Assessing exchange-correlation functionals for heterogeneous catalysis of nitrogen species
arxiv(2024)
摘要
Increasing interest in sustainable synthesis of ammonia, nitrates, and urea
has led to an increase in studies of catalytic conversion between
nitrogen-containing compounds using heterogeneous catalysts. Density functional
theory (DFT) is commonly employed to obtain molecular-scale insight into these
reactions, but there have been relatively few assessments of the
exchange-correlation functionals that are best suited for heterogeneous
catalysis of nitrogen compounds. Here, we assess a range of functionals ranging
from the generalized gradient approximation (GGA) to the random phase
approximation (RPA) for the formation energies of gas-phase nitrogen species,
the lattice constants of representative solids from several common classes of
catalysts (metals, oxides, and metal-organic frameworks (MOFs)), and the
adsorption energies of a range of nitrogen-containing intermediates on these
materials. The results reveal that the choice of exchange-correlation
functional and van der Waals correction can have a surprisingly large effect
and that increasing the level of theory does not always improve the accuracy
for nitrogen-containing compounds. This suggests that the selection of
functionals should be carefully evaluated on the basis of the specific reaction
and material being studied.
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