Engineering frustrated lewis pair active sites in porous organic scaffolds for catalytic CO₂ hydrogenation
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"revision": 3,
"id": "2145",
"created": "2024-04-17T14:10:41.132420+00:00",
"metadata": {
"doi": "10.24435/materialscloud:90-b6",
"status": "published",
"title": "Engineering frustrated lewis pair active sites in porous organic scaffolds for catalytic CO\u2082 hydrogenation",
"mcid": "2024.58",
"license_addendum": null,
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"owner": 643,
"_oai": {
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"keywords": [
"catalysis",
"volcano plot",
"frustrated lewis pairs",
"molecular catalysts",
"metal-organic frameworks",
"EPFL"
],
"conceptrecid": "1733",
"is_last": true,
"references": [
{
"type": "Preprint",
"doi": "https://doi.org/10.26434/chemrxiv-2023-09mdd",
"url": "https://chemrxiv.org/engage/chemrxiv/article-details/641c2dcf647e3dca995edf4f",
"comment": "Preprint where the data is discussed.",
"citation": "S. Das, R. Laplaza, J.T. Blaskovits, C. Corminboeuf, ChemRxiv (2023)"
}
],
"publication_date": "Apr 17, 2024, 16:51:19",
"license": "Creative Commons Attribution 4.0 International",
"id": "2145",
"description": "Frustrated Lewis pairs (FLPs), featuring reactive combinations of Lewis acids and Lewis bases, have been utilized for myriad metal-free homogeneous catalytic processes. Immobilizing the active Lewis sites to a solid support, especially to porous scaffolds, has shown great potential to ameliorate FLP catalysis by circumventing some of its inherent drawbacks, such as product separation and catalyst recyclability. Nevertheless, designing immobilized Lewis pair active sites (LPASs) is challenging due to the requirement of placing the donor and acceptor centers in appropriate geometric arrangements while maintaining the necessary chemical environment to perform catalysis, and clear design rules have not yet been established. In this work, we formulate simple guidelines to build highly active LPASs for direct catalytic hydrogenation of CO\u2082 through a large-scale screening of a diverse library of 25,000 immobilized FLPs. \nThe library is built by introducing boron-containing acidic sites in the vicinity of the existing basic nitrogen sites of the organic linkers of metal-organic frameworks collected in a \"top-down\" fashion from an experimental database. The chemical and geometrical appropriateness of these LPASs for CO\u2082 hydrogenation is determined by evaluating a series of simple descriptors representing the intrinsic strength (acidity and basicity) of the components and their spatial arrangement in the active sites. Analysis of the leading candidates enables the formulation of pragmatic and experimentally-relevant design principles and they constitute the starting point for further exploration of FLP-based catalysts for the reduction of CO\u2082.",
"version": 3,
"contributors": [
{
"affiliations": [
"Laboratory for Computational Molecular Design (LCMD), Institute of Chemical Sciences and Engineering (ISIC), \u00c9cole Polytechnique F\u00e9d\u00e9rale de Lausanne (EPFL), CH-1015 Lausanne, Switzerland"
],
"familyname": "Das",
"givennames": "Shubhajit"
},
{
"affiliations": [
"Laboratory for Computational Molecular Design (LCMD), Institute of Chemical Sciences and Engineering (ISIC), \u00c9cole Polytechnique F\u00e9d\u00e9rale de Lausanne (EPFL), CH-1015 Lausanne, Switzerland",
"National Center for Competence in Research \u2013 Catalysis (NCCR-Catalysis), Ecole Polytechnique F\u00e9d\u00e9rale de Lausanne (EPFL), 1015 Lausanne, Switzerland"
],
"familyname": "Laplaza",
"givennames": "Ruben"
},
{
"affiliations": [
"Laboratory for Computational Molecular Design (LCMD), Institute of Chemical Sciences and Engineering (ISIC), \u00c9cole Polytechnique F\u00e9d\u00e9rale de Lausanne (EPFL), CH-1015 Lausanne, Switzerland"
],
"familyname": "Blaskovits",
"givennames": "J. Terence"
},
{
"email": "clemence.corminboeuf@epfl.ch",
"affiliations": [
"Laboratory for Computational Molecular Design (LCMD), Institute of Chemical Sciences and Engineering (ISIC), \u00c9cole Polytechnique F\u00e9d\u00e9rale de Lausanne (EPFL), CH-1015 Lausanne, Switzerland",
"National Center for Competence in Research \u2013 Catalysis (NCCR-Catalysis), Ecole Polytechnique F\u00e9d\u00e9rale de Lausanne (EPFL), 1015 Lausanne, Switzerland"
],
"familyname": "Corminboeuf",
"givennames": "Clemence"
}
],
"edited_by": 643
},
"updated": "2024-07-01T14:56:25.919818+00:00"
}