Nature of the N-Pd interaction in nitrogen-doped carbon nanotube catalysts

By Rosa Arrigo, M. Schuster, Zailai Xie, Youngmi Yi, G. Wowsnick, Lili Sun, K. Hermann, M. Friedrich, P. Kast, M. Hävecker and 2 more. 2015

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In this work, the geometric and electronic structure of N species in N-doped carbon nanotubes (NCNTs) is derived by X-ray photoemission (XPS) and absorption spectroscopy (NEXAFS) of the N 1s core excitation. Substitutional N species in pyridine-like configuration and another form of N with higher thermal stability are found in NCNTs. The structural configuration of the high thermally stable N species, in the literature often referred to as graphitic N, is assessed in this work by a combined theoretical and experimental study as a 3-fold substitutional N species in an NCNT basic structural unit (BSU). Furthermore, the nature of the interaction of those N species with a Pd metal center immobilized onto NCNTs is of σ-type donation from the filled π-orbital of the N atom to the empty d-orbital of the Pd atom and a π back-donation from the filled Pd atomic d-orbital to the π* antibonding orbital of the N atom. We have found that the interaction of pyridine N with Pd is characterized by a charge transfer typica...

Subfields: Electrical and Electronic Engineering, Materials Chemistry, Renewable Energy, Sustainability and the Environment

View Paper: https://www.semanticscholar.org/paper/52efd18006db4c32c9f45cc1db7048eb74e140c8