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论文类型： 期刊论文

发表时间： 2010-05-10

发表刊物： CHEMISTRY-A EUROPEAN JOURNAL

收录刊物： SCIE、EI

卷号： 16

期号： 18

页面范围： 5379-5384

ISSN号： 0947-6539

关键字： ammonia; calorimetry; carbon nanotubes; confinement; ruthenium

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-programmed 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.