IDEAS home Printed from https://ideas.repec.org/a/nat/natcom/v15y2024i1d10.1038_s41467-024-48609-2.html
   My bibliography  Save this article

A reactive neural network framework for water-loaded acidic zeolites

Author

Listed:
  • Andreas Erlebach

    (Charles University)

  • Martin Šípka

    (Charles University
    Charles University)

  • Indranil Saha

    (Charles University)

  • Petr Nachtigall

    (Charles University)

  • Christopher J. Heard

    (Charles University)

  • Lukáš Grajciar

    (Charles University)

Abstract

Under operating conditions, the dynamics of water and ions confined within protonic aluminosilicate zeolite micropores are responsible for many of their properties, including hydrothermal stability, acidity and catalytic activity. However, due to high computational cost, operando studies of acidic zeolites are currently rare and limited to specific cases and simplified models. In this work, we have developed a reactive neural network potential (NNP) attempting to cover the entire class of acidic zeolites, including the full range of experimentally relevant water concentrations and Si/Al ratios. This NNP has the potential to dramatically improve sampling, retaining the (meta)GGA DFT level accuracy, with the capacity for discovery of new chemistry, such as collective defect formation mechanisms at the zeolite surface. Furthermore, we exemplify how the NNP can be used as a basis for further extensions/improvements which include data-efficient adoption of higher-level (hybrid) references via Δ-learning and the acceleration of rare event sampling via automatic construction of collective variables. These developments represent a significant step towards accurate simulations of realistic catalysts under operando conditions.

Suggested Citation

  • Andreas Erlebach & Martin Šípka & Indranil Saha & Petr Nachtigall & Christopher J. Heard & Lukáš Grajciar, 2024. "A reactive neural network framework for water-loaded acidic zeolites," Nature Communications, Nature, vol. 15(1), pages 1-14, December.
  • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-48609-2
    DOI: 10.1038/s41467-024-48609-2
    as

    Download full text from publisher

    File URL: https://www.nature.com/articles/s41467-024-48609-2
    File Function: Abstract
    Download Restriction: no

    File URL: https://libkey.io/10.1038/s41467-024-48609-2?utm_source=ideas
    LibKey link: if access is restricted and if your library uses this service, LibKey will redirect you to where you can use your library subscription to access this item
    ---><---

    References listed on IDEAS

    as
    1. Christopher J. Heard & Lukas Grajciar & Cameron M. Rice & Suzi M. Pugh & Petr Nachtigall & Sharon E. Ashbrook & Russell E. Morris, 2019. "Fast room temperature lability of aluminosilicate zeolites," Nature Communications, Nature, vol. 10(1), pages 1-7, December.
    2. Simon Batzner & Albert Musaelian & Lixin Sun & Mario Geiger & Jonathan P. Mailoa & Mordechai Kornbluth & Nicola Molinari & Tess E. Smidt & Boris Kozinsky, 2022. "E(3)-equivariant graph neural networks for data-efficient and accurate interatomic potentials," Nature Communications, Nature, vol. 13(1), pages 1-11, December.
    3. Matteo Fasano & Thomas Humplik & Alessio Bevilacqua & Michael Tsapatsis & Eliodoro Chiavazzo & Evelyn N. Wang & Pietro Asinari, 2016. "Interplay between hydrophilicity and surface barriers on water transport in zeolite membranes," Nature Communications, Nature, vol. 7(1), pages 1-8, November.
    4. So Takamoto & Chikashi Shinagawa & Daisuke Motoki & Kosuke Nakago & Wenwen Li & Iori Kurata & Taku Watanabe & Yoshihiro Yayama & Hiroki Iriguchi & Yusuke Asano & Tasuku Onodera & Takafumi Ishii & Taka, 2022. "Towards universal neural network potential for material discovery applicable to arbitrary combination of 45 elements," Nature Communications, Nature, vol. 13(1), pages 1-11, December.
    5. Massimo Bocus & Ruben Goeminne & Aran Lamaire & Maarten Cools-Ceuppens & Toon Verstraelen & Veronique Van Speybroeck, 2023. "Nuclear quantum effects on zeolite proton hopping kinetics explored with machine learning potentials and path integral molecular dynamics," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    6. Jonathan Vandermause & Yu Xie & Jin Soo Lim & Cameron J. Owen & Boris Kozinsky, 2022. "Active learning of reactive Bayesian force fields applied to heterogeneous catalysis dynamics of H/Pt," Nature Communications, Nature, vol. 13(1), pages 1-12, December.
    Full references (including those not matched with items on IDEAS)

