Dehydration Pathway for the Dissociation of Gas-Phase Formic Acid on Pt(111) Surface Observed via Ambient-Pressure XPS

Beomgyun Jeong, Hongrae Jeon, Ryo Toyoshima, Ethan J. Crumlin, Hiroshi Kondoh, Bongjin Simon Mun, Jaeyoung Lee

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4 Citations (Scopus)

Abstract

While model studies of surface science under ultrahigh vacuum (UHV) have made significant contributions to understanding electrochemistry, many issues related to electrochemical phenomena still remain unanswered due to the extreme environmental differences between UHV and liquid conditions. Electrochemical formic acid (HCOOH) oxidation is one such example. While the dehydration step in the indirect oxidation pathway (HCOOH → H2O + COad → 2H+ + 2e- + CO2) is observed in the electrochemical oxidation of formic acid on Pt(111) surface, the surface science studies conducted in UHV condition reported the complete HCOOH dissociation to H2 and CO2 on Pt(111) surface with no adsorbed CO at room temperature. A dehydration mechanism may also exist in gas-phase HCOOH dissociation in some conditions different from UHV, but it has not been demonstrated with a surface science method due to pressure limitations. Using ambient pressure X-ray photoelectron spectroscopy (AP-XPS), we observed the dehydration mechanism of gas-phase HCOOH in unprecedented high pressure environment for the first time. This study is a demonstration of reconciling the disagreement between electrocatalysis and surface science by bridging the environment gap.

Original languageEnglish
Pages (from-to)2064-2069
Number of pages6
JournalJournal of Physical Chemistry C
Volume122
Issue number4
DOIs
Publication statusPublished - 2018 Feb 1

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ASJC Scopus subject areas

  • Electronic, Optical and Magnetic Materials
  • Energy(all)
  • Physical and Theoretical Chemistry
  • Surfaces, Coatings and Films

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