Self‐Terminating Surface Reconstruction Induced by High‐Index Facets of Delafossite for Accelerating Ammonia Oxidation Reaction Involving Lattice Oxygen

• DOI: 10.1002/smll.202207727
• Publication Date: 2023-01-21T03:44:06Z
• Authors: Shuo Zhang; Huimin Jiang; Liting Yan; Yanchao Zhao; Lingzhi Yang; Qiuju Fu; Dawei Li; Jun Zhang; Xuebo Zhao
• Keywords: Delafossite

Abstract Ammonia (NH 3 ) is a promising hydrogen (H 2 carrier for future carbon‐free energy systems, due to its high content and easiness be liquefied. Inexpensive efficient catalysts ammonia electro‐oxidation reaction (AOR) are desired in whole ammonia‐based systems. In this work, ultrasmall delafossite (CuFeO polyhedrons with exposed high‐index facets prepared by one‐step NH ‐assisted hydrothermal method, serving as AOR pre‐catalysts. The CuFeO facet revealed facilitate surface reconstruction into active Cu‐doped FeOOH nanolayers during processes alkaline solutions, which driven the favorable Cu leaching terminates 2p levels of internal lattice oxygen change. reconstructed heterostructures effectively activate dehydrogenation steps exhibit potential improvement 260 mV electrocatalytic at 10 mA cm −2 compared pre‐restructured phase. Further, density functional theory (DFT) calculations confirm that lower barrier rate‐determining step (*NH *NH presented on covered nanolayers. Innovatively, atoms Fe‐based oxides oxyhydroxide involved proton acceptor, broadening horizons rational designs catalysts.