Effects of global orbital cutoff value and numerical basis set size on accuracies of theoretical atomization energies

Luo, Yanjiao; Yin, Shiwei; Lai, Weipeng; Wang, Yun

doi:10.1007/s00214-014-1580-8

Cited by 29 publications

(7 citation statements)

References 53 publications

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“…In the case of DN basis set, the global orbital cutoff (defined by the presence of a heavy Ln atom) is 4.3 Å; for DND, it increases to 5.0 Å; and for DNP, to 5.8 Å. The global orbital cutoff is applied to the generation of the numerical basis sets to limit the range of the numerical integrations and reduce the computational cost: this is a reasonable simplification, since the charge density decreases quickly as the distance from an atomic nucleus increases [54][55][56]. All the calculations were spin-polarized.…”

Section: Computational Methodologymentioning

confidence: 99%

Lanthanide bisphthalocyanine single-molecule magnets: A DFT survey of their geometries and electronic properties from lanthanum to lutetium

Martínez‐Flores

Bolivar-Pineda

Basiuk

2022

Materials Chemistry and Physics

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Section: Computational Methodologymentioning

confidence: 99%

Lanthanide bisphthalocyanine single-molecule magnets: A DFT survey of their geometries and electronic properties from lanthanum to lutetium

Martínez‐Flores

Bolivar-Pineda

Basiuk

2022

Materials Chemistry and Physics

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“…The exchange−correlation of the electron within the density functional theory (DFT) framework was considered by the generalized gradient approximation (GGA) in the form of the Perdew−Burke−Ernzerhof (PBE) functional 40 with double numerical plus d-functions (DNP) basis set. 41 The geometrical structures and adsorption energy of one Kr or Xe atom adsorbed on the cluster of top six MOFs were optimized and calculated with the abovementioned level. The empirical dispersion correction of DFT-D2 proposed by Grimme was chosen to describe the weak van der Waals interaction.…”

mentioning

confidence: 99%

Multiscale Computational Screening of Metal–Organic Frameworks for Kr/Xe Adsorption Separation: A Structure–Property Relationship-Based Screening Strategy

Lin

Xue-lian

Heng

et al. 2021

ACS Appl. Mater. Interfaces

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The separation of radioactive noble gases, such as Xe and Kr, has attracted special attention in the context of used nuclear fuel (UNF). In this study, 180 metal–organic frameworks (MOFs) formally used for selective adsorptions of ethane and ethylene, with a similar kinetic diameter to Kr and Xe, were initially screened for the Kr/Xe separation using the grand canonical Monte Carlo (GCMC) method. Then, the structure–adsorption property relationships were generalized, that is, the MOFs of higher Kr/Xe selectivity are with the porosity at 0.2–0.4 and the ratio of the largest cavity diameter/pore limiting diameter at 1.0–2.4. Based on the relationships, six reported MOFs with large Kr uptakes and Kr/Xe selectivities were experimentally screened out and validated by GCMC simulations within the CoRE-MOF database, which are higher than most reported MOFs under conditions pertinent to nuclear fuel reprocessing of an 80/20 v/v mixture of Kr/Xe at normal temperature and pressure. Further simulations reveal that higher Kr uptakes and Kr/Xe selectivities of six MOFs result from the confinement effect of the pores. Molecular dynamic simulations showed that the six MOFs are ideal membrane separation materials of Kr from Xe, which are driven by adsorption and diffusion. Analyses of electronic structure-based density functional theory calculations showed that the main interaction between Kr and the six MOFs is van der Waals force dominated by dispersion and induction interactions. Therefore, the generalized structure–adsorption property relationships may assist the screening of MOFs for the separation and production of Kr/Xe from UNF industrially.

