MatCreatioNN: Machine learning-guided computational discovery of photocatalysts for environmental applications

Abstract

The rational design of photocatalysts for environmental remediation and CO2 conversion remains limited by the high computational cost and sparse experimental data describing multi-parameter photocatalytic behavior. This work presents an integrated machine-learning framework that couples reinforcement learning-based metal-organic framework (MOF) generation with a multi-stage Crystal Graph Convolutional Neural Network (CGCNN) prediction funnel to identify photocatalysts optimized across multiple electronic and structural features. 120,000 MOF candidates were generated and screened using 13 key descriptors, including band-gap suitability, CO2/H2O selectivity, adsorption energy, and structural stability. The funnel approach reduced computational cost by 4.13-fold while maintaining predictive robustness. Two top candidates, a Cr-based and a Zn-based MOF, exhibited predicted photocatalytic fitness values of 1.70 +/- 0.25 and 1.20 +/- 0.05 fold higher respectively than benchmark materials such as PCN-224(Zr), demonstrating simultaneous improvements in light absorption, redox energetics, and framework durability. Simulated X-ray diffraction patterns confirmed strong structural agreement with experimentally synthesized MOFs, indicating high synthesizability. Post-hoc analysis revealed recurring structural motifs, such as the N262 metal cluster, that correlated strongly with high predicted photocatalytic activity. These results highlight the potential of data-driven methods to accelerate discovery of efficient and durable photocatalysts for environmental and energy-related transformations, providing a foundation for experimental realization and large-scale implementation of computationally designed MOFs.