Fast Correction of Errors in the DFT‐Calculated Energies of Gaseous Nitrogen‐Containing Species

Urrego‐Ortiz, Ricardo; Builes, Santiago; Calle‐Vallejo, Federico

doi:10.1002/cctc.202100125

Fast Correction of Errors in the DFT‐Calculated Energies of Gaseous Nitrogen‐Containing Species

Journal Article · Wed Mar 31 00:00:00 EDT 2021 · ChemCatChem

DOI:https://doi.org/10.1002/cctc.202100125· OSTI ID:1786197

^[1]; ^[1]; ^[2]

Departamento de Ingeniería de Procesos Universidad EAFIT Carrera 49 No 7 sur – 50 050022 Medellín Colombia
Departament de Ciència de Materials i Química Física &, Institut de Química Teòrica i Computacional (IQTCUB) Universitat de Barcelona Martí i Franquès 1 08028 Barcelona Spain

Abstract

Modeling adsorption phenomena on surfaces by DFT calculations often involves substantial errors, resulting in inaccurate predictions of catalytic activities. Such errors partly stem from the inaccurate description of the energetics of free molecules. Herein, we use a semiempirical group‐additivity method to correct the DFT‐calculated heats of formation of 106 carbon‐ and nitrogen‐containing gaseous compounds belonging to 15 different chemical families. PBE, PW91, RPBE and BEEF‐vdW initially yield mean absolute errors (MAEs) with respect to experiments in the range of 0.32–0.75 eV. After correcting the systematic errors, the overall MAEs decrease to ∼0.05 eV. Additionally, upon applying the corrections to three types of reaction enthalpies, the resulting MAEs are below 0.10 eV. These functional‐group corrections can be used in (electro)catalysis to correct the gas‐phase references necessary to evaluate equilibrium potentials and adsorption energies, predict error cancellation, and assess conflicting experimental data.

View Accepted Manuscript (Publisher)

Sponsoring Organization:: USDOE

Grant/Contract Number:: NONE; SC0012704

OSTI ID:: 1786197

Journal Information:: ChemCatChem, Journal Name: ChemCatChem Journal Issue: 10 Vol. 13; ISSN 1867-3880

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

References (70)

