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Probing the electronic effect of carbon nanotubes in catalysis: NH _3 synthesis with Ru nanoparticles

机译：探索碳纳米管在催化中的电子效应：Ru纳米粒子合成NH _3

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摘要

Carbon nanotubes (CNTs) have been shown to modify some properties of nanomaterials and to modify chemical reactions confined inside their channels, which are formed by curved graphene layers. Here we studied ammonia synthesis over Ru as a probe reaction to understand the effect of the electron structure of CNTs on the confined metal particles and their catalytic activity. The catalyst with Ru nanoparticles dispersed almost exclusively on the exterior nanotube surface exhibits a higher activity than the CNT-confined Ru, although both have a similar metal particle size. Characterization with TEM, N _2 physisorption, H_2 chemisorption, temperature-pro-grammed reduction, CO adsorption microcalorimetry, and first-principles calculations suggests that the outside Ru exhibits a higher electron density than the inside Ru. As a result, the dissociative adsorption of N_2, which is an electrophilic process and the rate-determining step of ammonia synthesis, is more facile over the outside Ru than that over the inside one.
机译：碳纳米管（CNT）已被证明可以改变纳米材料的某些特性，并可以改变其通道内部的化学反应，这些化学反应是由弯曲的石墨烯层形成的。在这里，我们研究了Ru上的氨合成作为探针反应，以了解CNTs的电子结构对受限金属颗粒及其催化活性的影响。具有Ru纳米颗粒的催化剂几乎仅分散在纳米管的外部表面上，但其活性比CNT限制的Ru高，尽管两者的金属粒径相似。用TEM表征，N _2物理吸附，H_2化学吸附，程序升温还原，CO吸附微量量热法和第一性原理计算表明，外部Ru的电子密度高于内部Ru。结果，N 2的解离吸附是亲电过程和氨合成的速率决定步骤，它比外部Ru容易吸附在外部Ru上。

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