General reactive element-based machine learning potentials for heterogeneous catalysis

Machine Learning


  • Liu, Z.-P. & Hu, P. General rules for predicting where a catalytic reaction should occur on metal surfaces: a density functional theory study of C–H and C–O bond breaking/making on flat, stepped, and kinked metal surfaces. J. Am. Chem. Soc. 125, 1958–1967 (2003).

    Article 
    PubMed 
    CAS 

    Google Scholar 

  • Alavi, A., Hu, P., Deutsch, T., Silvestrelli, P. L. & Hutter, J. CO oxidation on Pt(111): an ab initio density functional theory study. Phys. Rev. Lett. 80, 3650–3653 (1998).

    Article 
    CAS 

    Google Scholar 

  • Oganov, A. R., Pickard, C. J., Zhu, Q. & Needs, R. J. Structure prediction drives materials discovery. Nat. Rev. Mater. 4, 331–348 (2019).

    Article 

    Google Scholar 

  • Behler, J. & Parrinello, M. Generalized neural-network representation of high-dimensional potential-energy surfaces. Phys. Rev. Lett. 98, 146401 (2007).

    Article 
    PubMed 

    Google Scholar 

  • Behler, J. First principles neural network potentials for reactive simulations of large molecular and condensed systems. Angew. Chem. Int. Ed. 56, 12828–12840 (2017).

    Article 
    CAS 

    Google Scholar 

  • Zuo, Y. et al. Performance and cost assessment of machine learning interatomic potentials. J. Phys. Chem. A 124, 731–745 (2020).

    Article 
    PubMed 
    CAS 

    Google Scholar 

  • Huang, S.-D., Shang, C., Zhang, X.-J. & Liu, Z.-P. Material discovery by combining stochastic surface walking global optimization with a neural network. Chem. Sci. 8, 6327–6337 (2017).

    Article 
    PubMed 
    PubMed Central 
    CAS 

    Google Scholar 

  • Ma, S., Shang, C. & Liu, Z.-P. Heterogeneous catalysis from structure to activity via SSW-NN method. J. Chem. Phys. 151, 050901 (2019).

    Article 

    Google Scholar 

  • Wang, H., Zhang, L., Han, J. & E, W. DeePMD-kit: a deep learning package for many-body potential energy representation and molecular dynamics. Comput. Phys. Commun. 228, 178–184 (2018).

    Article 
    CAS 

    Google Scholar 

  • Zhang, Y., Xia, J. & Jiang, B. Physically motivated recursively embedded atom neural networks: incorporating local completeness and nonlocality. Phys. Rev. Lett. 127, 156002 (2021).

    Article 
    PubMed 
    CAS 

    Google Scholar 

  • Batzner, S. et al. E(3)-equivariant graph neural networks for data-efficient and accurate interatomic potentials. Nat. Commun. 13, 2453 (2022).

    Article 
    PubMed 
    PubMed Central 
    CAS 

    Google Scholar 

  • Batatia, I. et al. The design space of E(3)-equivariant atom-centred interatomic potentials. Nat. Mach. Intell. 7, 56–67 (2025).

    Article 
    PubMed 
    PubMed Central 

    Google Scholar 

  • Young, T. A., Johnston-Wood, T., Deringer, V. L. & Duarte, F. A transferable active-learning strategy for reactive molecular force fields. Chem. Sci. 12, 10944–10955 (2021).

    Article 
    PubMed 
    PubMed Central 
    CAS 

    Google Scholar 

  • Smith, J. S. et al. Automated discovery of a robust interatomic potential for aluminum. Nat. Commun. 12, 1257 (2021).

    Article 
    PubMed 
    PubMed Central 
    CAS 

    Google Scholar 

  • Xu, J., Xie, W., Han, Y. & Hu, P. Atomistic insights into the oxidation of flat and stepped platinum surfaces using large-scale machine learning potential-based grand-canonical Monte Carlo. ACS Catal. 12, 14812–14824 (2022).

    Article 
    CAS 

    Google Scholar 

  • Liu, Y. & Guo, H. A Gaussian process based Δ-machine learning approach to reactive potential energy surfaces. J. Phys. Chem. A 127, 8765–8772 (2023).

    Article 
    PubMed 
    CAS 

    Google Scholar 

  • Nandi, A., Qu, C., Houston, P. L., Conte, R. & Bowman, J. M. Δ -machine learning for potential energy surfaces: a PIP approach to bring a DFT-based PES to CCSD(T) level of theory. J. Chem. Phys. 154, 051102 (2021).

    Article 
    PubMed 
    CAS 

    Google Scholar 

  • Morrow, J. D., Gardner, J. L. A. & Deringer, V. L. How to validate machine-learned interatomic potentials. J. Chem. Phys. 158, 121501 (2023).

    Article 
    PubMed 
    CAS 

    Google Scholar 

  • Smith, J. S., Nebgen, B., Lubbers, N., Isayev, O. & Roitberg, A. E. Less is more: sampling chemical space with active learning. J. Chem. Phys. 148, 241733 (2018).

