Assessing the Sensitivity of Pourbaix Diagrams to Computational Protocols: Electrochemical Stability of Ni Oxides as a Case Study

Sun, Wenyu; Govindarajan, Nitish; Prajapati, Aditya; Feaster, Jeremy T.; Hahn, Christopher; Akhade, Sneha A.

doi:10.1021/acs.jpcc.4c06788

Title: Assessing the Sensitivity of Pourbaix Diagrams to Computational Protocols: Electrochemical Stability of Ni Oxides as a Case Study

Journal Article · 08 December 2024 · Journal of Physical Chemistry. C

DOI: https://doi.org/10.1021/acs.jpcc.4c06788 · OSTI ID:2497915

^[1];

^[1]; Feaster, Jeremy T. ^[1];

^[1];

^[1]

Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States). Laboratory for Energy Applications for the Future (LEAF)

Pourbaix diagrams stand as a useful tool in assessing and visualizing materials’ electrochemical stability and are widely used for electrocatalyst design. However, their reliability hinges on the accuracy of the chemical potentials of involved phases, which may bear uncertainties and can be significantly impacted by decision-making steps in the computational protocol. Here, this study introduces a robust sensitivity analysis framework, exemplified through a detailed examination of the computational Pourbaix diagram of Ni, the oxides of which are used as high-activity and cost-friendly catalysts for many electrochemical reactions. Quantities of interest derived from the Pourbaix diagram include the appearance and stability domain of the catalytically active Ni oxide phases along with the onset electrochemical potentials of phase transitions. These metrics can guide the design of operational conditions for Ni oxide electrocatalysts. We find that the employed DFT exchange-correlation functional has the most significant influence on the computed Pourbaix diagram. Uncertainties on crystal structures, along with their related ab initio energetics, are also found to affect the size of the phase stability domain. Higher-order coupling among input parameters is found to play a crucial role in influencing the appearance and distribution of Ni phases in the diagram. Our findings suggest a need to consider variations and uncertainties associated with the computational procedures on predicted Pourbaix diagrams for materials design.

View Accepted Manuscript (DOE)

Cite

Export

Save

Research Organization:: Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)

Sponsoring Organization:: USDOE Laboratory Directed Research and Development (LDRD) Program; USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: AC52-07NA27344

OSTI ID:: 2497915

Report Number(s):: LLNL--JRNL-857211; 1087030

Journal Information:: Journal of Physical Chemistry. C, Journal Name: Journal of Physical Chemistry. C Journal Issue: 50 Vol. 128; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

References (62)