    Citations

    Citations are extracted by the CitEc Project, subscribe to its RSS feed for this item.
    as


    Cited by:

    1. Swagata Roy & Johannes P. Dürholt & Thomas S. Asche & Federico Zipoli & Rafael Gómez-Bombarelli, 2024. "Learning a reactive potential for silica-water through uncertainty attribution," Nature Communications, Nature, vol. 15(1), pages 1-10, December.

    Most related items

    These are the items that most often cite the same works as this one and are cited by the same works as this one.
    1. Li Zheng & Konstantinos Karapiperis & Siddhant Kumar & Dennis M. Kochmann, 2023. "Unifying the design space and optimizing linear and nonlinear truss metamaterials by generative modeling," Nature Communications, Nature, vol. 14(1), pages 1-14, December.
    2. Katja-Sophia Csizi & Miguel Steiner & Markus Reiher, 2024. "Nanoscale chemical reaction exploration with a quantum magnifying glass," Nature Communications, Nature, vol. 15(1), pages 1-15, December.
    3. J. Thorben Frank & Oliver T. Unke & Klaus-Robert Müller & Stefan Chmiela, 2024. "A Euclidean transformer for fast and stable machine learned force fields," Nature Communications, Nature, vol. 15(1), pages 1-16, December.
    4. Yaolong Zhang & Bin Jiang, 2023. "Universal machine learning for the response of atomistic systems to external fields," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    5. Wei Lu & Jixian Zhang & Weifeng Huang & Ziqiao Zhang & Xiangyu Jia & Zhenyu Wang & Leilei Shi & Chengtao Li & Peter G. Wolynes & Shuangjia Zheng, 2024. "DynamicBind: predicting ligand-specific protein-ligand complex structure with a deep equivariant generative model," Nature Communications, Nature, vol. 15(1), pages 1-13, December.
    6. Adil Kabylda & Valentin Vassilev-Galindo & Stefan Chmiela & Igor Poltavsky & Alexandre Tkatchenko, 2023. "Efficient interatomic descriptors for accurate machine learning force fields of extended molecules," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    7. Junjie Wang & Yong Wang & Haoting Zhang & Ziyang Yang & Zhixin Liang & Jiuyang Shi & Hui-Tian Wang & Dingyu Xing & Jian Sun, 2024. "E(n)-Equivariant cartesian tensor message passing interatomic potential," Nature Communications, Nature, vol. 15(1), pages 1-9, December.
    8. Alessio Fallani & Leonardo Medrano Sandonas & Alexandre Tkatchenko, 2024. "Inverse mapping of quantum properties to structures for chemical space of small organic molecules," Nature Communications, Nature, vol. 15(1), pages 1-14, December.
    9. Kangming Li & Daniel Persaud & Kamal Choudhary & Brian DeCost & Michael Greenwood & Jason Hattrick-Simpers, 2023. "Exploiting redundancy in large materials datasets for efficient machine learning with less data," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    10. Xiaoxun Gong & He Li & Nianlong Zou & Runzhang Xu & Wenhui Duan & Yong Xu, 2023. "General framework for E(3)-equivariant neural network representation of density functional theory Hamiltonian," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    11. Rishi Verma & Charvi Singhvi & Amrit Venkatesh & Vivek Polshettiwar, 2024. "Defects tune the acidic strength of amorphous aluminosilicates," Nature Communications, Nature, vol. 15(1), pages 1-16, December.
    12. Yusong Wang & Tong Wang & Shaoning Li & Xinheng He & Mingyu Li & Zun Wang & Nanning Zheng & Bin Shao & Tie-Yan Liu, 2024. "Enhancing geometric representations for molecules with equivariant vector-scalar interactive message passing," Nature Communications, Nature, vol. 15(1), pages 1-13, December.
