Structure and electronic properties of rare earth DOBDC metal–organic-frameworks

Vogel, Dayton J.; Sava Gallis, Dorina F.; Nenoff, Tina M.; Rimsza, Jessica M.

doi:10.1039/C9CP04038B

Title: Structure and electronic properties of rare earth DOBDC metal–organic-frameworks

Journal Article · Fri Oct 11 00:00:00 EDT 2019 · Physical Chemistry Chemical Physics. PCCP

DOI:https://doi.org/10.1039/C9CP04038B· OSTI ID:1574447

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Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)

In our report, we apply density functional theory (DFT) to investigate rare-earth metal organic frameworks (RE-MOFs), RE₁₂(μ₃-OH)₁₆(C₈O₆H₄)₈(C₈O₆H₅)₄ (RE = Y, Eu, Tb, Yb), and characterize the level of theory needed to accurately predict structural and electronic properties in MOF materials with 4f-electrons. A two-step calculation approach of geometry optimization with spin-restricted DFT and large core potential (LCPs), and detailed electronic structures with spin-unrestricted DFT with a full valence potential + Hubbard U correction is investigated. Spin-restricted DFT with LCPs resulted in good agreement between experimental lattice parameters and optimized geometries, while a full valence potential is necessary for accurate representation of the electronic structure. The electronic structure of Eu-DOBDC MOF suggested a strong dependence on the treatment of highly localized 4f-electrons and spin polarization, as well as variation within a range of Hubbard corrections (U = 1–9 eV). For Hubbard corrected spin-unrestricted calculations, a U value of 1–4 eV maintains the non-metallic character of the band gap with slight deviations in f-orbital energetics. When compared with experimentally reported results, the importance of the full valence calculation and the Hubbard correction in correctly predicting the electronic structure is highlighted.

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Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Center for Understanding and Control of Acid Gas-induced Evolution of Materials for Energy (UNCAGE-ME); Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: AC04-94AL85000; SC0012577; NA0003525; UNCAGE-ME Energy Frontier Research Center (EFRC) A; #DE-SC0012577

OSTI ID:: 1574447

Alternate ID(s):: OSTI ID: 1570052

Report Number(s):: SAND-2019-12496J; PPCPFQ; 680399; TRN: US2100017

Journal Information:: Physical Chemistry Chemical Physics. PCCP, Vol. 21, Issue 41; ISSN 1463-9076

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 20 works

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