Molecular and solid-state tests of density functional approximations: LSD, GGAs, and meta-GGAs Kurth, Stefan; Perdew, John P.; Blaha, Peter International Journal of Quantum Chemistry, Vol. 75, Issue 4-5 https://doi.org/10.1002/(SICI)1097-461X(1999)75:4/5<889::AID-QUA54>3.0.CO;2-8	journal	January 1999
Integration of modern computational chemistry and ASPEN PLUS for chemical process design Tsai, Chang‐Che; Lin, Shiang‐Tai AIChE Journal, Vol. 66, Issue 10 https://doi.org/10.1002/aic.16987	journal	August 2020
Trends in Stability of Perovskite Oxides Calle-Vallejo, Federico; Martínez, José I.; García-Lastra, Juan M. Angewandte Chemie, Vol. 122, Issue 42 https://doi.org/10.1002/ange.201002301	journal	September 2010
Trends in Stability of Perovskite Oxides Calle-Vallejo, Federico; Martínez, José I.; García-Lastra, Juan M. Angewandte Chemie International Edition, Vol. 49, Issue 42 https://doi.org/10.1002/anie.201002301	journal	September 2010
The Mechanism of CO and CO ₂ Hydrogenation to Methanol over Cu-Based Catalysts Studt, Felix; Behrens, Malte; Kunkes, Edward L. ChemCatChem, Vol. 7, Issue 7 https://doi.org/10.1002/cctc.201500123	journal	March 2015
Influence of Van der Waals Interactions on the Solvation Energies of Adsorbates at Pt‐Based Electrocatalysts Granda‐Marulanda, Laura P.; Builes, Santiago; Koper, Marc T. M. ChemPhysChem, Vol. 20, Issue 22 https://doi.org/10.1002/cphc.201900512	journal	August 2019
Effect of the damping function in dispersion corrected density functional theory Grimme, Stefan; Ehrlich, Stephan; Goerigk, Lars Journal of Computational Chemistry, Vol. 32, Issue 7 https://doi.org/10.1002/jcc.21759	journal	March 2011
Advances and challenges in modeling solvated reaction mechanisms for renewable fuels and chemicals Basdogan, Yasemin; Maldonado, Alex M.; Keith, John A. WIREs Computational Molecular Science, Vol. 10, Issue 2 https://doi.org/10.1002/wcms.1446	journal	August 2019
Thermochemical Data of Organic Compounds Pedley, J. B.; Naylor, R. D.; Kirby, S. P. Springer Dordrecht https://doi.org/10.1007/978-94-009-4099-4	book	January 1986
CO and CO2 Hydrogenation to Methanol Calculated Using the BEEF-vdW Functional Studt, Felix; Abild-Pedersen, Frank; Varley, Joel B. Catalysis Letters, Vol. 143, Issue 1 https://doi.org/10.1007/s10562-012-0947-5	journal	December 2012
Microscopic determination of the interlayer binding energy in graphite Benedict, Lorin X.; Chopra, Nasreen G.; Cohen, Marvin L. Chemical Physics Letters, Vol. 286, Issue 5-6 https://doi.org/10.1016/S0009-2614(97)01466-8	journal	April 1998
Substantial improvement of electrocatalytic predictions by systematic assessment of solvent effects on adsorption energies Rendón-Calle, Alejandra; Builes, Santiago; Calle-Vallejo, Federico Applied Catalysis B: Environmental, Vol. 276 https://doi.org/10.1016/j.apcatb.2020.119147	journal	November 2020
The standard enthalpies of formation of some intermetallic compounds of early 4d and 5d transition metals by high temperature direct synthesis calorimetry Meschel, S. V.; Chen, X. Q.; Kleppa, O. J. Calphad, Vol. 33, Issue 1 https://doi.org/10.1016/j.calphad.2008.07.013	journal	March 2009
Ab initio quantum chemical predictions of enthalpies of formation, heat capacities, and entropies of gas-phase energetic compounds Osmont, Antoine; Catoire, Laurent; Gökalp, Iskender Combustion and Flame, Vol. 151, Issue 1-2 https://doi.org/10.1016/j.combustflame.2007.05.001	journal	October 2007
DFT-GGA errors in NO chemisorption energies on (111) transition metal surfaces Huang, Xu; Mason, Sara E. Surface Science, Vol. 621 https://doi.org/10.1016/j.susc.2013.09.024	journal	March 2014
Catalytic Stability Studies Employing Dedicated Model Catalysts Hess, Franziska; Smarsly, Bernd M.; Over, Herbert Accounts of Chemical Research, Vol. 53, Issue 2 https://doi.org/10.1021/acs.accounts.9b00467	journal	January 2020
Functional Independent Scaling Relation for ORR/OER Catalysts Christensen, Rune; Hansen, Heine A.; Dickens, Colin F. The Journal of Physical Chemistry C, Vol. 120, Issue 43 https://doi.org/10.1021/acs.jpcc.6b09141	journal	October 2016
Haber Process Made Efficient by Hydroxylated Graphene: Ab Initio Thermochemistry and Reactive Molecular Dynamics Chaban, Vitaly V.; Prezhdo, Oleg V. The Journal of Physical Chemistry Letters, Vol. 7, Issue 13 https://doi.org/10.1021/acs.jpclett.6b01178	journal	June 2016
