Jin, H.Yu, H.Li, H.Davey, K.Song, T.Paik, U.Qiao, S.2022-05-162022-05-162022Angewandte Chemie International Edition, 2022; 61(27)1433-78511521-3773https://hdl.handle.net/2440/135122First published: 19 April 2022Electrocatalysts for high-rate hydrogen evolution reaction (HER) are crucial to clean fuel production. Nitrogen-rich 2D transition metal nitride, designated “nitridene”, has shown promising HER performance because of its unique physical/chemical properties. However, its synthesis is hindered by the sluggish growth kinetics. Here for the first time using a catalytic molten-salt method, we facilely synthesized a V−Mo bimetallic nitridene solid solution, V0.2Mo0.8N1.2, with tunable electrocatalytic property. The molten-salt synthesis reduces the growth barrier of V0.2Mo0.8N1.2 and facilitates V dissolution via a monomer assembly, as confirmed by synchrotron spectroscopy and ex situ electron microscopy. Furthermore, by merging computational simulations, we confirm that the V doping leads to an optimized electronic structure for fast protons coupling to produce hydrogen. These findings offer a quantitative engineering strategy for developing analogues of MXenes for clean energy conversions.en© 2022 The Authors.Angewandte Chemie International Edition published by Wiley-VCHGmbH.This is an open access article under the terms of the Creative Commons Attribution License,which permits use, distribution and reproduction in any medium,provided the original work is properly cited.2D NitrideneCatalyst DesignElectrocatalysisHydrogen EvolutionMXenesJournal article10.1002/anie.2022038502022-05-16608977Jin, H. [0000-0002-1950-2364]Li, H. [0000-0002-9448-6771]Davey, K. [0000-0002-7623-9320]Qiao, S. [0000-0002-1220-1761] [0000-0002-4568-8422]