Catalytic NO reduction by CO into N₂ and CO₂ is imperative owing to the increasingly rigorous emission regulation. Identifying the nature of active sites that govern the reactivity and selectivity of NO reduction is pivotal to tailor catalysts, while it is extremely challenging because of the complexity of real-life systems. Guided by our newly discovered triatomic Lewis acid–base–acid (LABA, Ce^δ+–Rh^δ−–Ce^δ+) site that accounts for the selective reduction of NO into N₂ catalyzed by the RhCe₂O₃^– cluster in gas-phase experiments, the reactivity of the RhM₂O₃^– (M = Ta, V, and Al) clusters in catalytic NO reduction by CO was explored. We determined theoretically that the LABA site still prevails to reduce NO to N₂ mediated by RhTa₂O₃^– and RhV₂O₃^–, and the strong M-oxygen affinity was emphasized to construct the LABA site. An overall assessment highlights that RhV₂O₃^– functions as a more promising catalyst because the well-fitting V–O bonding strength facilitates both elementary reactions of NO reduction and CO oxidation.

中文翻译：

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由 RhM2O3– 簇（M = Ta、V 和 Al）催化的 NO 选择性还原成 N2：三原子路易斯酸–碱–酸 Mδ+–Rhδ––Mδ+ 位点的重要性


由于排放法规日益严格，通过 CO 催化 NO 还原为 N₂ 和 CO₂ 势在必行。确定控制 NO 还原反应性和选择性的活性位点的性质对于定制催化剂至关重要，但由于实际系统的复杂性，这极具挑战性。在我们新发现的三原子路易斯酸-碱酸 （LABA， Ce^δ+–Rh^δ−–Ce^δ+） 位点的指导下，该位点解释了气相实验中 RhCe₂O₃^– 催化 NO 转化为 N₂ 的原因，探索了 RhM₂O₃^– （M = Ta、V 和 Al） 簇在 CO 催化还原 NO 中的反应性。我们从理论上确定 LABA 位点仍然盛行，将 NO 还原为 N₂，由 RhTa₂O₃^– 和 RhV₂O₃^– 介导，强调强 M-氧亲和力来构建 LABA 位点。总体评估强调，RhV₂O₃^– 是一种更有前途的催化剂，因为拟合良好的 V-O 键合强度促进了 NO 还原和 CO 氧化的基本反应。