A Semiempirical Method to Detect and Correct DFT-Based Gas-Phase Errors and Its Application in Electrocatalysis Granda-Marulanda, Laura P.; Rendón-Calle, Alejandra; Builes, Santiago ACS Catalysis, Vol. 10, Issue 12 https://doi.org/10.1021/acscatal.0c01075	journal	May 2020
The Importance of the Electrochemical Environment in the Electro-Oxidation of Methanol on Pt(111) Sakong, Sung; Groß, Axel ACS Catalysis, Vol. 6, Issue 8 https://doi.org/10.1021/acscatal.6b00931	journal	July 2016
Role of Defects in the Interplay between Adsorbate Evolving and Lattice Oxygen Mechanisms of the Oxygen Evolution Reaction in RuO ₂ and IrO ₂ Zagalskaya, Alexandra; Alexandrov, Vitaly ACS Catalysis, Vol. 10, Issue 6 https://doi.org/10.1021/acscatal.9b05544	journal	February 2020
Why Is Bulk Thermochemistry a Good Descriptor for the Electrocatalytic Activity of Transition Metal Oxides? Calle-Vallejo, Federico; Díaz-Morales, Oscar A.; Kolb, Manuel J. ACS Catalysis, Vol. 5, Issue 2 https://doi.org/10.1021/cs5016657	journal	January 2015
Bulk Properties of Transition Metals: A Challenge for the Design of Universal Density Functionals Janthon, Patanachai; Luo, Sijie (Andy); Kozlov, Sergey M. Journal of Chemical Theory and Computation, Vol. 10, Issue 9 https://doi.org/10.1021/ct500532v	journal	August 2014
Heats of Formation from DFT Calculations: An Examination of Several Parameterizations Guthrie, J. Peter The Journal of Physical Chemistry A, Vol. 105, Issue 40 https://doi.org/10.1021/jp010355k	journal	October 2001
Theoretical Thermochemistry: Ab Initio Heat of Formation for Hydroxylamine Saraf, S. R.; Rogers, W. J.; Mannan, M. S. The Journal of Physical Chemistry A, Vol. 107, Issue 8 https://doi.org/10.1021/jp026027h	journal	January 2003
Computational predictions of energy materials using density functional theory Jain, Anubhav; Shin, Yongwoo; Persson, Kristin A. Nature Reviews Materials, Vol. 1, Issue 1 https://doi.org/10.1038/natrevmats.2015.4	journal	January 2016
Alloys of platinum and early transition metals as oxygen reduction electrocatalysts Greeley, J.; Stephens, I. E. L.; Bondarenko, A. S. Nature Chemistry, Vol. 1, Issue 7, p. 552-556 https://doi.org/10.1038/nchem.367	journal	September 2009
Measurement of the cleavage energy of graphite Wang, Wen; Dai, Shuyang; Li, Xide Nature Communications, Vol. 6, Issue 1 https://doi.org/10.1038/ncomms8853	journal	August 2015
The Open Quantum Materials Database (OQMD): assessing the accuracy of DFT formation energies Kirklin, Scott; Saal, James E.; Meredig, Bryce npj Computational Materials, Vol. 1, Issue 1 https://doi.org/10.1038/npjcompumats.2015.10	journal	December 2015
Enhancing materials property prediction by leveraging computational and experimental data using deep transfer learning Jha, Dipendra; Choudhary, Kamal; Tavazza, Francesca Nature Communications, Vol. 10, Issue 1 https://doi.org/10.1038/s41467-019-13297-w	journal	November 2019
The role of decomposition reactions in assessing first-principles predictions of solid stability Bartel, Christopher J.; Weimer, Alan W.; Lany, Stephan npj Computational Materials, Vol. 5, Issue 1 https://doi.org/10.1038/s41524-018-0143-2	journal	January 2019
Accuracy of theoretical catalysis from a model of iron-catalyzed ammonia synthesis Kepp, Kasper P. Communications Chemistry, Vol. 1, Issue 1 https://doi.org/10.1038/s42004-018-0063-6	journal	October 2018
High capacity hydrogenstorage materials: attributes for automotive applications and techniques for materials discovery Yang, Jun; Sudik, Andrea; Wolverton, Christopher Chem. Soc. Rev., Vol. 39, Issue 2 https://doi.org/10.1039/B802882F	journal	January 2010
Choosing a proper exchange–correlation functional for the computational catalysis on surface Teng, Bo-Tao; Wen, Xiao-Dong; Fan, Maohong Phys. Chem. Chem. Phys., Vol. 16, Issue 34 https://doi.org/10.1039/C4CP01868K	journal	January 2014
Identifying systematic DFT errors in catalytic reactions Christensen, Rune; Hansen, Heine A.; Vegge, Tejs Catalysis Science & Technology, Vol. 5, Issue 11 https://doi.org/10.1039/C5CY01332A	journal	January 2015