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“…The structural optimization of related reactants, products, and intermediates, as well as transition state search, was performed by the DFT method implemented in the Dmol3 module of Materials Studio software, in which the revised Perdew–Burke–Ernzerhof generalized gradient approximation (RPBE-GGA) functional was employed . The effective core potentials (ECPs) proposed by Bergner were used to describe the inner electrons, while the polarizable DND basis set was employed in all of these calculations. The transition states were found using the LST/QST method, and the transition state structures were verified by frequency analysis.…”

Section: Model and Calculation Methodsmentioning

confidence: 99%

Mechanism of Photocatalytic Reduction of CO₂ to CH₃OH by Cu Nanoparticle and Metal Atom (Ag, Au, Pd, Zn)-Doped Cu Catalyst: A Theoretical Study

Zeng

Chen

et al. 2022

Organometallics

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In this study, density functional theory was used to optimize five catalyst models consisting of one Cu 38 nanoparticle and four Zn-, Pd-, Ag-, and Audoped Cu 37 -X nanoparticles. The energy gap value of the Cu 38 nanoparticle catalyst was calculated as 15.3 kcal mol −1 , and the energy gap values of Cu 37 -X (X: Au, Ag, Zn, Pd) were 15.0 kcal mol −1 , 15.2, 11.2, and 12.9 kcal mol −1 , respectively. All of these catalysts are photoactive in the visible-light range and can be used as good photocatalysts. The photocatalytic mechanism of CO 2 reduction on these optimized catalysts has been investigated in detail. Two possible reaction pathways for photocatalytic reduction of CO 2 to CO and four possible reaction pathways for the further reduction of CO to CH 3 OH were investigated. In the first stage of catalytic reduction, i.e., from CO 2 to CO, Au doping of the catalyst has the best photocatalytic effect on the process of catalytic CO 2 reduction to CO. The optimal reaction process catalyzed by these Cu-based nanoparticles is the direct transfer of the H atom of the H 2 O molecule to the O atom of the CO 2 molecule without surface bridging, which can determine the catalytic CO 2 reduction process, but the hydrogen evolution reaction cannot occur simultaneously. During the reduction of CO to CH 3 OH, we propose that the photocatalytic activity of these models still follows the order Cu 37 -Au > Cu 37 -Ag ≥ Cu 37 -Zn > Cu 37 -Pd > Cu 38 . Our research found that doping with Zn, Ag, and Au is beneficial to improve the activity of photocatalysts.

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Effects of global orbital cutoff value and numerical basis set size on accuracies of theoretical atomization energies

Cited by 29 publications

References 53 publications

Lanthanide bisphthalocyanine single-molecule magnets: A DFT survey of their geometries and electronic properties from lanthanum to lutetium

Lanthanide bisphthalocyanine single-molecule magnets: A DFT survey of their geometries and electronic properties from lanthanum to lutetium

Multiscale Computational Screening of Metal–Organic Frameworks for Kr/Xe Adsorption Separation: A Structure–Property Relationship-Based Screening Strategy

Mechanism of Photocatalytic Reduction of CO₂ to CH₃OH by Cu Nanoparticle and Metal Atom (Ag, Au, Pd, Zn)-Doped Cu Catalyst: A Theoretical Study

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Effects of global orbital cutoff value and numerical basis set size on accuracies of theoretical atomization energies

Cited by 29 publications

References 53 publications

Lanthanide bisphthalocyanine single-molecule magnets: A DFT survey of their geometries and electronic properties from lanthanum to lutetium

Lanthanide bisphthalocyanine single-molecule magnets: A DFT survey of their geometries and electronic properties from lanthanum to lutetium

Multiscale Computational Screening of Metal–Organic Frameworks for Kr/Xe Adsorption Separation: A Structure–Property Relationship-Based Screening Strategy

Mechanism of Photocatalytic Reduction of CO2 to CH3OH by Cu Nanoparticle and Metal Atom (Ag, Au, Pd, Zn)-Doped Cu Catalyst: A Theoretical Study

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Mechanism of Photocatalytic Reduction of CO₂ to CH₃OH by Cu Nanoparticle and Metal Atom (Ag, Au, Pd, Zn)-Doped Cu Catalyst: A Theoretical Study