Redox Cycling of Ni-Based Solid Oxide Fuel Cell Anodes: A Review Sarantaridis, D.; Atkinson, A. Fuel Cells, Vol. 7, Issue 3 https://doi.org/10.1002/fuce.200600028	journal	June 2007
Continuous electrochemical oxidation of biomass derived 5-(hydroxymethyl)furfural into 2,5-furandicarboxylic acid Latsuzbaia, R.; Bisselink, R.; Anastasopol, A. Journal of Applied Electrochemistry, Vol. 48, Issue 6 https://doi.org/10.1007/s10800-018-1157-7	journal	February 2018
Making best use of model evaluations to compute sensitivity indices Saltelli, Andrea Computer Physics Communications, Vol. 145, Issue 2 https://doi.org/10.1016/S0010-4655(02)00280-1	journal	May 2002
Gibbs free energies of formation of RuO 2 , IrO 2 , and OsO 2 : A high-temperature electrochemical and calorimetric study O'Neill, Hugh St. C.; Nell, Johan Geochimica et Cosmochimica Acta, Vol. 61, Issue 24 https://doi.org/10.1016/S0016-7037(97)00317-7	journal	December 1997
Global sensitivity indices for nonlinear mathematical models and their Monte Carlo estimates Sobol′, I. M. Mathematics and Computers in Simulation, Vol. 55, Issue 1-3 https://doi.org/10.1016/S0378-4754(00)00270-6	journal	February 2001
Resolving Potential-Dependent Degradation of Electrodeposited Ni(OH)2 Catalysts in Alkaline Oxygen Evolution Reaction (OER): In Situ XANES Studies Lee, Sang-Yeon; Kim, Ik-Sun; Cho, Hyun-Seok Applied Catalysis B: Environmental, Vol. 284 https://doi.org/10.1016/j.apcatb.2020.119729	journal	May 2021
Variance based sensitivity analysis of model output. Design and estimator for the total sensitivity index Saltelli, Andrea; Annoni, Paola; Azzini, Ivano Computer Physics Communications, Vol. 181, Issue 2 https://doi.org/10.1016/j.cpc.2009.09.018	journal	February 2010
Designed constitution of NiO/Ni nanostructured electrode for high performance lithium ion battery Ni, Shibing; Li, Tao; Lv, Xiaohu Electrochimica Acta, Vol. 91 https://doi.org/10.1016/j.electacta.2012.12.113	journal	February 2013
A versatile ionic liquid-assisted approach to synthesize hierarchical structures of β-Ni(OH) 2 nanosheets for high performance pseudocapacitor Chen, Jun Song; Gui, Yang; Blackwood, Daniel John Electrochimica Acta, Vol. 188 https://doi.org/10.1016/j.electacta.2015.12.029	journal	January 2016
Preparation of mesoporous microspheres of NiO with high surface area and analysis on their pseudocapacitive behavior Abbas, Syed Asad; Jung, Kwang-Deog Electrochimica Acta, Vol. 193 https://doi.org/10.1016/j.electacta.2016.02.054	journal	March 2016
Lamellar-crossing-structured Ni(OH)2/CNTs/Ni(OH)2 nanocomposite for electrochemical supercapacitor materials Wu, Qingnan; Wen, Ming; Chen, Shipei Journal of Alloys and Compounds, Vol. 646 https://doi.org/10.1016/j.jallcom.2015.05.227	journal	October 2015
Effects of the Aqueous Environment on the Stability and Chemistry of β-NiOOH Surfaces Martirez, John Mark P.; Carter, Emily A. Chemistry of Materials, Vol. 30, Issue 15 https://doi.org/10.1021/acs.chemmater.8b01866	journal	July 2018
Benchmarking Density Functional Theory Based Methods To Model NiOOH Material Properties: Hubbard and van der Waals Corrections vs Hybrid Functionals Zaffran, Jeremie; Caspary Toroker, Maytal Journal of Chemical Theory and Computation, Vol. 12, Issue 8 https://doi.org/10.1021/acs.jctc.6b00657	journal	July 2016
Towards First Principles-Based Prediction of Highly Accurate Electrochemical Pourbaix Diagrams Zeng, Zhenhua; Chan, Maria K. Y.; Zhao, Zhi-Jian The Journal of Physical Chemistry C, Vol. 119, Issue 32 https://doi.org/10.1021/acs.jpcc.5b03169	journal	July 2015
Structural and Electronic Features of β-Ni(OH) ₂ and β-NiOOH from First Principles Tkalych, Alexander J.; Yu, Kuang; Carter, Emily A. The Journal of Physical Chemistry C, Vol. 119, Issue 43 https://doi.org/10.1021/acs.jpcc.5b08481	journal	October 2015
Improved Electrochemical Phase Diagrams from Theory and Experiment: The Ni–Water System and Its Complex Compounds Huang, L. -F.; Hutchison, M. J.; Santucci, R. J. The Journal of Physical Chemistry C, Vol. 121, Issue 18 https://doi.org/10.1021/acs.jpcc.7b02771	journal	May 2017