Thermodynamic assessment of the oxygen reduction activity in aqueous solutions Tripkovic, Vladimir Physical Chemistry Chemical Physics, Vol. 19, Issue 43 https://doi.org/10.1039/C7CP05448C	journal	January 2017
The adhesion energy measured by a stress accumulation-peeling mechanism in the exfoliation of graphite Xia, Minggang; Liang, Chunping; Cheng, Zhaofang Physical Chemistry Chemical Physics, Vol. 21, Issue 3 https://doi.org/10.1039/C8CP06608F	journal	January 2019
How copper catalyzes the electroreduction of carbon dioxide into hydrocarbon fuels Peterson, Andrew A.; Abild-Pedersen, Frank; Studt, Felix Energy & Environmental Science, Vol. 3, Issue 9 https://doi.org/10.1039/c0ee00071j	journal	January 2010
Theoretical design and experimental implementation of Ag/Au electrodes for the electrochemical reduction of nitrate Calle-Vallejo, Federico; Huang, Minghua; Henry, John B. Physical Chemistry Chemical Physics, Vol. 15, Issue 9 https://doi.org/10.1039/c2cp44620k	journal	January 2013
Energy of Cohesion, Compressibility, and the Potential Energy Functions of the Graphite System Girifalco, L. A.; Lad, R. A. The Journal of Chemical Physics, Vol. 25, Issue 4 https://doi.org/10.1063/1.1743030	journal	October 1956
Additivity Rules for the Estimation of Molecular Properties. Thermodynamic Properties Benson, Sidney W.; Buss, Jerry H. The Journal of Chemical Physics, Vol. 29, Issue 3 https://doi.org/10.1063/1.1744539	journal	September 1958
A consistent and accurate ab initio parametrization of density functional dispersion correction (DFT-D) for the 94 elements H-Pu Grimme, Stefan; Antony, Jens; Ehrlich, Stephan The Journal of Chemical Physics, Vol. 132, Issue 15 https://doi.org/10.1063/1.3382344	journal	April 2010
Assessment of Gaussian-2 and density functional theories for the computation of enthalpies of formation Curtiss, Larry A.; Raghavachari, Krishnan; Redfern, Paul C. The Journal of Chemical Physics, Vol. 106, Issue 3 https://doi.org/10.1063/1.473182	journal	January 1997
An assessment of theoretical procedures for the calculation of reliable free radical thermochemistry: A recommended new procedure Mayer, Paul M.; Parkinson, Christopher J.; Smith, David M. The Journal of Chemical Physics, Vol. 108, Issue 2 https://doi.org/10.1063/1.476256	journal	January 1998
On the errors of local density (LDA) and generalized gradient (GGA) approximations to the Kohn-Sham potential and orbital energies Gritsenko, O. V.; Mentel, Ł. M.; Baerends, E. J. The Journal of Chemical Physics, Vol. 144, Issue 20 https://doi.org/10.1063/1.4950877	journal	May 2016
Facing the challenge of predicting the standard formation enthalpies of n -butyl-phosphate species with ab initio methods Saab, Mohamad; Réal, Florent; Šulka, Martin The Journal of Chemical Physics, Vol. 146, Issue 24 https://doi.org/10.1063/1.4986953	journal	June 2017
Special points for Brillouin-zone integrations Monkhorst, Hendrik J.; Pack, James D. Physical Review B, Vol. 13, Issue 12, p. 5188-5192 https://doi.org/10.1103/PhysRevB.13.5188	journal	June 1976
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set Kresse, G.; Furthmüller, J. Physical Review B, Vol. 54, Issue 16, p. 11169-11186 https://doi.org/10.1103/PhysRevB.54.11169	journal	October 1996
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
Simplified generalized-gradient approximation and anharmonicity: Benchmark calculations on molecules Patton, David C.; Porezag, Dirk V.; Pederson, Mark R. Physical Review B, Vol. 55, Issue 12 https://doi.org/10.1103/PhysRevB.55.7454	journal	March 1997
From ultrasoft pseudopotentials to the projector augmented-wave method Kresse, G.; Joubert, D. Physical Review B, Vol. 59, Issue 3, p. 1758-1775 https://doi.org/10.1103/PhysRevB.59.1758	journal	January 1999
Improved adsorption energetics within density-functional theory using revised Perdew-Burke-Ernzerhof functionals Hammer, B.; Hansen, L. B.; Nørskov, J. K. Physical Review B, Vol. 59, Issue 11 https://doi.org/10.1103/PhysRevB.59.7413	journal	March 1999
First-principles study of the stability and electronic structure of metal hydrides Smithson, H.; Marianetti, C. A.; Morgan, D. Physical Review B, Vol. 66, Issue 14 https://doi.org/10.1103/PhysRevB.66.144107	journal	October 2002
Interlayer cohesive energy of graphite from thermal desorption of polyaromatic hydrocarbons Zacharia, Renju; Ulbricht, Hendrik; Hertel, Tobias Physical Review B, Vol. 69, Issue 15 https://doi.org/10.1103/PhysRevB.69.155406	journal	April 2004
