as a particularly promising and appealing technology because it has the potential to be both environmentally friendly and low cost. [2] This application creates demand for non-noble-metal-based electrocatalysts to substitute for the currently used highcost Pt catalysts; however, the development remains extremely challenging.High-entropy materials (HEMs) with unique microstructures and unprecedented physicochemical and mechanical properties have attracted a great deal of research interest in many different applied research fields. [3,4] High-entropy alloys (HEAs), as a prominent and already wellestablished group of HEMs, are generally defined as containing five or more principal components alloyed into a crystalline solid-solution phase with unexpected stability and chemical complexity. Many HEAs have demonstrated superior properties relative to traditional alloys, including unprecedented fracture toughness at cryogenic temperatures, [5] ultra-high mechanical performance overcoming the trade-off between strength and ductility, [6] and excellent catalytic selectivity and activities. [7] Largely because of their proximal arrangement of Electrochemical water splitting offers an attractive approach for hydrogen production. However, the lack of high-performance cost-effective electrocatalyst severely hinders its applications. Here, a multinary highentropy intermetallic (HEI) that possesses an unusual periodically ordered structure containing multiple non-noble elements is reported, which can serve as a highly efficient electrocatalyst for hydrogen evolution. This HEI exhibits excellent activities in alkalinity with an overpotential of 88.2 mV at a current density of 10 mA cm −2 and a Tafel slope of 40.1 mV dec −1 , which are comparable to those of noble catalysts. Theoretical calculations reveal that the chemical complexity and surprising atomic configurations provide a strong synergistic function to alter the electronic structure. Furthermore, the unique L1 2 -type ordered structure enables a specific site-isolation effect to further stabilize the H 2 O/H* adsorption/desorption, which dramatically optimizes the energy barrier of hydrogen evolution. Such an HEI strategy uncovers a new paradigm to develop novel electrocatalyst with superior reaction activities.As society seeks to drastically reduce the future usage of fossil fuels, molecular hydrogen is widely recognized as one of the most sustainable and regenerative alternative energy resources. [1] When considering the wide range of hydrogen production methods, electrochemical water splitting has been identifiedThe ORCID identification number(s) for the author(s) of this article can be found under https://doi.
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