Investigations of Hydrocarbon Species on Solid Catalysts by Inelastic Neutron Scattering
Investigations of Hydrocarbon Species on Solid Catalysts by Inelastic Neutron Scattering
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DOI：
10.1007/s11244-020-01389-7
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发表时间：
2020-10
影响因子：
3.6
通讯作者：
Longfei Lin;Q. Mei;Xue Han;S. Parker;Sihai Yang
中科院分区：
文献类型：
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作者：
Longfei Lin;Q. Mei;Xue Han;S. Parker;Sihai Yang
多相催化过程中固体催化剂表面物种的状态通常是神秘的。对这些表面物种的研究对于解卷积反应网络和设计更有效的催化剂至关重要。振动光谱是研究表面物种与催化剂之间相互作用的强大技术，红外（IR）和拉曼光谱已广泛应用于研究多相催化中的反应机制。然而，红外/拉曼光谱很难通过计算建模，并且由于光学选择规则的限制，重要的振动模式可能是红外、拉曼（或两者）不活跃。非弹性中子散射（INS）是振动光谱的另一种形式，依赖于原子核对中子的散射。这样做的结果是 INS 不受任何光学选择规则的约束，并且原则上所有振动都是可测量的。 INS 光谱已用于研究各种非均相催化反应中催化剂的表面物质。在这篇小综述中，我们重点关注 INS 在两个重要领域的应用：石油化学反应和 C1 化学。我们介绍了 INS 技术的基本原理，然后讨论了其在研究两个关键催化系统中的应用：（i）碳氢化合物在金属氧化物和沸石催化剂上的行为以及（ii）在甲烷重整和费托催化剂上烃类物质的形成。 INS 在研究这些重要催化系统方面的能力得到了证明。
The status of surface species on solid catalysts during heterogeneous catalysis is often mysterious. Investigations of these surface species are crucial to deconvolute the reaction network and design more efficient catalysts. Vibrational spectroscopy is a powerful technique to study the interactions between surface species and the catalysts and infrared (IR) and Raman spectroscopies have been widely applied to study reaction mechanisms in heterogeneous catalysis. However, IR/Raman spectra are difficult to model computationally and important vibrational modes may be IR-, Raman- (or both) inactive due to restrictions by optical selection rules. Inelastic neutron scattering (INS) is another form of vibrational spectroscopy and relies on the scattering of neutrons by the atomic nucleus. A consequence of this is that INS is not subject to any optical selection rules and all vibrations are measurable in principle. INS spectroscopy has been used to investigate surface species on catalysts in a wide range of heterogeneous catalytic reactions. In this mini-review, we focus on applications of INS in two important fields: petrochemical reactions and C1 chemistry. We introduce the basic principles of the INS technique, followed by a discussion of its application in investigating two key catalytic systems: (i) the behaviour of hydrocarbons on metal-oxide and zeolite catalysts and (ii) the formation of hydrocarbonaceous species on methane reforming and Fischer–Tropsch catalysts. The power of INS in studying these important catalytic systems is demonstrated.