An accurate and efficient framework for modelling the surface chemistry of ionic materials

0
An accurate and efficient framework for modelling the surface chemistry of ionic materials
  • Nørskov, J. K., Bligaard, T., Rossmeisl, J. & Christensen, C. H. Towards the computational design of solid catalysts. Nat. Chem. 1, 37–46 (2009).

    PubMed 

    Google Scholar 

  • Patel, H. A., Byun, J. & Yavuz, C. T. Carbon dioxide capture adsorbents: chemistry and methods. ChemSusChem 10, 1303–1317 (2017).

    CAS 
    PubMed 

    Google Scholar 

  • Rosen, A. S. et al. Tuning the redox activity of metal–organic frameworks for enhanced, selective O2 binding: design rules and ambient temperature O2 chemisorption in a cobalt–triazolate framework. J. Am. Chem. Soc. 142, 4317–4328 (2020).

    CAS 
    PubMed 

    Google Scholar 

  • Bligaard, T. et al. The Brønsted–Evans–Polanyi relation and the volcano curve in heterogeneous catalysis. J. Catal. 224, 206–217 (2004).

    CAS 

    Google Scholar 

  • Michaelides, A. et al. Identification of general linear relationships between activation energies and enthalpy changes for dissociation reactions at surfaces. J. Am. Chem. Soc. 125, 3704–3705 (2003).

    CAS 
    PubMed 

    Google Scholar 

  • Sauer, J. Ab initio calculations for molecule–surface interactions with chemical accuracy. Acc. Chem. Res. 52, 3502–3510 (2019).

    CAS 
    PubMed 

    Google Scholar 

  • Kubas, A. et al. Surface adsorption energetics studied with “gold standard” wave-function-based ab initio methods: small-molecule binding to TiO2(110). J. Phys. Chem. Lett. 7, 4207–4212 (2016).

    CAS 
    PubMed 

    Google Scholar 

  • Araujo, R. B., Rodrigues, G. L. S., dos Santos, E. C. & Pettersson, L. G. M. Adsorption energies on transition metal surfaces: towards an accurate and balanced description. Nat. Commun. 13, 6853 (2022).

    CAS 
    PubMed 
    PubMed Central 

    Google Scholar 

  • Hamada, I. Van der Waals density functional made accurate. Phys. Rev. B 89, 121103 (2014).

    Google Scholar 

  • Platero, E. E., Scarano, D., Spoto, G. & Zecchina, A. Dipole coupling and chemical shifts of CO and NO adsorbed on oxides and halides with rock-salt structure. Faraday Discuss. Chem. Soc. 80, 183–193 (1985).

    Google Scholar 

  • Di Valentin, C. et al. NO monomers on MgO powders and thin films. J. Phys. Chem. B 106, 1637–1645 (2002).

    Google Scholar 

  • Hamlyn, R. C. E. et al. Imaging the ordering of a weakly adsorbed two-dimensional condensate: ambient-pressure microscopy and spectroscopy of CO2 molecules on rutile TiO2(110). Phys. Chem. Chem. Phys. 20, 13122–13126 (2018).

    CAS 
    PubMed 

    Google Scholar 

  • Meixner, D. L., Arthur, D. A. & George, S. M. Kinetics of desorption, adsorption, and surface diffusion of CO2 on MgO(100). Surf. Sci. 261, 141–154 (1992).

    CAS 

    Google Scholar 

  • Chakradhar, A. & Burghaus, U. Carbon dioxide adsorption on MgO(001)–CO2 kinetics and dynamics. Surf. Sci. 616, 171–177 (2013).

    CAS 

    Google Scholar 

  • Pacchioni, G., Ricart, J. M. & Illas, F. Ab initio cluster model calculations on the chemisorption of CO2 and SO2 probe molecules on MgO and CaO (100) surfaces. A theoretical measure of oxide basicity. J. Am. Chem. Soc. 116, 10152–10158 (1994).

    CAS 

    Google Scholar 

  • Jensen, M. B., Pettersson, L. G. M., Swang, O. & Olsbye, U. CO2 sorption on MgO and CaO surfaces: a comparative quantum chemical cluster study. J. Phys. Chem. B 109, 16774–16781 (2005).

    CAS 
    PubMed 

    Google Scholar 

  • Downing, C. A., Sokol, A. A. & Catlow, C. R. A. The reactivity of CO2 on the MgO(100) surface. Phys. Chem. Chem. Phys. 16, 184–195 (2013).

