MOF-808中Pt团簇稳定性的密度泛函理论研究,Physical Chemistry Chemical Physics

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MOF-808中Pt团簇稳定性的密度泛函理论研究
Physical Chemistry Chemical Physics ( IF 2.9 ) Pub Date : 2020-09-28 , DOI: 10.1039/d0cp04444j
Xiaohui Song _{1,

2,

3,

4} , Donghai Mei _{1,

2,

3,

4}

Affiliation

由于金属团簇的几何和电子性质，金属有机骨架（MOF）封装的金属团簇已显示出优异的催化活性，这在很大程度上取决于吸附位点以及封装的金属团簇的大小和形态。在目前的工作中，使用密度泛函理论计算和从头算分子动力学模拟研究了MOF-808框架结构上Pt _n（n = 1-23）簇的锚定位，稳定性和团聚概率。已经发现，Pt _n（n = 1–7）团簇在Zr ₆处的结合更牢固金属节点站点比在接口站点和链接器站点要多。吸附后，大量电子（+0.92至+1.96 | e |）从Pt _n团簇转移至MOF骨架。在Zr ₆金属节点上单个Pt ₁原子的团聚不可能形成Pt _n簇，而在界面或连接体上的团聚在能量上是可行的。与单个Zr ₆节点相比，Pt _n簇与两个Zr ₆金属节点的键合更弱，电子更少（+0.12至+0.89 | e|）转移。最后，我们的计算表明，在单个Pt原子上的CO吸附在界面处稳定，从而防止了它与两个Zr ₆金属节点之间的Pt _n团簇进一步聚集。

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A density functional theoretical study on the stability of Pt clusters in MOF-808

Metal organic framework (MOF)-encapsulated metal clusters have shown superior catalytic activity due to geometric and electronic properties of metal clusters, which are largely determined by adsorption sites and sizes and morphologies of encapsulated metal clusters. In the present work, anchoring sites, the stability, and the agglomeration probability of Pt_n (n = 1–23) clusters over an MOF-808 framework structure were studied using density functional theory calculations and ab initio molecular dynamics simulation. It has been found that Pt_n (n = 1–7) clusters bind more strongly at the Zr₆ metal node sites than at the interface and linker sites. Upon adsorption, significant amounts of electrons (+0.92 to +1.96 |e|) are transferred from Pt_n clusters to the MOF framework. The agglomeration of single Pt₁ atoms at the Zr₆ metal node to form a Pt_n cluster is unlikely, while the agglomeration at the interface or the linker is energetically feasible. Compared with the single Zr₆ node, the bonding of Pt_n clusters with two Zr₆ metal nodes is weaker, with less electron (+0.12 to +0.89 |e|) transfer. Finally, our calculations show that CO adsorption at the single Pt atom is stabilized at the interface site, preventing its further agglomeration with Pt_n clusters between the two Zr₆ metal nodes.

更新日期：2020-10-15

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