Kang, Bobin Ha, Thanh Duy Cam Barakat, Alaelddin Michailidis Lee, Gyumin Lee, Heehyeon Oh, Youngtak Kim, Hyunjeong Chung, In Yoon, Seok Min Kim, Myung-gil 2026-01-15T08:00:34Z 2026-01-15T08:00:34Z 2026-01-12 2026-01 1433-7851 https://pubs.kist.re.kr/handle/201004/154011 The metal cation linker in metathesis-derived chalcogels critically governs structural evolution, porosity, and resultant physicochemical properties. However, most studies have emphasized atomic-scale functionality of metal linker within chalcogel network, with limited attention to local structural transformation and even long-range ordering. This work demonstrates the unprecedented role of cerium ions in directing the formation of a sustainable 2D crystalline Ce–Sn–S (CTS) chalcogel. The crystalline framework arises from coordination transformation of SnS4 tetrahedra within Sn2S6 dimers into distorted Sn3S4 broken-cube clusters, yielding a [Sn3S7]n2n− layered geometry. Cerium oxidation states, particularly Ce3+ enrichment, further stabilize the crystalline network via a templating effect and enhance electrocatalytic activity. The optimized CTS-5 chalcogel exhibits superior oxygen evolution reaction performance, including a low overpotential of 300 mV at 10 mA cm−2, the lowest Tafel slope of 80 mV dec−1, and stable operation for 50 h at 10 mA cm−2. The crystalline CTS chalcogel represents a new class of aerogel materials, where robust 2D crystallinity persists even under high cation loading, enabling functional tunability without compromising network integrity. English John Wiley & Sons Ltd. All-Scale Structural Optimization of Resiliently Crystalline Na–Ce–Sn–S Chalcogel for Efficient Oxygen Evolution Reaction Electrocatalyst Article 10.1002/anie.202523034 1 Angewandte Chemie International Edition, v.65, no.5 Angewandte Chemie International Edition 65 5 N scie 2-s2.0-105024765312 Chemistry, Multidisciplinary Chemistry Article; Early Access HIGHLY EFFICIENT THIOSTANNATE CS+ CHEMISTRY AEROGELS Crystalline aerogels Electrocatalysis Metal-chalcogenide aerogels Oxygen evolution reaction (OER)