Molecular approaches to heterogeneous catalysis
Molecular approaches to heterogeneous catalysis
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DOI：
10.1016/j.ccr.2021.214179
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发表时间：
2021-12
影响因子：
20.6
通讯作者：
F. Zaera
中科院分区：
文献类型：
--
作者：
F. Zaera
在涉及催化的工业中的大多数应用中，当可用时，非均相催化剂优于其均相对应物。然而，不能容易地使前者对复杂的化学转化具有像后者那样的选择性。选择性需要在分子水平上控制催化位点的结构和电子性质，而这通常在固体中很难实现。尽管如此，近年来已经朝着这一目标提出了一些新的方法。在这个简短的观点中，我们提供了一些可用于制造高选择性多相催化剂的途径的个人观点。首先，我们讨论了在固体表面上系留或以其他方式固定均相催化剂的可能性。或者，分子复杂性可以通过离散改性剂的吸附添加到固体表面。在多相催化剂的合成过程中或之后，也可以产生具有独特分子特征的孤立催化位点。固体的暴露面的结构本身可以用来控制催化性能。最后，可以合成复杂的纳米结构，如Janus和核壳纳米颗粒，并用作多种催化功能的支架。所有这些方法，主要是从我们自己的实验室，提供了一些例子，并提供了每种方法的利弊的讨论。
In most applications in industry involving catalysis, heterogeneous catalysts are preferred over their homogeneous counterparts when available. However, the former cannot be easily made as selective for complex chemical conversions as the latter. Selectivity requires control of the structural and electronic properties of the catalytic sites at a molecular level, and that is in general quite difficult to accomplish in solids. Nevertheless, a number of novel approaches have been advanced in recent years toward that goal. In this brief Perspective we provide a personal view of some of the avenues available to make highly selective heterogeneous catalysts. First, we discuss the possibility of tethering or otherwise immobilizing homogeneous catalysts on solid surfaces. Alternatively, molecular complexity can be added to solid surfaces via the adsorption of discrete modifiers. Isolated catalytic sites with unique molecular characteristics can also be created during or after the synthesis of heterogeneous catalysts. The structure of the exposed facets of solids can themselves be exploited to control catalytic performance. Finally, complex nanostructures such as Janus and core-shell nanoparticles can be synthesized and employed as scaffolds for multiple catalytic functionalities. A few examples of all of these methodologies, mainly from our own laboratory, are provided, and a discussion of the pros and cons of each approach is provided.