Adsorbate chemical environment-based machine learning framework for heterogeneous catalysis

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  "metadata": {
    "edited_by": 576, 
    "owner": 714, 
    "description": "Heterogeneous catalytic reactions are influenced by a subtle interplay of atomic-scale factors, ranging from the catalysts\u2019 local morphology to the presence of high adsorbate coverages. Describing such phenomena via computational models requires generation and analysis of a large space of surface atomic configurations. To address this challenge, we present the Adsorbate Chemical Environment-based Graph Convolution Neural Network (ACE-GCN), a screening workflow that can account for atomistic configurations comprising diverse adsorbates, binding locations, coordination environments, and substrate morphologies. Using this workflow, we develop catalyst surface models for two illustrative systems: (i) NO adsorbed on a Pt3Sn(111) alloy surface, of interest for nitrate electroreduction processes, where high adsorbate coverages combine with the low symmetry of the alloy substrate to produce a large configurational space, and (ii) OH* adsorbed on a stepped Pt(221) facet, of relevance to the Oxygen Reduction Reaction, wherein the presence of irregular crystal surfaces, high adsorbate coverages, and directionally-dependent adsorbate-adsorbate interactions result in the configurational complexity. In both cases, the ACE-GCN model, having trained on a fraction (~10%) of the total DFT-relaxed configurations, successfully ranks the relative stabilities of unrelaxed atomic configurations sampled from a large configurational space. This approach is expected to accelerate development of rigorous descriptions of catalyst surfaces under in-situ conditions.", 
    "keywords": [
      "density-functional theory", 
      "machine learning", 
      "electronic structure"
    ], 
    "is_last": true, 
    "title": "Adsorbate chemical environment-based machine learning framework for heterogeneous catalysis", 
    "status": "published", 
    "license_addendum": null, 
    "doi": "10.24435/materialscloud:td-hf", 
    "conceptrecid": "1305", 
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        "description": "Raw files (graph objects and atom trajectories) for Pt-OH analysis", 
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    "references": [
      {
        "citation": "Ghanekar P, Deshpande S, Greeley J. Adsorbate chemical environment-based machine learning framework for heterogeneous catalysis. ChemRxiv. Cambridge: Cambridge Open Engage; 2021", 
        "comment": "Preprint version of the manuscript where the data is discussed", 
        "url": "https://chemrxiv.org/engage/chemrxiv/article-details/60f5d5bf7bf0c92ab45f6c29", 
        "doi": "10.26434/chemrxiv-2021-8fcxm", 
        "type": "Preprint"
      }
    ], 
    "contributors": [
      {
        "givennames": "Pushkar", 
        "affiliations": [
          "Davidson School of Chemical Engineering, Purdue University, West Lafayette, Indiana 47907, USA"
        ], 
        "familyname": "Ghanekar", 
        "email": "pghaneka@purdue.edu"
      }, 
      {
        "givennames": "Siddharth", 
        "affiliations": [
          "Davidson School of Chemical Engineering, Purdue University, West Lafayette, Indiana 47907, USA", 
          "Department of Chemical Engineering, University of Delaware, Newark, DE"
        ], 
        "familyname": "Deshpande", 
        "email": "sdeshpan@udel.edu"
      }, 
      {
        "givennames": "Jeffrey", 
        "affiliations": [
          "Davidson School of Chemical Engineering, Purdue University, West Lafayette, Indiana 47907, USA"
        ], 
        "familyname": "Greeley", 
        "email": "jgreeley@purdue.edu"
      }
    ], 
    "_oai": {
      "id": "oai:materialscloud.org:1306"
    }, 
    "publication_date": "Apr 11, 2022, 14:37:43", 
    "mcid": "2022.50", 
    "version": 1, 
    "id": "1306", 
    "license": "MIT License"
  }, 
  "revision": 4, 
  "created": "2022-04-03T21:06:39.671159+00:00", 
  "id": "1306", 
  "updated": "2022-04-11T12:37:43.529364+00:00"
}