TY - JOUR
T1 - Quantum-continuum simulation of underpotential deposition at electrified metal-solution interfaces
AU - Weitzner, Stephen E.
AU - Dabo, Ismaila
N1 - Funding Information:
1Department of Materials Science and Engineering, Materials Research Institute, and Penn State Institutes of Energy and the Environment, The Pennsylvania State University, University Park, PA 16802, USA Correspondence: Stephen E. Weitzner ([email protected])
Funding Information:
This work was funded by the Soltis Faculty Support Gift, the Ralph E. Powe Junior Faculty Award from Oak Ridge Associated Universities, and by the Center for Dielectrics and Piezoelectrics at Penn State University. We thank the Penn State Institute for CyberScience for providing high-performance computing resources and technical support throughout this work.
Publisher Copyright:
© 2017 The Author(s).
PY - 2017/12/1
Y1 - 2017/12/1
N2 - The underpotential deposition of transition metal ions is a critical step in many electrosynthetic approaches. While underpotential deposition has been intensively studied at the atomic level, first-principles calculations in vacuum can strongly underestimate the stability of underpotentially deposited metals. It has been shown recently that the consideration of co-adsorbed anions can deliver more reliable descriptions of underpotential deposition reactions; however, the influence of additional key environmental factors such as the electrification of the interface under applied voltage and the activities of the ions in solution have yet to be investigated. In this work, copper underpotential deposition on gold is studied under realistic electrochemical conditions using a quantum-continuum model of the electrochemical interface. We report here on the influence of surface electrification, concentration effects, and anion co-adsorption on the stability of the copper underpotential deposition layer on the gold (100) surface.
AB - The underpotential deposition of transition metal ions is a critical step in many electrosynthetic approaches. While underpotential deposition has been intensively studied at the atomic level, first-principles calculations in vacuum can strongly underestimate the stability of underpotentially deposited metals. It has been shown recently that the consideration of co-adsorbed anions can deliver more reliable descriptions of underpotential deposition reactions; however, the influence of additional key environmental factors such as the electrification of the interface under applied voltage and the activities of the ions in solution have yet to be investigated. In this work, copper underpotential deposition on gold is studied under realistic electrochemical conditions using a quantum-continuum model of the electrochemical interface. We report here on the influence of surface electrification, concentration effects, and anion co-adsorption on the stability of the copper underpotential deposition layer on the gold (100) surface.
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U2 - 10.1038/s41524-016-0004-9
DO - 10.1038/s41524-016-0004-9
M3 - Article
AN - SCOPUS:85015897698
SN - 2057-3960
VL - 3
JO - npj Computational Materials
JF - npj Computational Materials
IS - 1
M1 - 1
ER -