    13. Rama Oktavian & Ruben Goeminne & Lawson T. Glasby & Ping Song & Racheal Huynh & Omid Taheri Qazvini & Omid Ghaffari-Nik & Nima Masoumifard & Joan L. Cordiner & Pierre Hovington & Veronique Speybroeck , 2024. "Gas adsorption and framework flexibility of CALF-20 explored via experiments and simulations," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    14. Lucien F. Krapp & Luciano A. Abriata & Fabio Cortés Rodriguez & Matteo Dal Peraro, 2023. "PeSTo: parameter-free geometric deep learning for accurate prediction of protein binding interfaces," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    15. Ziduo Yang & Yi-Ming Zhao & Xian Wang & Xiaoqing Liu & Xiuying Zhang & Yifan Li & Qiujie Lv & Calvin Yu-Chian Chen & Lei Shen, 2024. "Scalable crystal structure relaxation using an iteration-free deep generative model with uncertainty quantification," Nature Communications, Nature, vol. 15(1), pages 1-15, December.
    16. Fasano, Matteo & Morciano, Matteo & Bergamasco, Luca & Chiavazzo, Eliodoro & Zampato, Massimo & Carminati, Stefano & Asinari, Pietro, 2021. "Deep-sea reverse osmosis desalination for energy efficient low salinity enhanced oil recovery," Applied Energy, Elsevier, vol. 304(C).
    17. Chao Liang & Yilimiranmu Rouzhahong & Caiyuan Ye & Chong Li & Biao Wang & Huashan Li, 2023. "Material symmetry recognition and property prediction accomplished by crystal capsule representation," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    18. Zechen Tang & He Li & Peize Lin & Xiaoxun Gong & Gan Jin & Lixin He & Hong Jiang & Xinguo Ren & Wenhui Duan & Yong Xu, 2024. "A deep equivariant neural network approach for efficient hybrid density functional calculations," Nature Communications, Nature, vol. 15(1), pages 1-9, December.
    19. Albert Musaelian & Simon Batzner & Anders Johansson & Lixin Sun & Cameron J. Owen & Mordechai Kornbluth & Boris Kozinsky, 2023. "Learning local equivariant representations for large-scale atomistic dynamics," Nature Communications, Nature, vol. 14(1), pages 1-15, December.
    20. Cameron J. Owen & Yu Xie & Anders Johansson & Lixin Sun & Boris Kozinsky, 2024. "Low-index mesoscopic surface reconstructions of Au surfaces using Bayesian force fields," Nature Communications, Nature, vol. 15(1), pages 1-13, December.

    More about this item

    Statistics

    Access and download statistics

    Corrections

    All material on this site has been provided by the respective publishers and authors. You can help correct errors and omissions. When requesting a correction, please mention this item's handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-48609-2. See general information about how to correct material in RePEc.

    If you have authored this item and are not yet registered with RePEc, we encourage you to do it here. This allows to link your profile to this item. It also allows you to accept potential citations to this item that we are uncertain about.

    If CitEc recognized a bibliographic reference but did not link an item in RePEc to it, you can help with this form .

    If you know of missing items citing this one, you can help us creating those links by adding the relevant references in the same way as above, for each refering item. If you are a registered author of this item, you may also want to check the "citations" tab in your RePEc Author Service profile, as there may be some citations waiting for confirmation.

    For technical questions regarding this item, or to correct its authors, title, abstract, bibliographic or download information, contact: Sonal Shukla or Springer Nature Abstracting and Indexing (email available below). General contact details of provider: http://www.nature.com .

    Please note that corrections may take a couple of weeks to filter through the various RePEc services.

    IDEAS is a RePEc service. RePEc uses bibliographic data supplied by the respective publishers.