    Article 
    PubMed 

    Google Scholar 

  • Schran, C. et al. Machine learning potentials for complex aqueous systems made simple. Proc. Natl Acad. Sci. USA 118, e2110077118 (2021).

    Article 
    PubMed 
    PubMed Central 
    CAS 

    Google Scholar 

  • Shi, Y.-F., Kang, P.-L., Shang, C. & Liu, Z.-P. Methanol synthesis from CO2/CO mixture on Cu–Zn catalysts from microkinetics-guided machine learning pathway search. J. Am. Chem. Soc. 144, 13401–13414 (2022).

    Article 
    PubMed 
    CAS 

    Google Scholar 

  • Han, Y., Xu, J., Xie, W., Wang, Z. & Hu, P. Comprehensive study of oxygen vacancies on the catalytic performance of ZnO for CO/H2 activation using machine learning-accelerated first-principles simulations. ACS Catal. 13, 5104–5113 (2023).

    Article 
    PubMed 
    PubMed Central 
    CAS 

    Google Scholar 

  • Han, Y., Xu, J., Xie, W., Wang, Z. & Hu, P. Unravelling the impact of metal dopants and oxygen vacancies on syngas conversion over oxides: a machine learning-accelerated study of CO activation on Cr-doped ZnO surfaces. ACS Catal. 13, 15074–15086 (2023).

    Article 
    PubMed 
    PubMed Central 
    CAS 

    Google Scholar 

  • Deringer, V. L., Caro, M. A. & Csányi, G. Machine learning interatomic potentials as emerging tools for materials science. Adv. Mater. 31, 1902765 (2019).

    Article 
    CAS 

    Google Scholar 

  • Luo, L.-H., Huang, S.-D., Shang, C. & Liu, Z.-P. Resolving activation entropy of CO oxidation under the solid–gas and solid–liquid conditions from machine learning simulation. ACS Catal. 12, 6265–6275 (2022).

    Article 
    CAS 

    Google Scholar 

  • Xie, W., Xu, J., Ding, Y. & Hu, P. Quantitative studies of the key aspects in selective acetylene hydrogenation on Pd(111) by microkinetic modeling with coverage effects and molecular dynamics. ACS Catal. 11, 4094–4106 (2021).

    Article 
    CAS 

    Google Scholar 

  • Xie, W., Xu, J., Chen, J., Wang, H. & Hu, P. Achieving theory–experiment parity for activity and selectivity in heterogeneous catalysis using microkinetic modeling. Acc. Chem. Res. 55, 1237–1248 (2022).

    Article 
    PubMed 
    PubMed Central 
    CAS 

    Google Scholar 

  • Deng, B. et al. Systematic softening in universal machine learning interatomic potentials. NPJ Comput. Mater. 11, 9 (2025).

    Article 
    CAS 

    Google Scholar 

  • Zeng, J., Cao, L., Xu, M., Zhu, T. & Zhang, J. Z. H. Complex reaction processes in combustion unraveled by neural network-based molecular dynamics simulation. Nat. Commun. 11, 5713 (2020).

    Article 
    PubMed 
    PubMed Central 
    CAS 

    Google Scholar 

  • Schaaf, L. L., Fako, E., De, S., Schäfer, A. & Csányi, G. Accurate energy barriers for catalytic reaction pathways: an automatic training protocol for machine learning force fields. NPJ Comput. Mater. 9, 180 (2023).

    Article 

    Google Scholar 

  • Bernstein, N., Csányi, G. & Deringer, V. L. De novo exploration and self-guided learning of potential-energy surfaces. NPJ Comput. Mater. 5, 99 (2019).

    Article 

    Google Scholar 

  • Morrow, J. D. & Deringer, V. L. Indirect learning and physically guided validation of interatomic potential models. J. Chem. Phys. 157, 104105 (2022).

    Article 
    PubMed 
    CAS 

    Google Scholar 

  • Zhang, S. et al. Exploring the frontiers of condensed-phase chemistry with a general reactive machine learning potential. Nat. Chem. 16, 727–734 (2024).

    Article 
    PubMed 
    PubMed Central 
    CAS 

    Google Scholar 

  • Chiang, Y. & Benner, P. mace-universal (Revision e5ebd9b). Hugging Face https://doi.org/10.57967/hf/1202 (2023).

  • Liao, Y.-L., Wood, B. M., Das, A. & Smidt, T. EquiformerV2: improved equivariant transformer for scaling to higher-degree representations. In Twelfth International Conference on Learning Representations (2024).

  • Chen, C. & Ong, S. P. A universal graph deep learning interatomic potential for the periodic table. Nat. Comput. Sci. 2, 718–728 (2022).

    Article 
    PubMed 

    Google Scholar 

  • Hauschild, A. et al. Normal-incidence X-ray standing-wave determination of the adsorption geometry of PTCDA on Ag(111): comparison of the ordered room-temperature and disordered low-temperature phases. Phys. Rev. B 81, 125432 (2010).

    Article 

    Google Scholar 

  • Ruiz, V. G., Liu, W., Zojer, E., Scheffler, M. & Tkatchenko, A. Density-functional theory with screened van der Waals Interactions for the modeling of hybrid inorganic–organic systems. Phys. Rev. Lett. 108, 146103 (2012).

