Mechanism Switching of Ammonia Synthesis Over Ru-Loaded Electride Catalyst at Metal-Insulator Transition.
作者： Shinji Kanbara , Masaaki Kitano , Yasunori Inoue , Toshiharu Yokoyama , Michikazu Hara
DOI: 10.1021/JACS.5B10145
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摘要: The substitution of electrons for O2– anions in the crystallographic cages [Ca24Al28O64]4+(O2–)2 was investigated to clarify correlation between electronic properties and catalytic activity ammonia synthesis Ru-loaded [Ca24Al28O64]4+(O2–)2–x(e–)2x (0 ≤ x 2). This catalyst has low performance with an electron concentration (Ne) lower than 1 × 1021 cm–3 a high apparent activation energy (Ea) comparable that conventional Ru-based catalysts basic promoter such as alkali or alkaline earth compounds. Replacement more half cage (Ne ≈ cm–3) significantly changes reaction mechanism yield is order higher Ea. metal–insulator transition also occurs at Ne triggered by structural relaxation induced replacement electrons. These observat...
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