Visualizing the enhanced chemical reactivity of mesoporous ceria; simulating templated crystallization in silica scaffolds at the atomic level.
Visualizing the enhanced chemical reactivity of mesoporous ceria; simulating templated crystallization in silica scaffolds at the atomic level.
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DOI：
10.1021/ja500443m
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发表时间：
2014-02
影响因子：
15
通讯作者：
T. Sayle;D. Sayle
中科院分区：
文献类型：
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作者：
T. Sayle;D. Sayle
通过结构控制可以将独特的物理、化学和机械特性设计成功能性纳米材料。然而，随着纳米材料层次结构复杂性的增加，与生成原子模型相关的挑战也随之增加，这些模型足够现实，可以可靠地预测属性和过程。功能纳米材料的结构复杂性必然在合成过程中体现出来。因此，为了捕捉这种复杂性，我们模拟了合成方案中的每个步骤。具体来说，通过模拟介孔二氧化硅支架中二氧化铈的灌注和限制结晶，生成了介孔二氧化铈的原子模型。去除支架后，计算了模板化介孔二氧化铈的化学反应性，并预测其与没有模板生成的介孔二氧化铈相比具有更高的反应性；呈现视觉“反应指纹”。该策略提供了一种生成具有层次结构复杂性的原子模型的通用方法，可用于预测各种特性和过程，从而实现功能材料的纳米级设计。
Unique physical, chemical, and mechanical properties can be engineered into functional nanomaterials via structural control. However, as the hierarchical structural complexity of a nanomaterial increases, so do the challenges associated with generating atomistic models, which are sufficiently realistic that they can be interrogated to reliably predict properties and processes. The structural complexity of a functional nanomaterial necessarily emanates during synthesis. Accordingly, to capture such complexity, we have simulated each step in the synthetic protocol. Specifically, atomistic models of mesoporous ceria were generated by simulating the infusion and confined crystallization of ceria in a mesoporous silica scaffold. After removing the scaffold, the chemical reactivity of the templated mesoporous ceria was calculated and predicted to be more reactive compared to mesoporous ceria generated without template; visual "reactivity fingerprints" are presented. The strategy affords a general method for generating atomistic models, with hierarchical structural complexity, which can be used to predict a variety of properties and processes enabling the nanoscale design of functional materials.