title: In-Situ Platinum Deposition on Nitrogen-Doped Carbon Films as a Source of Catalytic Activity in a Hydrogen Evolution Reaction.
abstract: Copolymer-templated nitrogen-doped carbon (CTNC) films deposited on glassy carbon were used as electrodes to study electrochemically driven hydrogen evolution reaction (HER) in 0.5 M H2SO4. The activity of these materials was extremely enhanced when a platinum counter electrode was used instead of a graphite rod and reached the level of commercial Pt/C electrodes. Postreaction scanning electron microscopy (SEM) and X-ray photoelectron spectroscopy (XPS) measurements of electrode surfaces revealed that incorporation of even extremely low amounts of Pt resulted in this considerable gain of HER activity. High resolution XPS analysis and density functional theory (DFT) calculations confirmed that pyridinic nitrogen atoms act as active sites for Pt coordination and deposition. The Pt can be incorporated in both molecular (Pt(2+)) and metallic (Pt(0)) form. This study shows that great caution must be taken when designing "metal-free" HER catalysts based on N-doped carbons.
authors.affiliation: Department of Chemistry, Center for Macromolecular Engineering, Carnegie Mellon University , Pittsburgh, Pennsylvania 15213, United States.
authors.forename: Eric
authors.initials: E
authors.lastname: Gottlieb
authors.affiliation: Department of Chemistry, Center for Macromolecular Engineering, Carnegie Mellon University , Pittsburgh, Pennsylvania 15213, United States.
authors.forename: Maciej
authors.initials: M
authors.lastname: Kopeć
authors.affiliation: Department of Chemistry, Center for Macromolecular Engineering, Carnegie Mellon University , Pittsburgh, Pennsylvania 15213, United States.
authors.forename: Manali
authors.initials: M
authors.lastname: Banerjee
authors.affiliation: Department of Chemistry, Center for Macromolecular Engineering, Carnegie Mellon University , Pittsburgh, Pennsylvania 15213, United States.
authors.forename: Jacob
authors.initials: J
authors.lastname: Mohin
authors.affiliation: Department of Chemistry, Center for Macromolecular Engineering, Carnegie Mellon University , Pittsburgh, Pennsylvania 15213, United States.
authors.forename: David
authors.initials: D
authors.lastname: Yaron
authors.affiliation: Department of Chemistry, Center for Macromolecular Engineering, Carnegie Mellon University , Pittsburgh, Pennsylvania 15213, United States.
authors.forename: Krzysztof
authors.initials: K
authors.lastname: Matyjaszewski
authors.affiliation: Department of Chemistry, Center for Macromolecular Engineering, Carnegie Mellon University , Pittsburgh, Pennsylvania 15213, United States.
authors.forename: Tomasz
authors.initials: T
authors.lastname: Kowalewski
keywords: N-doped carbon; block copolymers; electrocatalysis; hydrogen evolution; platinum nanoparticles