<img src="Edit_bdc7d851-e537-40df-990c-d678defa9648.png" alt="" />(M = Au, Ag, Cu;<span lang="EN-US" style="font-size:9pt;font-family:"color:black;"><i>n&...<img src="Edit_bdc7d851-e537-40df-990c-d678defa9648.png" alt="" />(M = Au, Ag, Cu;<span lang="EN-US" style="font-size:9pt;font-family:"color:black;"><i>n</i></span>= 1, 2, 3) clusters were used as a cluster model to study the activation of oxygen molecules on single-atom catalysts. Structures of <img src="Edit_bb84deb7-e24a-4777-a2f6-a1621ddd2afc.png" alt="" /> clusters were studied by density functional calculations with global optimization. For each <span style="font-family:"color:black;white-space:normal;"><i>n</i></span>, the most stable structures are quite similar for different metal types, and the oxygen molecule prefers to be adsorbed onto M atoms. It is found that the activation degree of oxygen is higher on clusters with non-noble metal Cu than that of Ag or Au containing clusters, by comparing the changes of O-O bond length and vibrational frequency, natural charge population analysis, Fuzzy bond order analysis, and energy barriers of O<sub>2</sub> dissociation. CO oxidation was used as a probe reaction to study the reactivity of Cu-containing clusters, and it is found that the reactivity decreases with the increase of the size of silicon-oxygen clusters. Our results give a new aspect to understand the reaction mechanism of non-precious metal single-atom catalyst for oxygen activation with high efficiency.展开更多
文摘<img src="Edit_bdc7d851-e537-40df-990c-d678defa9648.png" alt="" />(M = Au, Ag, Cu;<span lang="EN-US" style="font-size:9pt;font-family:"color:black;"><i>n</i></span>= 1, 2, 3) clusters were used as a cluster model to study the activation of oxygen molecules on single-atom catalysts. Structures of <img src="Edit_bb84deb7-e24a-4777-a2f6-a1621ddd2afc.png" alt="" /> clusters were studied by density functional calculations with global optimization. For each <span style="font-family:"color:black;white-space:normal;"><i>n</i></span>, the most stable structures are quite similar for different metal types, and the oxygen molecule prefers to be adsorbed onto M atoms. It is found that the activation degree of oxygen is higher on clusters with non-noble metal Cu than that of Ag or Au containing clusters, by comparing the changes of O-O bond length and vibrational frequency, natural charge population analysis, Fuzzy bond order analysis, and energy barriers of O<sub>2</sub> dissociation. CO oxidation was used as a probe reaction to study the reactivity of Cu-containing clusters, and it is found that the reactivity decreases with the increase of the size of silicon-oxygen clusters. Our results give a new aspect to understand the reaction mechanism of non-precious metal single-atom catalyst for oxygen activation with high efficiency.
