Leveraging an all-fixed transfer framework to predict the interpretable formation energy of MXenes with hybrid terminals.

Abstract

MXenes have attracted substantial attention for their various applications in energy storage, sensors, and catalysts. Experimental exploration of MXenes with hybrid terminal surfaces offers a unique means of property tailoring that is crucial for expanding the performance space of MXenes, wherein the formation energy of an MXene with mixed surface terminals plays a key role in determining its relative stability and practical applications. However, the challenge of identifying energetically stable MXenes with multifunctional surfaces persists, primarily due to the absence of precise surface modification during experiments and the vast structural space for DFT calculations. Herein, we use an all-fixed transfer (AFT) framework combined with first-principles calculations to predict the formation energies of MXenes terminated by binary elements from groups VIA and VIIA. The trained model exhibits a high average R2 of 0.99, maintaining transferability and accuracy in predicting larger supercells from smaller-sized MXenes and datasets despite the structural imbalance between the training and prediction sets. The underlying interpretation of the high accuracy is revealed through the capture of main attributes and comparison of node features. Additionally, it is important to mention that the factors influencing the average formation energy include the types of element pairs, the ratio of terminal groups, and the distribution of terminations on two surfaces, with the first one being dominant. Finally, we successfully streamline the diverse structural cardinality of a large hybrid terminated MXene space of over 700 million, thereby facilitating the rapid screening of the top 5 stable MXene classes with binary terminal elements (FO, FCl, FBr, FS, and FSe). Besides, in the scenarios of lithium storage, the TL-predicted MXene can enhance its relative stability by increasing the fluorine ratio where the capacity can be optimized by different surface group combinations. All results indicate that the AFT framework has the advantages of screening functional MXenes with a huge structure space from smaller and imbalanced data sets.