Insights into Active Sites and Mechanisms of Benzyl Alcohol Oxidation on Nickel–Iron Oxyhydroxide Electrodes Wei, Lingze; Hossain, Md Delowar; Boyd, Michael J. ACS Catalysis, Vol. 13, Issue 7 https://doi.org/10.1021/acscatal.2c05656	journal	March 2023
A Density Functional + U Assessment of Oxygen Evolution Reaction Mechanisms on β-NiOOH Tkalych, Alexander J.; Zhuang, Houlong L.; Carter, Emily A. ACS Catalysis, Vol. 7, Issue 8 https://doi.org/10.1021/acscatal.7b00999	journal	July 2017
A Comparative Study of Nickel, Cobalt, and Iron Oxyhydroxide Anodes for the Electrochemical Oxidation of 5-Hydroxymethylfurfural to 2,5-Furandicarboxylic Acid Taitt, Brandon J.; Nam, Do-Hwan; Choi, Kyoung-Shin ACS Catalysis, Vol. 9, Issue 1 https://doi.org/10.1021/acscatal.8b04003	journal	November 2018
Oxygen Evolution Activity on NiOOH Catalysts: Four-Coordinated Ni Cation as the Active Site and the Hydroperoxide Mechanism Li, Li-Fen; Li, Ye-Fei; Liu, Zhi-Pan ACS Catalysis, Vol. 10, Issue 4 https://doi.org/10.1021/acscatal.9b04975	journal	January 2020
Origins of the Instability of Nonprecious Hydrogen Evolution Reaction Catalysts at Open-Circuit Potential Wang, Zhenbin; Zheng, Ya-Rong; Montoya, Joseph ACS Energy Letters, Vol. 6, Issue 6 https://doi.org/10.1021/acsenergylett.1c00876	journal	May 2021
Fabrication of NiO Nanowall Electrodes for High Performance Lithium Ion Battery Varghese, Binni; Reddy, M. V.; Yanwu, Zhu Chemistry of Materials, Vol. 20, Issue 10 https://doi.org/10.1021/cm703512k	journal	May 2008
Mechanism and Activity of Water Oxidation on Selected Surfaces of Pure and Fe-Doped NiO _x Li, Ye-Fei; Selloni, Annabella ACS Catalysis, Vol. 4, Issue 4 https://doi.org/10.1021/cs401245q	journal	March 2014
The Heats of Formation of TiO, Ti₂O₃, Ti₃O₅ and TiO₂ from Combustion Calorimetry¹ Humphrey, George L. Journal of the American Chemical Society, Vol. 73, Issue 4 https://doi.org/10.1021/ja01148a051	journal	April 1951
Heats of Formation of Nickel and Cobalt Oxides (NiO and CoO) of Combustion Calorimetry Boyle, B. J.; King, E. G.; Conway, K. C. Journal of the American Chemical Society, Vol. 76, Issue 14 https://doi.org/10.1021/ja01643a072	journal	July 1954
Deciphering the Structural Transformations during Nickel Oxyhydroxide Electrode Operation Casas-Cabanas, Montse; Canales-Vázquez, Jesús; Rodríguez-Carvajal, Juan Journal of the American Chemical Society, Vol. 129, Issue 18 https://doi.org/10.1021/ja068433a	journal	May 2007
Identification of Highly Active Fe Sites in (Ni,Fe)OOH for Electrocatalytic Water Splitting Friebel, Daniel; Louie, Mary W.; Bajdich, Michal Journal of the American Chemical Society, Vol. 137, Issue 3 https://doi.org/10.1021/ja511559d	journal	January 2015
Unraveling Two Pathways for Electrochemical Alcohol and Aldehyde Oxidation on NiOOH Bender, Michael T.; Lam, Yan Choi; Hammes-Schiffer, Sharon Journal of the American Chemical Society, Vol. 142, Issue 51 https://doi.org/10.1021/jacs.0c10924	journal	December 2020
Operando Spectroscopic Identification of Active Sites in NiFe Prussian Blue Analogues as Electrocatalysts: Activation of Oxygen Atoms for Oxygen Evolution Reaction Su, Xiaozhi; Wang, Yu; Zhou, Jing Journal of the American Chemical Society, Vol. 140, Issue 36 https://doi.org/10.1021/jacs.8b05294	journal	August 2018
Unraveling Oxygen Evolution on Iron-Doped β-Nickel Oxyhydroxide: The Key Role of Highly Active Molecular-like Sites Martirez, John Mark P.; Carter, Emily A. Journal of the American Chemical Society, Vol. 141, Issue 1 https://doi.org/10.1021/jacs.8b12386	journal	November 2018
Facet-Independent Oxygen Evolution Activity of Pure β-NiOOH: Different Chemistries Leading to Similar Overpotentials Govind Rajan, Ananth; Martirez, John Mark P.; Carter, Emily A. Journal of the American Chemical Society, Vol. 142, Issue 7 https://doi.org/10.1021/jacs.9b13708	journal	January 2020
In Situ Raman Study of Nickel Oxide and Gold-Supported Nickel Oxide Catalysts for the Electrochemical Evolution of Oxygen Yeo, Boon Siang; Bell, Alexis T. The Journal of Physical Chemistry C, Vol. 116, Issue 15 https://doi.org/10.1021/jp3007415	journal	April 2012
