A similar observation can be made based on the correlation plots in Fig. , which highlight that both the KRR and 5p-LASSO methods have strong correlations with DFT predictions, as indicated by R-squared (R 2 ) values exceeding 0.9. Lippmaa's method shows the poorest correlation with DFT-calculated values, and the 2p-LASSO method, while generally reasonably accurate, fails to predict chemical shift of certain structures accurately. These outliers are associated with unique structural motifs for low water loadings, specifically those involving a hydrogen bond between the BAS proton and a framework oxygen, which stretches the Al-O bond. The 5p-LASSO method manages these outliers more effectively by accounting for the asymmetry of this bond length. The KRR model exhibits the best correlation overall, with an R 2 score of 0.97, indicating its robustness in predicting chemical shifts across diverse structural environments. In practice, despite its well-documented limitations, Lippmaa's approximation, correlating the chemical shifts only to T-O-T angles, continues to be used as a common method for assigning experimental NMR resonances to specific zeolite structures. However, based also on the tests presented in this section, the superior accuracy of the 2p-LASSO method suggests that Al-O bond lengths are more critical in predicting chemical shifts than previously believed, challenging the earlier conclusions by Liu et al., who provided a theoretical explanation based on bonding orbitals for the contribution of the T-O-T angles to be dominant. Importantly, the KRR model, which outperformed all other methods across the board, was particularly accurate in predicting shifts for hydrated structures. This is especially important because NMR measurements are typically performed on hydrated zeolites, where the water molecules can solvate the acidic proton. The presence of an unsolvated proton bound to the framework creates an asymmetric environment, which leads to the increase of the electric field and broadens the spectrum. Due to its superior performance, the KRR model is the main method of choice used in the remainder of this study. However, the 2p-LASSO and 5p-LASSO models are still valuable for the interpretation of the qualitative trends observed in the following sections.