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 energies of rutile metal dioxides using density functional theory Martínez, J. I.; Hansen, H. A.; Rossmeisl, J. Physical Review B, Vol. 79, Issue 4 https://doi.org/10.1103/PhysRevB.79.045120	journal	January 2009
Hybrid density functional calculations of redox potentials and formation energies of transition metal compounds Chevrier, V. L.; Ong, S. P.; Armiento, R. Physical Review B, Vol. 82, Issue 7 https://doi.org/10.1103/PhysRevB.82.075122	journal	August 2010
Correcting density functional theory for accurate predictions of compound enthalpies of formation: Fitted elemental-phase reference energies Stevanović, Vladan; Lany, Stephan; Zhang, Xiuwen Physical Review B, Vol. 85, Issue 11 https://doi.org/10.1103/PhysRevB.85.115104	journal	March 2012
Accuracy of density functional theory in predicting formation energies of ternary oxides from binary oxides and its implication on phase stability Hautier, Geoffroy; Ong, Shyue Ping; Jain, Anubhav Physical Review B, Vol. 85, Issue 15 https://doi.org/10.1103/PhysRevB.85.155208	journal	April 2012
Interlayer binding energy of graphite: A mesoscopic determination from deformation Liu, Ze; Liu, Jefferson Zhe; Cheng, Yao Physical Review B, Vol. 85, Issue 20 https://doi.org/10.1103/PhysRevB.85.205418	journal	May 2012
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
Approaching chemical accuracy with density functional calculations: Diatomic energy corrections Grindy, Scott; Meredig, Bryce; Kirklin, Scott Physical Review B, Vol. 87, Issue 7 https://doi.org/10.1103/PhysRevB.87.075150	journal	February 2013
Generalized Gradient Approximation Made Simple Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868 https://doi.org/10.1103/PhysRevLett.77.3865	journal	October 1996
Climbing the Density Functional Ladder: Nonempirical Meta–Generalized Gradient Approximation Designed for Molecules and Solids Tao, Jianmin; Perdew, John P.; Staroverov, Viktor N. Physical Review Letters, Vol. 91, Issue 14 https://doi.org/10.1103/PhysRevLett.91.146401	journal	September 2003
The density functional formalism, its applications and prospects Jones, R. O.; Gunnarsson, O. Reviews of Modern Physics, Vol. 61, Issue 3 https://doi.org/10.1103/RevModPhys.61.689	journal	July 1989
Control of Graphene's Properties by Reversible Hydrogenation: Evidence for Graphane Elias, D. C.; Nair, R. R.; Mohiuddin, T. M. G. Science, Vol. 323, Issue 5914 https://doi.org/10.1126/science.1167130	journal	January 2009
Quantum-chemical and group-additive calculations of the enthalpies of formation of hydroxylamines and oximes Shaikhlislamov, D. S.; Talipov, M. R.; Khursan, S. L. Russian Journal of Physical Chemistry A, Vol. 81, Issue 2 https://doi.org/10.1134/S003602440702015X	journal	February 2007
Enthalpies of Formation of LaMO ₃ Perovskites (M = Cr, Fe, Co, and Ni) Cheng, Jihong; Navrotsky, Alexandra; Zhou, Xiao-Dong Journal of Materials Research, Vol. 20, Issue 1 https://doi.org/10.1557/JMR.2005.0018	journal	January 2005
Recent trends on density functional theory–assisted calculations of structures and properties of metal–organic frameworks and metal–organic frameworks-derived nanocarbons Kharissova, Oxana V.; Kharisov, Boris I.; González, Lucy T. Journal of Materials Research, Vol. 35, Issue 11 https://doi.org/10.1557/jmr.2020.109	journal	June 2020
Toward Computational Materials Design: The Impact of Density Functional Theory on Materials Research Hafner, Jürgen; Wolverton, Christopher; Ceder, Gerbrand MRS Bulletin, Vol. 31, Issue 9 https://doi.org/10.1557/mrs2006.174	journal	September 2006

Similar Records

A comparative analysis of different van der Waals treatments for molecular adsorption on the basal plane of 2H-MoS₂

Journal Article · Tue Nov 22 23:00:00 EST 2022 · Surface Science · OSTI ID:2007819

Invariant Molecular Representations for Heterogeneous Catalysis

Journal Article · Tue Jan 09 23:00:00 EST 2024 · Journal of Chemical Information and Modeling · OSTI ID:2471146

Fast Correction of Errors in the DFT‐Calculated Energies of Gaseous Nitrogen‐Containing Species

Citation Formats

References (70)

Similar Records

Related Subjects