open access

https://hdl.handle.net/2115/79353

Oxygen Reduction Reaction Catalyzed by Self-Assembled Monolayers of Copper-Based Electrocatalysts on a Polycrystalline Gold Surface

英語

sum frequency generation spectroscopy

2016-07-28

American Chemical Society

The Journal of Physical Chemistry C

120(29)

15814-15822

We report two-dimensional model systems to study the electrocatalytic activities of dinuclear copper complexes for various electrocatalytic reactions including the oxygen reduction reaction (ORR), where we can use electrochemical techniques as well as surface-sensitive techniques such as X-ray photoelectron spectroscopy and vibrational sum frequency generation spectroscopy. Heteroaromatic thiols, including four triazoles and a thiadiazole, are used as metal ligands as well as anchors to a polycrystalline gold electrode. The thiols are self-assembled on the polycrystalline gold electrode and then react with copper(II) ions to give monolayers of copper-based ORR catalysts on the surface. The dinuclear copper complexes of 1,2,4-triazole-3-thiol and 3-amino-1,2,4-triazole-5-thiol show ORR activity and pH-dependent catalytic behavior similar to that of counterparts supported on carbon black, suggesting that our two-dimensional systems can serve as model catalysts for carbon-supported molecular catalysts. We have also self-assembled dinuclear copper complexes with long alkyl or perfluoroalkyl chains on the surface and studied their orientation on the surface and oxygen transport.

学術雑誌論文

Accepted Manuscript

This document is the Accepted Manuscript version of a Published Work that appeared in final form in Journal of Physical Chemistry C, copyright c American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://pubs.acs.org/doi/10.1021/acs.jpcc.5b11663.

1932-7447

1932-7455

AA1217589X