Chen, XinyuXinyuChenChen, LizhenLizhenChenChen, ChuntaoChuntaoChenShi, DiweiDiweiShiSong, JiexiJiexiSongQin, YanqingYanqingQinWang, XiangmeiXiangmeiWangAmjad, Majeed MuhammadMajeed MuhammadAmjadSun, DongpingDongpingSunSun, BianjingBianjingSunZhang, KaiKaiZhang2024-04-022024-04-022024https://resolver.sub.uni-goettingen.de/purl?gro-2/142687Abstract Manipulating the structural and kinetic dissociation processes of water at the catalyst‐electrolyte interface is vital for alkaline hydrogen evolution reactions (HER) at industrial current density. This is seldom actualized due to the intricacies of the electrochemical reaction interface. Herein, we introduce a rapid, non‐equilibrium cooling technique for synthesizing ternary Turing catalysts with short‐range ordered structures (denoted as FeNiRu/C). These advanced structures empower the FeNiRu/C to exhibit excellent HER performance in 1 M KOH with an ultralow overpotential of 6.5 and 166.2 mV at 10 and 1000 mA cm −2 , respectively, and a specific activity 7.3 times higher than that of Pt/C. Comprehensive mechanistic analyses reveal that abundant atomic species form asymmetric atomic electric fields on the catalyst surface inducing a directed evolution and the dissociation process of interfacial H 2 O molecules. In addition, the locally topologized structure effectively mitigates the high hydrogen coverage of the active site induced by the high current density. The establishment of the relationship between free water population and HER activity provides a new paradigm for the design of industrially relevant high performance alkaline HER catalysts. This article is protected by copyright. All rights reservedenhttp://onlinelibrary.wiley.com/termsAndConditions#vorjournal_article10.1002/adma.202401110