Grafting metal complexes onto amorphous supports: from elementary steps to catalyst site populations via kernel regression,Reaction Chemistry & Engineering

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Grafting metal complexes onto amorphous supports: from elementary steps to catalyst site populations via kernel regression
Reaction Chemistry & Engineering ( IF 3.4 ) Pub Date : 2019-10-31 , DOI: 10.1039/c9re00357f
Salman A. Khan _{1,

2,

3,

4} , Craig A. Vandervelden _{1,

2,

3,

4} , Susannah L. Scott _{1,

2,

3,

4,

5} , Baron Peters _{4,

6,

7,

8,

9}

Affiliation

Ab initio computational studies have made tremendous progress in describing the behavior of molecular (homogeneous) catalysts and crystalline versions of heterogeneous catalysts, but not for amorphous heterogeneous catalysts. Even widely used industrial amorphous catalysts like atomically dispersed Cr on silica remain poorly understood and largely intractable to computational investigation. The central problems are that (i) the amorphous support presents an unknown quenched disordered structure, (ii) metal atoms attach to various surface grafting sites with different rates, and (iii) the resulting grafted sites have different activation and catalytic reaction kinetics. This study combines kernel regression and importance sampling techniques to efficiently model grafting of metal ions onto a non-uniform ensemble of support environments. Our analysis uses a simple model of the quenched disordered support environment, grafting chemistry, and catalytic activity of the resulting grafted sites.

中文翻译：

将金属络合物接枝到无定形载体上：通过核回归从基本步骤到催化剂位点填充

从头算计算研究在描述分子（均相）催化剂和非均相催化剂的结晶形式的行为方面取得了巨大进展，但对于非晶非均相催化剂却没有。即使广泛使用的工业无定形催化剂，例如原子分散在二氧化硅上的Cr仍知之甚少，并且在计算研究中非常棘手。中心问题是（i）无定形载体呈现未知的淬灭无序结构，（ii）金属原子以不同的速率连接到各种表面接枝位点，并且（iii）所得的接枝位点具有不同的活化和催化反应动力学。这项研究结合了内核回归和重要性采样技术，可以有效地将金属离子的接枝建模到支持环境的非均匀整体上。

更新日期：2019-10-31

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