Building a consistent and reproducible database for adsorption evaluation in Covalent-Organic Frameworks

Authors: Daniele Ongari1*, Aliaksandr V. Yakutovich2, Leopold Talirz2, Berend Smit1

  1. Institut des Sciences et Ingénierie Chimiques, École Polytechnique Fédérale de Lausanne (EPFL), CH-1951 Sion, Valais, Switzerland
  2. Institut des Sciences et Ingénierie Chimiques, École Polytechnique Fédérale de Lausanne (EPFL), CH-1951 Sion, Valais, Switzerland and Laboratory of Molecular Simulation (LSMO), Institut des Sciences et Ingénierie Chimiques, Ecole Polytechnique Fédérale de Lausanne (EPFL), Rue de l'Industrie 17, CH-1951 Sion, Valais, Switzerland
  • Corresponding author email: daniele.ongari@epfl.ch

DOI10.24435/materialscloud:2019.0034/v1 (version v1, submitted on 25 June 2019)

How to cite this entry

Daniele Ongari, Aliaksandr V. Yakutovich, Leopold Talirz, Berend Smit, Building a consistent and reproducible database for adsorption evaluation in Covalent-Organic Frameworks, Materials Cloud Archive (2019), doi: 10.24435/materialscloud:2019.0034/v1.

Description

We present a workflow that traces the path from the bulk structure of a crystalline material to assessing its performance in carbon capture from coal's post-combustion flue gases. We apply the workflow to a database of 324 covalent-organic frameworks (COFs) reported in the literature to characterize their CO2 adsorption properties using the following steps:
(1) optimization of the crystal structure (atomic positions and cell) using density functional theory,
(2) fitting atomic point charges based on the electron density,
(3) characterizing the (pore) geometry of the structures before and after optimization,
(4) computing carbon dioxide and nitrogen isotherms using grand canonical Monte Carlo simulations (empirical interaction potential) and, finally,
(5) assessing the CO2 parasitic energy via process modelling.

The full workflow has been encoded in the Automated Interactive Infrastructure and Database for Computational Science (AiiDA). Both the workflow and the automatically generated provenance graph of our calculations are made available on the Materials Cloud, allowing peers to inspect inspect every input parameter and result along the workflow, download structures and files at intermediate stages and start their research right from where this work has left off.
In particular, our set of CURATED COFs with optimized geometry and high quality DFT-derived point charges is available for further investigations of gas adsorption properties. We plan to update the database as new COFs are being reported.

Materials Cloud sections using this data

Files

File name Size Description
cofs_export_v2.aiida
MD5MD5: 42eca1f997fd87aaa496e318c5755801
902.4 MiB AiiDA provenance graph exported using aiida-core 0.12.3
cifs_cellopt.zip
MD5MD5: dd81deab100ea58d49f2cae6c2113e5b
1.6 MiB CIF files with DFT-optimized coordinates/unit cell and atomic DDEC charges.
workchains.zip
MD5MD5: 32ea8b1828559804acca94d248153164
15.5 KiB AiiDA workchains for:
1) DFT-optimization (three stages protocol) and DDEC charges evaluation
2) Calculation of CO2 and N2 isotherms
3) Evaluation of minimal CO2 parasitic energy for post combustion

License

Files and data are licensed under the terms of the following license: Creative Commons Attribution 4.0 International.

External references

Journal reference
Paper submitted.

Keywords

MARVEL covalent-organic-framework Reproducibility AiiDA Workflows

Version history

25 June 2019 [This version]