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.