    Article 
    PubMed 

    Google Scholar 

  • Eren, B. et al. Activation of Cu(111) surface by decomposition into nanoclusters driven by CO adsorption. Science 351, 475–478 (2016).

    Article 
    PubMed 
    CAS 

    Google Scholar 

  • Xu, L. & Mavrikakis, M. Adsorbate-induced adatom formation on lithium, iron, cobalt, ruthenium, and rhenium surfaces. JACS Au 3, 2216–2225 (2023).

    Article 
    PubMed 
    PubMed Central 
    CAS 

    Google Scholar 

  • Xie, W. & Hu, P. Influence of surface defects on activity and selectivity: a quantitative study of structure sensitivity of Pd catalysts for acetylene hydrogenation. Catal. Sci. Technol. 11, 5212–5222 (2021).

    Article 
    CAS 

    Google Scholar 

  • Wu, J., Chen, D., Chen, J. & Wang, H. Structural and composition evolution of palladium catalyst for CO oxidation under steady-state reaction conditions. J. Phys. Chem. C 127, 6262–6270 (2023).

    Article 
    CAS 

    Google Scholar 

  • Li, X.-T., Chen, L., Shang, C. & Liu, Z.-P. In situ surface structures of PdAg catalyst and their influence on acetylene semihydrogenation revealed by machine learning and experiment. J. Am. Chem. Soc. 143, 6281–6292 (2021).

    Article 
    PubMed 
    CAS 

    Google Scholar 

  • Baker, J. & Chan, F. The location of transition states: a comparison of Cartesian, Z-matrix, and natural internal coordinates. J. Comput. Chem. 17, 888–904 (1996).

    Article 
    CAS 

    Google Scholar 

  • Cordero, B. et al. Covalent radii revisited. Dalton Trans. https://doi.org/10.1039/B801115J (2008).

  • Bartók, A. P., Kondor, R. & Csányi, G. On representing chemical environments. Phys. Rev. B 87, 184115 (2013).

    Article 

    Google Scholar 

  • Behler, J. Atom-centered symmetry functions for constructing high-dimensional neural network potentials. J. Chem. Phys. 134, 074106 (2011).

    Article 
    PubMed 

    Google Scholar 

  • Thompson, A. P., Swiler, L. P., Trott, C. R., Foiles, S. M. & Tucker, G. J. Spectral neighbor analysis method for automated generation of quantum-accurate interatomic potentials. J. Comput. Phys. 285, 316–330 (2015).

    Article 
    CAS 

    Google Scholar 

  • Mahoney, M. W. & Drineas, P. CUR matrix decompositions for improved data analysis. Proc. Natl Acad. Sci. USA 106, 697–702 (2009).

    Article 
    PubMed 
    PubMed Central 
    CAS 

    Google Scholar 

  • Harris, C. R. et al. Array programming with NumPy. Nature 585, 357–362 (2020).

    Article 
    PubMed 
    PubMed Central 
    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).

    Article 
    CAS 

    Google Scholar 

  • Perdew, J. P. et al. Restoring the density-gradient expansion for exchange in solids and surfaces. Phys. Rev. Lett. 100, 136406 (2008).

    Article 
    PubMed 

    Google Scholar 

  • Kresse, G. & Joubert, D. From ultrasoft pseudopotentials to the projector augmented-wave method. Phys. Rev. B 59, 1758–1775 (1999).

    Article 
    CAS 

    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).

    Article 
    PubMed 

    Google Scholar 

  • Thompson, A. P. et al. LAMMPS—a flexible simulation tool for particle-based materials modeling at the atomic, meso, and continuum scales. Comput. Phys. Commun. 271, 108171 (2022).

    Article 
    CAS 

    Google Scholar 

  • Steinhardt, P. J., Nelson, D. R. & Ronchetti, M. Bond-orientational order in liquids and glasses. Phys. Rev. B 28, 784–805 (1983).

    Article 
    CAS 

    Google Scholar 

  • Menon, S., Leines, G. & Rogal, J. pyscal: a Python module for structural analysis of atomic environments. J. Open Source Softw. 4, 1824 (2019).

    Article 

    Google Scholar 

  • Larsen, A. H. et al. The atomic simulation environment—a Python library for working with atoms. J. Phys. Condens. Matter 29, 273002 (2017).

    Article 

    Google Scholar 

  • Wang, H.-F. & Liu, Z.-P. Comprehensive mechanism and structure-sensitivity of ethanol oxidation on platinum: new transition-state searching method for resolving the complex reaction network. J. Am. Chem. Soc. 130, 10996–11004 (2008).

    Article 
    PubMed 
    CAS 

    Google Scholar 

  • Henkelman, G., Uberuaga, B. P. & Jónsson, H. A climbing image nudged elastic band method for finding saddle points and minimum energy paths. J. Chem. Phys. 113, 9901–9904 (2000).

    Article 
    CAS 

    Google Scholar 

  • Xie, W. Electronic structure calculations. Figshare https://doi.org/10.6084/m9.figshare.29484686.v1 (2025).



  • Source link

    Leave a Reply

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