utilizing the angstrom‐confinement of laminar reduced graphene oxide (rGO) nanochannels is introduced to obtain a centimeter‐scale network of atomically thin (2O₃, a material without significant catalytic activity for the oxygen evolution reaction (OER) in bulk form, can be activated as a high‐performing catalyst if synthesized in the 2D sub‐unit‐cell form. This method displays the high activity of sub‐unit‐cell form while retaining the stability of bulk form, promising to yield unexplored fundamental science and applications. It is shown that while retaining the advantages of bottom‐up electrochemical synthesis, like simplicity, high yield, and mild conditions, the thickness of TMO can be limited to sub‐unit‐cell dimensions.