碳纳米管生长过程中过渡表面碳化铂的形成

IF 10.5 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Carbon Pub Date : 2024-06-26 DOI:10.1016/j.carbon.2024.119399
Hannah C. Nerl , Christian S. Ahart , Alberto Eljarrat , Christoph T. Koch , Clotilde S. Cucinotta , Milivoj Plodinec
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引用次数: 0

摘要

通过将结构信息与催化活性联系起来,可以确定催化剂的活性结构。然而,这远非一蹴而就,即使是在使用贵金属催化剂(如铂(Pt))进行的石墨碳形成反应中,活性结构也仍然存在争议。一个主要障碍是静态观察无法获得催化剂的过渡状态。在此,我们利用原子分辨率气体原位透射电子显微镜并结合密度泛函理论,证明了在碳纳米管的生长过程中形成了深达数层的过渡表面碳化铂以及铂-碳复合相。由于贵金属铂在异质催化中的应用,了解贵金属铂的活性结构具有重大意义。最重要的是,它为抑制催化剂结焦开辟了新途径。在包括丙烷脱氢在内的重要工业反应中,不必要的积碳是催化剂失活的主要原因,会对经济和环境造成重大影响。
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Transitional surface Pt carbide formation during carbon nanotube growth

By correlating structural information with catalytic activity, it is possible to determine the active structure of a catalyst. However, this is far from straightforward and the active structure remains debated even in the well-studied reaction of graphitic carbon formation using noble metal catalysts such as platinum (Pt). One major hindrance is that static observations do not provide access to transitional catalyst states. Here we prove the formation of transitional surface Pt carbide several layers deep as well as a Pt-carbon composite phase during the growth process of carbon nanotubes using atomic-resolution gas in situ transmission electron microscopy combined with density functional theory. Knowledge of the active structure of noble metal Pt is of great interest due to its usage in heterogeneous catalysis. Most importantly, it opens up new avenues to suppress catalyst coking. The unwanted build-up of carbon is the major source of catalyst deactivation in important industrial reactions including propane dehydrogenation, with major financial and environmental consequences.

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来源期刊
Carbon
Carbon 工程技术-材料科学:综合
CiteScore
20.80
自引率
7.30%
发文量
0
审稿时长
23 days
期刊介绍: The journal Carbon is an international multidisciplinary forum for communicating scientific advances in the field of carbon materials. It reports new findings related to the formation, structure, properties, behaviors, and technological applications of carbons. Carbons are a broad class of ordered or disordered solid phases composed primarily of elemental carbon, including but not limited to carbon black, carbon fibers and filaments, carbon nanotubes, diamond and diamond-like carbon, fullerenes, glassy carbon, graphite, graphene, graphene-oxide, porous carbons, pyrolytic carbon, and other sp2 and non-sp2 hybridized carbon systems. Carbon is the companion title to the open access journal Carbon Trends. Relevant application areas for carbon materials include biology and medicine, catalysis, electronic, optoelectronic, spintronic, high-frequency, and photonic devices, energy storage and conversion systems, environmental applications and water treatment, smart materials and systems, and structural and thermal applications.
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