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Surface Hydride Formation on Cu(111) and its Decomposition to Form H2 in Acid Electrolytes

Published

Author(s)

David Raciti, Thomas P. Moffat, Angela R. Hight Walker, Brian Tackett

Abstract

Mass spectrometry and Raman vibrational spectroscopy were used to follow competitive dynamics between adsorption and desorption of H and anions during potential cycling of three low index Cu surfaces in acid electrolytes. Unique to Cu(111) is a redox wave for surface hydride formation coincident with anion desorption, while the reverse reaction of hydride decomposition with anion adsorption yields H2 by recombination rather than oxidation to H3O+. Charge imbalance between the reactions account for the asymmetric voltammetry in SO42-, ClO4-, PO43-, and Cl- electrolytes with pH 0.68 to 4.5. Two-dimensional hydride formation is evidenced by the reduction wave prior to H2 evolution and vibrational bands between 995 cm-1 and 1130 cm-1. In contrast to Cu(111), no distinct voltammetric signature of surface hydride formation is observed on Cu(110) and Cu(100). The Cu(111) hydride surface phase catalyzes hydrofunctionalization reactions such as CO2 reduction to CH4 and should be broadly useful in electro-organic synthesis.
Citation
Journal of Physical Chemistry Letters

Keywords

Electrochemical Mass Spectrometry, Surface Enhanced Raman Spectroscopy, SHINERS, Anion Adsorption, Hydrogen Adsorption and Absorption, Copper Hydride, Copper Single Crystal

Citation

Raciti, D. , Moffat, T. , Hight Walker, A. and Tackett, B. (2021), Surface Hydride Formation on Cu(111) and its Decomposition to Form H2 in Acid Electrolytes, Journal of Physical Chemistry Letters, [online], https://tsapps.nist.gov/publication/get_pdf.cfm?pub_id=933233 (Accessed December 7, 2022)
Created November 4, 2021, Updated November 29, 2022