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{
"metadata": {
"edited_by": 576,
"owner": 643,
"_oai": {
"id": "oai:materialscloud.org:2064"
},
"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.",
"mcid": "2024.15",
"id": "2064",
"license": "Creative Commons Attribution 4.0 International",
"license_addendum": null,
"references": [
{
"citation": "S. Das, R. Laplaza, J.T. Blaskovits, C. Corminboeuf, ChemRxiv (2023)",
"type": "Preprint",
"url": "https://chemrxiv.org/engage/chemrxiv/article-details/641c2dcf647e3dca995edf4f",
"comment": "Preprint where the data is discussed.",
"doi": "https://doi.org/10.26434/chemrxiv-2023-09mdd"
}
],
"doi": "10.24435/materialscloud:dq-z3",
"keywords": [
"catalysis",
"volcano plot",
"frustrated lewis pairs",
"molecular catalysts",
"metal-organic frameworks",
"EPFL"
],
"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"
},
{
"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",
"email": "clemence.corminboeuf@epfl.ch",
"givennames": "Clemence"
}
],
"conceptrecid": "1733",
"version": 2,
"publication_date": "Jan 29, 2024, 19:10:10",
"is_last": false,
"status": "published",
"_files": [
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"checksum": "md5:d68d80db815226438d37f78c103de3ba",
"description": "README file detailing the contents of this record.",
"key": "README.txt"
},
{
"size": 59035,
"checksum": "md5:54514429171569ae3472ea159d184cbb",
"description": "Chemiscope file containing the properties and structures of the final BPh2 functionalized linkers.",
"key": "I2-BPh2-final_chemiscope.json.gz"
},
{
"size": 4987,
"checksum": "md5:2051f8702b5c42c3046f3fbe43b3a0f1",
"description": "Chemiscope file containing the properties and structures of the final BMe2 functionalized linkers.",
"key": "I2-BMe2-final_chemiscope.json.gz"
},
{
"size": 26372,
"checksum": "md5:66ba60e0a3024cad111f39cf3b66d140",
"description": "Chemiscope file containing the properties and structures of the final BBN functionalized linkers.",
"key": "I2-BBN-final_chemiscope.json.gz"
},
{
"size": 5745,
"checksum": "md5:635f6deebd73b7c4ab6566bf3557f3d9",
"description": "CSV file containing the tabulated properties for the final BPh2-functionalized linkers.",
"key": "I2-BPh2-final.csv"
},
{
"size": 532,
"checksum": "md5:d98097fb743d73b81e6ff018be41cd90",
"description": "CSV file containing the tabulated properties for the final BMe2-functionalized linkers.",
"key": "I2-BMe2-final.csv"
},
{
"size": 2707,
"checksum": "md5:0b2b945e3a53be0b2427f90a949d65e6",
"description": "CSV file containing the tabulated properties for the final BBN-functionalized linkers.",
"key": "I2-BBN-final.csv"
},
{
"size": 14885250,
"checksum": "md5:22ce2481629f337f5baf28295a55bbcf",
"description": "Compressed file with all the XYZ files of the filtered, pre and post screened I2 of the functionalized linkers.",
"key": "I2.tar.gz"
},
{
"size": 17206812,
"checksum": "md5:b4df3718fe70c9456697cc53415a175c",
"description": "Compressed file with all the XYZ files of the filtered functionalized linkers.",
"key": "LPAS.tar.gz"
},
{
"size": 31196641,
"checksum": "md5:dbf1118341b6add829acf456ce5cb44e",
"description": "Compressed file with all the XYZ files of the functionalized linkers.",
"key": "DL-database.tar.gz"
},
{
"size": 774285,
"checksum": "md5:64128ee5d2b44ed2854639b9522715ef",
"description": "Compressed file with all the XYZ files of the initial N-containing linkers.",
"key": "seed-database.tar.gz"
},
{
"size": 6679,
"checksum": "md5:3f1f769af8f50f9efacffa2791359107",
"description": "Notebook exemplifying how the provided XYZ structures and csv files can be combined to generate the Chemiscope json files.",
"key": "chemiscopify.ipynb"
},
{
"size": 1133719,
"checksum": "md5:e080b276abd94560ed14ca6fd95c5cae",
"description": "Predicted PLD for the functionalized linkers.",
"key": "predicted_PLD.csv"
}
],
"title": "Engineering frustrated lewis pair active sites in porous organic scaffolds for catalytic CO\u2082 hydrogenation"
},
"id": "2064",
"updated": "2024-04-17T14:51:19.876688+00:00",
"created": "2024-01-26T16:05:32.123474+00:00",
"revision": 3
}