TY - JOUR
T1 - Dehydration Pathway for the Dissociation of Gas-Phase Formic Acid on Pt(111) Surface Observed via Ambient-Pressure XPS
AU - Jeong, Beomgyun
AU - Jeon, Hongrae
AU - Toyoshima, Ryo
AU - Crumlin, Ethan J.
AU - Kondoh, Hiroshi
AU - Mun, Bongjin Simon
AU - Lee, Jaeyoung
N1 - Funding Information:
The authors are grateful to Dr. Toru Shimada for his valuable help during the course of the experiment at Photon Factory, KEK. This work was supported by the GIST Research Institute (GRI) in 2017. B.S.M. would like to acknowledge the support from the SRC (C-AXS, NRF-2015R1A5A1009962) and a Korea Basic Science Institute Grant (E36800). This research used resources of the Advanced Light Source, which is a DOE Office of Science User Facility under Contract No. DE-AC02- 05CH11231. The experiments were performed under the approval of the Photon Factory Program Advisory Committee (PF PAC No. 2012S2-006).
Funding Information:
The authors are grateful to Dr. Toru Shimada for his valuable help during the course of the experiment at Photon Factory, KEK. This work was supported by the GIST Research Institute (GRI) in 2017. B.S.M. would like to acknowledge the support from the SRC (C-AXS, NRF-2015R1A5A1009962) and a Korea Basic Science Institute Grant (E36800). This research used resources of the Advanced Light Source, which is a DOE Office of Science User Facility under Contract No. DE-AC02-05CH11231. The experiments were performed under the approval of the Photon Factory Program Advisory Committee (PF PAC No. 2012S2-006).
PY - 2018/2/1
Y1 - 2018/2/1
N2 - 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.
AB - 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.
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U2 - 10.1021/acs.jpcc.7b07735
DO - 10.1021/acs.jpcc.7b07735
M3 - Article
AN - SCOPUS:85041437081
SN - 1932-7447
VL - 122
SP - 2064
EP - 2069
JO - Journal of Physical Chemistry C
JF - Journal of Physical Chemistry C
IS - 4
ER -