C–H Bond Activation on Bimetallic Two-Atom Co-M Oxide Clusters Deposited on Zr-Based MOF Nodes: Effects of Doping at the Molecular Level,ACS Catalysis

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C–H Bond Activation on Bimetallic Two-Atom Co-M Oxide Clusters Deposited on Zr-Based MOF Nodes: Effects of Doping at the Molecular Level
ACS Catalysis ( IF 11.3 ) Pub Date : 2018-02-22 00:00:00 , DOI: 10.1021/acscatal.8b00012
Matthew C. Simons _{1,

2} , Manuel A. Ortuño ₂ , Varinia Bernales ₂ , Carlo Alberto Gaggioli ₂ , Christopher J. Cramer ₂ , Aditya Bhan ₁ , Laura Gagliardi ₂

Affiliation

Cluster-based density functional theory calculations show that energy barriers for the dissociative adsorption of propane on two-cation, Co-M oxide clusters supported on Zr-based nodes of NU-1000, a metal–organic framework material, vary from 57 to 9 kcal mol^–1 based on the identity of the dopant. Systematic changes in spin density and positive partial charge on oxygen atoms bridging the two metal atoms (Co–O-M) are noted upon addition of dopants to cobalt, with increasing values of both giving lower enthalpic barriers to C–H scission. These observed correlations can be rationalized in terms of concepts applicable to bulk systems and provide target materials for synthesis.

中文翻译：

基于Zr的MOF节点上沉积的双金属双原子Co-M氧化物簇上的C–H键活化：在分子水平上掺杂的影响

基于簇的密度泛函理论计算表明，金属-有机骨架材料NU-1000的Zr基节点上支撑的丙烷在两个阳离子，Co-M氧化物簇上的解离吸附能垒从57变为9 kcal mol ^–1基于掺杂剂的身份。在钴中添加掺杂剂后，会注意到自旋密度和桥接两个金属原子的氧原子上的正部分电荷的系统变化（钴-OM），两者的值都增加，则对C-H分裂产生较低的焓垒。可以根据适用于整体系统的概念合理化这些观察到的相关性，并为合成提供目标材料。

更新日期：2018-02-22

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