Photocatalytic Reduction of CO2 to CO in 100%: The Synergistic Effect of Nickel and Europiumin Heterometallic Clusters.

Kaipeng Bai, Wei-Peng Chen, Meng-Di Cui, Yan-Zhen Zheng
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Abstract

Heterometallic transition-rare earth metal (3d-4f) clusters with synergestic catalytic activity are rarely identified. Herein, two families of closely related 3d-Eu clusters were designed to analyze the role of Eu(III) ions during the photocatalytic reduction of CO2 into CO. The [M24Eu8] family, where M = Co or Ni, shows much lower activity (CO production < 2078 μmol g-1 h-1) compared to the [M24Eu10] family (CO production > 5838 μmol g-1 h-1). This is due to the two additional Eu(III) ions in the apical position of the latter which are very active for converting CO2 into CO. Moreover, we found the nickel analogues are better than the cobalt ones, especially for [Ni24Eu10] which exhibits 100 % CO selectivity and very high efficacy of 6545.3 μmol g-1 h-1, while the [Co24Eu10] only shows 55 % CO selectivity. Therefore, the coexistence of both apical Eu(III) and Ni(II) ions has been experimentally revealed to be critical for this exceptional catalytic performance of the [Ni24Eu10] cluster. As such, this work unambiguously reveals a synergistic effect of bimetallic catalysts and may open a new avenue for more sophisticated reaction design by using the heterometallic coordination clusters.

光催化将CO2还原为100%的CO:镍和铕异金属团簇的协同作用。
具有协同催化活性的异金属过渡-稀土金属(3d-4f)簇很少被发现。本文设计了两个密切相关的3d-Eu簇族来分析Eu(III)离子在CO2光催化还原成CO过程中的作用。[M24Eu8]簇族,当M = CO或Ni时,其CO产率< 2078 μmol g-1 h-1),远低于[M24Eu10]簇族(CO产率> 5838 μmol g-1 h-1)。另外,我们发现镍的类似物优于钴的类似物,特别是[Ni24Eu10]具有100%的CO选择性和高达6545.3 μmol g-1 h-1的效率,而[Co24Eu10]只有55%的CO选择性。因此,实验表明,顶端Eu(III)和Ni(II)离子的共存对[Ni24Eu10]簇的特殊催化性能至关重要。因此,这项工作明确地揭示了双金属催化剂的协同效应,并可能通过使用异金属配位簇为更复杂的反应设计开辟新的途径。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
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