Efficient Kr/Xe separation from triangular g-C3N4 nanopores: density-functional theory calculations benchmarked with random phase approximation


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{
  "id": "735", 
  "metadata": {
    "title": "Efficient Kr/Xe separation from triangular g-C3N4 nanopores: density-functional theory calculations benchmarked with random phase approximation", 
    "doi": "10.24435/materialscloud:vp-ms", 
    "license": "Creative Commons Attribution 4.0 International", 
    "keywords": [
      "carbon nitrides", 
      "nanoscale transport", 
      "density-functional theory", 
      "random phase approximation", 
      "van-der-Waals approximations", 
      "MARVEL", 
      "EPFL", 
      "SNSF", 
      "CSCS"
    ], 
    "contributors": [
      {
        "affiliations": [
          "Laboratory of Advanced Separations (LAS), \u00c9cole Polytechnique F\u00e9d\u00e9rale de Lausanne (EPFL), Switzerland", 
          "Theory and Simulation of Materials (THEOS) and National Centre for Computational Design and Discovery of Novel Materials (MARVEL), EPFL, Lausanne, Switzerland"
        ], 
        "familyname": "Tohidivahdat", 
        "email": "mohammad.vahdat@epfl.ch", 
        "givennames": "Mohammad"
      }, 
      {
        "affiliations": [
          "Theory and Simulation of Materials (THEOS) and National Centre for Computational Design and Discovery of Novel Materials (MARVEL), EPFL, Lausanne, Switzerland"
        ], 
        "familyname": "Campi", 
        "email": "davide.campi@epfl.ch", 
        "givennames": "Davide"
      }, 
      {
        "affiliations": [
          "Theory and Simulation of Materials (THEOS) and National Centre for Computational Design and Discovery of Novel Materials (MARVEL), EPFL, Lausanne, Switzerland", 
          "Laboratory for Neutron Scattering and Imaging (LSN), Paul Scherrer Institute, 5232 Villigen PSI, Switzerland"
        ], 
        "familyname": "Colonna", 
        "email": "nicola.colonna@psi.ch", 
        "givennames": "Nicola"
      }, 
      {
        "affiliations": [
          "Laboratory of Advanced Separations (LAS), \u00c9cole Polytechnique F\u00e9d\u00e9rale de Lausanne (EPFL), Switzerland"
        ], 
        "familyname": "Villalobos", 
        "email": "francisco.villalobos@epfl.ch", 
        "givennames": "Luis Francisco"
      }, 
      {
        "affiliations": [
          "Theory and Simulation of Materials (THEOS) and National Centre for Computational Design and Discovery of Novel Materials (MARVEL), EPFL, Lausanne, Switzerland"
        ], 
        "familyname": "Marzari", 
        "email": "nicola.marzari@epfl.ch", 
        "givennames": "Nicola"
      }, 
      {
        "affiliations": [
          "Laboratory of Advanced Separations (LAS), \u00c9cole Polytechnique F\u00e9d\u00e9rale de Lausanne (EPFL), Switzerland"
        ], 
        "familyname": "Agrawal Varoon", 
        "email": "kumar.agrawal@epfl.ch", 
        "givennames": "Kumar"
      }
    ], 
    "_files": [
      {
        "description": "It explains what is inside the folder", 
        "checksum": "md5:6320b4df670c86d6370c1c29080ad749", 
        "size": 2133, 
        "key": "README.txt"
      }, 
      {
        "description": "Contains all the DFT and RPA calculations", 
        "checksum": "md5:a4eee83dbe3c8c16efddd3232a590a30", 
        "size": 26439694, 
        "key": "Calculations.zip"
      }
    ], 
    "references": [
      {
        "type": "Journal reference", 
        "doi": "10.1039/D0TA03071F", 
        "citation": "M. T. Vahdat, D. Campi, N. Colonna, L. F. Villalobos, N. Marzari, K. V. Agrawal, J. Mater. Chem. A, 8, 17747\u201317755 (2020).", 
        "url": "https://pubs.rsc.org/fa/content/articlehtml/2020/ta/d0ta03071f"
      }
    ], 
    "conceptrecid": "734", 
    "version": 1, 
    "edited_by": 100, 
    "id": "735", 
    "owner": 304, 
    "mcid": "2021.30", 
    "is_last": true, 
    "status": "published", 
    "description": "Poly(triazine imide) or PTI is a promising material for molecular sieving membranes, thanks to its atom-thick ordered lattice with an extremely high density (1.6 \u00d7 10^14 pores/cm2) of triangular-shaped nanopores of ~0.34 nm diameter. Here, we investigate the application of PTI nanopores in the purification of Kr from Xe to reduce the storage volume of the mixture of 85Kr/Xe. Using van-der-Waals density-functional theory (vdW-DFT) calculations, benchmarked against the random phase approximation (RPA), we calculate the potential energy profiles for Kr and Xe across the nanopores. For each gas, starting from the RPA potential-energy profile, the force-field parameters to be used in the classical molecular dynamics framework are trained to calculate the Helmholtz free energy barrier as a function of temperature, and therefore, the corresponding entropic loss. Overall, due to the much higher activation energy from the adsorbed state in Xe (17.61 and 42.10 kJ/mole for Kr and Xe, respectively), a large Kr/Xe separation selectivity is postulated from the PTI membrane. Furthermore, the combination of atom-thick PTI lattice and high pore density leads to extremely large yet selective permeances for Kr. For example, Kr permeance of 1000 gas permeation units (GPU) accompanying a large Kr/Xe selectivity (>10000) is calculated at 25 \u00b0C, significantly better than the state-of-the-art membranes for Kr/Xe separation, making PTI-based membranes a leading candidate to process the hazardous waste of 85Kr/Xe mixture.", 
    "license_addendum": null, 
    "_oai": {
      "id": "oai:materialscloud.org:735"
    }, 
    "publication_date": "Feb 07, 2021, 21:34:51"
  }, 
  "revision": 6, 
  "updated": "2021-02-07T20:34:51.925729+00:00", 
  "created": "2021-01-27T14:24:05.095190+00:00"
}