Predictive control of selective secondary alcohol oxidation of glycerol on NiOOH Goetz, McKenna K.; Bender, Michael T.; Choi, Kyoung-Shin Nature Communications, Vol. 13, Issue 1 https://doi.org/10.1038/s41467-022-33637-7	journal	October 2022
Reliable electrochemical phase diagrams of magnetic transition metals and related compounds from high-throughput ab initio calculations Huang, Liang-Feng; Rondinelli, James M. npj Materials Degradation, Vol. 3, Issue 1 https://doi.org/10.1038/s41529-019-0088-z	journal	June 2019
Uncovering The Role of Oxygen in Ni-Fe(OxHy) Electrocatalysts using In situ Soft X-ray Absorption Spectroscopy during the Oxygen Evolution Reaction Drevon, Dorian; Görlin, Mikaela; Chernev, Petko Scientific Reports, Vol. 9, Issue 1 https://doi.org/10.1038/s41598-018-37307-x	journal	February 2019
A framework for quantifying uncertainty in DFT energy corrections Wang, Amanda; Kingsbury, Ryan; McDermott, Matthew Scientific Reports, Vol. 11, Issue 1 https://doi.org/10.1038/s41598-021-94550-5	journal	July 2021
Surface configuration and wettability of nickel(oxy)hydroxides: a first-principles investigation Eslamibidgoli, Mohammad Javad; Groß, Axel; Eikerling, Michael Physical Chemistry Chemical Physics, Vol. 19, Issue 34 https://doi.org/10.1039/C7CP03396F	journal	January 2017
Efficient Pourbaix diagrams of many-element compounds Patel, Anjli M.; Nørskov, Jens K.; Persson, Kristin A. Physical Chemistry Chemical Physics, Vol. 21, Issue 45 https://doi.org/10.1039/C9CP04799A	journal	January 2019
Electrochemical biomass valorization on gold-metal oxide nanoscale heterojunctions enables investigation of both catalyst and reaction dynamics with operando surface-enhanced Raman spectroscopy Heidary, Nina; Kornienko, Nikolay Chemical Science, Vol. 11, Issue 7 https://doi.org/10.1039/D0SC00136H	journal	January 2020
Influence of the exchange screening parameter on the performance of screened hybrid functionals Krukau, Aliaksandr V.; Vydrov, Oleg A.; Izmaylov, Artur F. The Journal of Chemical Physics, Vol. 125, Issue 22 https://doi.org/10.1063/1.2404663	journal	December 2006
Commentary: The Materials Project: A materials genome approach to accelerating materials innovation Jain, Anubhav; Ong, Shyue Ping; Hautier, Geoffroy APL Materials, Vol. 1, Issue 1 https://doi.org/10.1063/1.4812323	journal	July 2013
Characterization of NiFe oxyhydroxide electrocatalysts by integrated electronic structure calculations and spectroelectrochemistry Goldsmith, Zachary K.; Harshan, Aparna K.; Gerken, James B. Proceedings of the National Academy of Sciences, Vol. 114, Issue 12 https://doi.org/10.1073/pnas.1702081114	journal	March 2017
The atomic simulation environment—a Python library for working with atoms Hjorth Larsen, Ask; Jørgen Mortensen, Jens; Blomqvist, Jakob Journal of Physics: Condensed Matter, Vol. 29, Issue 27 https://doi.org/10.1088/1361-648X/aa680e	journal	June 2017
Electrochemical phase diagrams of Ni from ab initio simulations: role of exchange interactions on accuracy Huang, Liang-Feng; Rondinelli, James M. Journal of Physics: Condensed Matter, Vol. 29, Issue 47 https://doi.org/10.1088/1361-648X/aa9140	journal	October 2017
BEEF-vdW+U method applied to perovskites: thermodynamic, structural, electronic, and magnetic properties Li, Yang; Zheng, Ya-Shan; Zhu, Yi-An Journal of Physics: Condensed Matter, Vol. 31, Issue 14 https://doi.org/10.1088/1361-648X/aafe3e	journal	February 2019
Band theory and Mott insulators: Hubbard U instead of Stoner I Anisimov, Vladimir I.; Zaanen, Jan; Andersen, Ole K. Physical Review B, Vol. 44, Issue 3, p. 943-954 https://doi.org/10.1103/PhysRevB.44.943	journal	July 1991
Generalized gradient approximation for the exchange-correlation hole of a many-electron system Perdew, John P.; Burke, Kieron; Wang, Yue Physical Review B, Vol. 54, Issue 23 https://doi.org/10.1103/PhysRevB.54.16533	journal	December 1996
Electron-energy-loss spectra and the structural stability of nickel oxide: An LSDA+U study Dudarev, S. L.; Botton, G. A.; Savrasov, S. Y. Physical Review B, Vol. 57, Issue 3, p. 1505-1509 https://doi.org/10.1103/PhysRevB.57.1505	journal	January 1998
Oxidation energies of transition metal oxides within the GGA + U framework Wang, Lei; Maxisch, Thomas; Ceder, Gerbrand Physical Review B, Vol. 73, Issue 19 https://doi.org/10.1103/PhysRevB.73.195107	journal	May 2006
