Necessity of Heteroatoms for Realizing Hypothetical Aluminophosphate Zeolites: A High-Throughput Computational Approach

Aluminophosphate
zeolites (AlPOs) have important applications in
adsorption, separation, and catalysis. Millions of hypothetical zeolite
structures have been predicted, but experimentally realizing them
as AlPOs requires a priori knowledge on whether heteroatom incorporations
are necessary to stabilize their frameworks. Previous computations
focus on the energy difference before and after heteroatom incorporation,
which are not applicable for high-throughput computations because
of the combinatorial explosion of possible incorporation sites. Here,
we establish a new model to estimate the probability of a hypothetical
structure being a pure or a heteroatom-stabilized AlPO, which is based
on the Mahalanobis distances between a hypothetical structure and
its neighboring reference structures in distortion–energy plots.
Our approach avoids numerous attempts at heteroatom incorporation
and is therefore applicable for high-throughput structure evaluation.
Using this model, we have predicted 17 050 hypothetical structures
being realizable as pure AlPOs and 12 039 structures realizable
only via heteroatom incorporation. This will provide important guidance
toward the synthesis of new AlPOs.