    Google Scholar 

  • Mazheika, A. & Levchenko, S. V. Ni substitutional defects in bulk and at the (001) surface of MgO from first-principles calculations. J. Phys. Chem. C 120, 26934–26944 (2016).

    CAS 

    Google Scholar 

  • Yanagisawa, Y., Takaoka, K., Yamabe, S. & Ito, T. Interaction of CO2 with magnesium oxide surfaces: a TPD, FTIR, and cluster-model calculation study. J. Phys. Chem. 99, 3704–3710 (1995).

    CAS 

    Google Scholar 

  • Sorescu, D. C., Lee, J., Al-Saidi, W. A. & Jordan, K. D. CO2 adsorption on TiO2(110) rutile: insight from dispersion-corrected density functional theory calculations and scanning tunneling microscopy experiments. J. Chem. Phys. 134, 104707 (2011).

    PubMed 

    Google Scholar 

  • Huesges, Z., Müller, C., Paulus, B. & Maschio, L. Dispersion corrected DFT calculations for the adsorption of N2O on MgO. Surf. Sci. 627, 11–15 (2014).

    CAS 

    Google Scholar 

  • Shi, B. X., Wales, D. J., Michaelides, A. & Myung, C. W. Going for gold(-standard): attaining coupled cluster accuracy in oxide-supported nanoclusters. J. Chem. Theory Comput. 20, 5306–5316 (2024).

    CAS 
    PubMed 

    Google Scholar 

  • Campbell, C. T. & Sellers, J. R. V. Enthalpies and entropies of adsorption on well-defined oxide surfaces: experiment measurements. Chem. Rev. 113, 4106–4135 (2013).

    CAS 
    PubMed 

    Google Scholar 

  • Grimme, S., Antony, J., Ehrlich, S. & Krieg, H. A consistent and accurate ab initio parametrization of density functional dispersion correction (DFT-D) for the 94 elements H-Pu. J. Chem. Phys. 132, 154104 (2010).

    PubMed 

    Google Scholar 

  • Ehlert, S. et al. r2SCAN-D4: dispersion corrected meta-generalized gradient approximation for general chemical applications. J. Chem. Phys. 154, 061101 (2021).

    CAS 
    PubMed 

    Google Scholar 

  • Ning, J. et al. Workhorse minimally empirical dispersion-corrected density functional with tests for weakly bound systems: r2SCAN + rVV10. Phys. Rev. B 106, 075422 (2022).

    CAS 

    Google Scholar 

  • Bučko, T., Lebègue, S., Ángyán, J. G. & Hafner, J. Extending the applicability of the Tkatchenko-Scheffler dispersion correction via iterative Hirshfeld partitioning. J. Chem. Phys. 141, 034114 (2014).

    PubMed 

    Google Scholar 

  • Klimeš, J., Kaltak, M., Maggio, E. & Kresse, G. Singles correlation energy contributions in solids. J. Chem. Phys. 143, 102816 (2015).

    PubMed 

    Google Scholar 

  • Ehrlich, S., Moellmann, J., Reckien, W., Bredow, T. & Grimme, S. System-dependent dispersion coefficients for the DFT-D3 treatment of adsorption processes on ionic surfaces. ChemPhysChem 12, 3414–3420 (2011).

    CAS 
    PubMed 

    Google Scholar 

  • Kothakonda, M. et al. Testing the r2SCAN density functional for the thermodynamic stability of solids with and without a van der Waals correction. ACS Mater. Au 3, 102–111 (2023).

    CAS 
    PubMed 

    Google Scholar 

  • Shi, B. X. et al. Many-body methods for surface chemistry come of age: achieving consensus with experiments. J. Am. Chem. Soc. 145, 25372–25381 (2023).

    CAS 
    PubMed 
    PubMed Central 

    Google Scholar 

  • Ye, H.-Z. & Berkelbach, T. C. Ab initio surface chemistry with chemical accuracy. Preprint at (2024).

  • Karalti, O., Alfè, D., Gillan, M. J. & Jordan, K. D. Adsorption of a water molecule on the MgO(100) surface as described by cluster and slab models. Phys. Chem. Chem. Phys. 14, 7846–7853 (2012).

    CAS 
    PubMed 

    Google Scholar 

  • Alessio, M., Usvyat, D. & Sauer, J. Chemically accurate adsorption energies: CO and H2O on the MgO(001) surface. J. Chem. Theory Comput. 15, 1329–1344 (2019).

    CAS 
    PubMed 

    Google Scholar 

  • Lu, Y. et al. Multiscale QM/MM modelling of catalytic systems with ChemShell. Phys. Chem. Chem. Phys. 25, 21816–21835 (2023).