Formation enthalpies by mixing GGA and GGA + U calculations Jain, Anubhav; Hautier, Geoffroy; Ong, Shyue Ping Physical Review B, Vol. 84, Issue 4 https://doi.org/10.1103/PhysRevB.84.045115	journal	July 2011
Density functionals for surface science: Exchange-correlation model development with Bayesian error estimation Wellendorff, Jess; Lundgaard, Keld T.; Møgelhøj, Andreas Physical Review B, Vol. 85, Issue 23 https://doi.org/10.1103/PhysRevB.85.235149	journal	June 2012
Prediction of solid-aqueous equilibria: Scheme to combine first-principles calculations of solids with experimental aqueous states Persson, Kristin A.; Waldwick, Bryn; Lazic, Predrag Physical Review B, Vol. 85, Issue 23 https://doi.org/10.1103/PhysRevB.85.235438	journal	June 2012
Electrochemical phase diagrams for Ti oxides from density functional calculations Huang, Liang-Feng; Rondinelli, James M. Physical Review B, Vol. 92, Issue 24 https://doi.org/10.1103/PhysRevB.92.245126	journal	December 2015
Energetics of MnO 2 polymorphs in density functional theory Kitchaev, Daniil A.; Peng, Haowei; Liu, Yun Physical Review B, Vol. 93, Issue 4 https://doi.org/10.1103/PhysRevB.93.045132	journal	January 2016
Restoring the Density-Gradient Expansion for Exchange in Solids and Surfaces Perdew, John P.; Ruzsinszky, Adrienn; Csonka, Gábor I. Physical Review Letters, Vol. 100, Issue 13 https://doi.org/10.1103/PhysRevLett.100.136406	journal	April 2008
Strongly Constrained and Appropriately Normed Semilocal Density Functional Sun, Jianwei; Ruzsinszky, Adrienn; Perdew, John P. Physical Review Letters, Vol. 115, Issue 3 https://doi.org/10.1103/PhysRevLett.115.036402	journal	July 2015
Magnitude and Origin of the Band Gap in NiO Sawatzky, G. A.; Allen, J. W. Physical Review Letters, Vol. 53, Issue 24 https://doi.org/10.1103/PhysRevLett.53.2339	journal	December 1984
New developments in the Inorganic Crystal Structure Database (ICSD): accessibility in support of materials research and design Belsky, Alec; Hellenbrandt, Mariette; Karen, Vicky Lynn Acta Crystallographica Section B Structural Science, Vol. 58, Issue 3 https://doi.org/10.1107/S0108768102006948	journal	May 2002
Modeling Corrosion with First-Principles Electrochemical Phase Diagrams Huang, Liang-Feng; Scully, John R.; Rondinelli, James M. Annual Review of Materials Research, Vol. 49, Issue 1 https://doi.org/10.1146/annurev-matsci-070218-010105	journal	July 2019
Photoelectrochemistry of Nickel Hydroxide Thin Films Carpenter, Michael K. Journal of The Electrochemical Society, Vol. 136, Issue 4 https://doi.org/10.1149/1.2096777	journal	January 1989
The Synergistic Influences of OH[sup −] Concentration and Electrolyte Conductivity on the Redox Behavior of Ni(OH)[sub 2]/NiOOH Hu, Chi-Chang; Chang, Kuo-Hsin; Hsu, Tung-Yu Journal of The Electrochemical Society, Vol. 155, Issue 8 https://doi.org/10.1149/1.2945911	journal	January 2008
SALib: An open-source Python library for Sensitivity Analysis Herman, Jon; Usher, Will The Journal of Open Source Software, Vol. 2, Issue 9 https://doi.org/10.21105/joss.00097	journal	January 2017

Similar Records

Towards First Principles-Based Prediction of Highly Accurate Electrochemical Pourbaix Diagrams

Journal Article · 2015 · Journal of Physical Chemistry. C · OSTI ID:1390935

Zeng, Zhenhua; Chan, Maria K. Y.; Zhao, Zhi-Jian; +3 more

Pourbaix diagrams for the ternary system of iron-chromium-nickel

Journal Article · 1999 · Corrosion (Houston) · OSTI ID:20002039

Beverskog, B; Puigdomenech, I

Efficient Pourbaix diagrams of many-element compounds

Journal Article · 2019 · Physical Chemistry Chemical Physics. PCCP · OSTI ID:1573508

Patel, Anjli M.; Nørskov, Jens K.; Persson, Kristin A.; +1 more

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
crystal structure
energy
oxides
phase transitions
solid state physics
thermodynamic properties

Title: Assessing the Sensitivity of Pourbaix Diagrams to Computational Protocols: Electrochemical Stability of Ni Oxides as a Case Study

Citation Formats

References (62)

Similar Records

Related Subjects