    CAS 
    PubMed 

    Google Scholar 

  • Jain, A. et al. Commentary: the Materials Project: a materials genome approach to accelerating materials innovation. APL Mater 1, 011002 (2013).

    Google Scholar 

  • Ye, H.-Z. & Berkelbach, T. C. Adsorption and vibrational spectroscopy of CO on the surface of MgO from periodic local coupled-cluster theory. Faraday Discuss 254, 628–640 (2024).

    CAS 
    PubMed 
    PubMed Central 

    Google Scholar 

  • Campbell, C. T. & Sellers, J. R. V. The entropies of adsorbed molecules. J. Am. Chem. Soc. 134, 18109–18115 (2012).

    CAS 
    PubMed 

    Google Scholar 

  • Kirkpatrick, J. et al. Pushing the frontiers of density functionals by solving the fractional electron problem. Science 374, 1385–1389 (2021).

    CAS 
    PubMed 

    Google Scholar 

  • Sheldon, C., Paier, J., Usvyat, D. & Sauer, J. Hybrid RPA:DFT approach for adsorption on transition metal surfaces: methane and ethane on platinum (111). J. Chem. Theory Comput. 20, 2219–2227 (2024).

    PubMed 
    PubMed Central 

    Google Scholar 

  • Sillar, K., Hofmann, A. & Sauer, J. Ab initio study of hydrogen adsorption in MOF-5. J. Am. Chem. Soc. 131, 4143–4150 (2009).

    CAS 
    PubMed 

    Google Scholar 

  • Berger, F., Rybicki, M. & Sauer, J. Adsorption and cracking of propane by zeolites of different pore size. J. Catal. 395, 117–128 (2021).

    CAS 

    Google Scholar 

  • Wichtendahl, R., Rodriguez-Rodrigo, M., Härtel, U., Kuhlenbeck, H. & Freund, H.-J. Thermodesorption of CO and NO from vacuum-cleaved NiO(100) and MgO(100). Phys. Status Solidi A 173, 93–100 (1999).

    CAS 

    Google Scholar 

  • Dohnálek, Z., Kim, J., Bondarchuk, O., White, J. M. & Kay, B. D. Physisorption of N2, O2, and CO on fully oxidized TiO2(110). J. Phys. Chem. B 110, 6229–6235 (2006).

    PubMed 

    Google Scholar 

  • Shi, B. X. et al. General embedded cluster protocol for accurate modeling of oxygen vacancies in metal-oxides. J. Chem. Phys. 156, 124704 (2022).

    CAS 
    PubMed 

    Google Scholar 

  • Nagy, P. R. & Kállay, M. Approaching the basis set limit of CCSD(T) energies for large molecules with local natural orbital coupled-cluster methods. J. Chem. Theory Comput. 15, 5275–5298 (2019).

    CAS 
    PubMed 

    Google Scholar 

  • Riplinger, C. & Neese, F. An efficient and near linear scaling pair natural orbital based local coupled cluster method. J. Chem. Phys. 138, 034106 (2013).

    PubMed 

    Google Scholar 

  • Rosen, A. Quacc – the quantum accelerator. Zenodo (2024).

  • Sauer, J. Molecular models in ab initio studies of solids and surfaces: from ionic crystals and semiconductors to catalysts. Chem. Rev. 89, 199–255 (1989).

    CAS 

    Google Scholar 

  • Bogdanov, N. A., Li Manni, G., Sharma, S., Gunnarsson, O. & Alavi, A. Enhancement of superexchange due to synergetic breathing and hopping in corner-sharing cuprates. Nat. Phys. 18, 190–195 (2022).

    CAS 

    Google Scholar 

  • Dittmer, A., Izsák, R., Neese, F. & Maganas, D. Accurate band gap predictions of semiconductors in the framework of the similarity transformed equation of motion coupled cluster theory. Inorg. Chem. 58, 9303–9315 (2019).

    CAS 
    PubMed 
    PubMed Central 

    Google Scholar 

  • Chizallet, C. et al. Assignment of photoluminescence spectra of MgO powders: TD-DFT cluster calculations combined to experiments. Part I: structure effects on dehydroxylated surfaces. J. Phys. Chem. C 112, 16629–16637 (2008).

    CAS 

    Google Scholar 

  • Chung, L. W. et al. The ONIOM method and its applications. Chem. Rev. 115, 5678–5796 (2015).

    CAS 
    PubMed 

    Google Scholar 

  • Neese, F., Wennmohs, F., Becker, U. & Riplinger, C. The ORCA quantum chemistry program package. J. Chem. Phys. 152, 224108 (2020).

    CAS 
    PubMed 

    Google Scholar 

  • Kállay, M. et al. The MRCC program system: accurate quantum chemistry from water to proteins. J. Chem. Phys. 152, 074107 (2020).

    PubMed 

    Google Scholar 

  • Neese, F. & Valeev, E. F. Revisiting the atomic natural orbital approach for basis sets: robust systematic basis sets for explicitly correlated and conventional correlated ab initio methods. J. Chem. Theory Comput. 7, 33–43 (2011).

    CAS 
    PubMed 

    Google Scholar 

  • Kresse, G. & Furthmüller, J. Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set. Comput. Mater. Sci. 6, 15–50 (1996).

    CAS 

    Google Scholar 

  • Kresse, G. & Furthmüller, J. Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set. Phys. Rev. B 54, 11169–11186 (1996).

    CAS 

    Google Scholar 

  • Li, Y.-P., Gomes, J., Mallikarjun Sharada, S., Bell, A. T. & Head-Gordon, M. Improved force-field parameters for QM/MM simulations of the energies of adsorption for molecules in zeolites and a free rotor correction to the rigid rotor harmonic oscillator model for adsorption enthalpies. J. Phys. Chem. C 119, 1840–1850 (2015).

    CAS 

    Google Scholar 

  • Sun, Q. & Chan, G. K.-L. Quantum embedding theories. Acc. Chem. Res. 49, 2705–2712 (2016).

    CAS 
    PubMed 

    Google Scholar 

  • Lau, B. T. G., Knizia, G. & Berkelbach, T. C. Regional embedding enables high-level quantum chemistry for surface science. J. Phys. Chem. Lett. 12, 1104–1109 (2021).

    CAS 
    PubMed 

    Google Scholar 

  • Schäfer, T., Libisch, F., Kresse, G. & Grüneis, A. Local embedding of coupled cluster theory into the random phase approximation using plane waves. J. Chem. Phys. 154, 011101 (2021).

    PubMed 

    Google Scholar 

  • Huang, Z. et al. Advancing surface chemistry with large-scale ab-initio quantum many-body simulations. Preprint at (2025).

  • Al-Hamdani, Y. S. et al. Interactions between large molecules pose a puzzle for reference quantum mechanical methods. Nat. Commun. 12, 3927 (2021).

    CAS 
    PubMed 
    PubMed Central 

    Google Scholar 

  • Schäfer, T., Irmler, A., Gallo, A. & Grüneis, A. Understanding discrepancies of wavefunction theories for large molecules. Preprint at (2024).

  • Shi, B. X. et al. Systematic discrepancies between reference methods for noncovalent interactions within the S66 dataset. J. Chem. Phys. 162, 144107 (2025).

    CAS 
    PubMed 

    Google Scholar 

  • Cui, Z.-H., Zhai, H., Zhang, X. & Chan, G. K.-L. Systematic electronic structure in the cuprate parent state from quantum many-body simulations. Science 377, 1192–1198 (2022).

    CAS 
    PubMed 

    Google Scholar 

  • Shi, B. X. et al. Supporting data for ‘An accurate and efficient framework for modelling the surface chemistry of ionic materials’. Zenodo (2025).

  • Günster, J., Liu, G., Stultz, J. & Goodman, D. W. Interaction of methanol and water on MgO(100) studied by ultraviolet photoelectron and metastable impact electron spectroscopies. J. Chem. Phys. 110, 2558–2565 (1999).

    Google Scholar 

  • Stirniman, M. J., Huang, C., Scott Smith, R., Joyce, S. A. & Kay, B. D. The adsorption and desorption of water on single crystal MgO(100): the role of surface defects. J. Chem. Phys. 105, 1295–1298 (1996).

    CAS 

    Google Scholar 

  • Thompson, T. L., Diwald, O. & Yates, J. T. CO2 as a probe for monitoring the surface defects on TiO2(110) temperature-programmed desorption. J. Phys. Chem. B 107, 11700–11704 (2003).

    CAS 

    Google Scholar 

  • Lian, J. C. et al. N2O adsorption on the surface of MgO(001) thin films: an infrared and TPD study. J. Phys. Chem. C 114, 3148–3151 (2010).

    CAS 

    Google Scholar 

  • link

    Leave a Reply

    Your email address will not be published. Required fields are marked *