Boron-assisted synthesis of compositionally complex amorphous oxides via short-range-order-constrained generative design

Engineering short-range atomic order in amorphous materials offers a promising yet scarcely explored route to high-performance materials. Here, we establish a boron-assisted amorphization strategy using ApolloX, a theory-guided, short-range-order–constrained generative framework that enables the synthesis of multielement materials with tunable boron content and yields FeCoNiMoBOx compositions with promising oxygen evolution reaction (OER) activity. In particular, ApolloX identifies an ensemble of candidate low-energy amorphous configurations for the FeCoNiMoBOx family across systematically varied boron contents. Ab initio molecular dynamics simulations based on these configurations reveal that increasing boron content slows atomic diffusion and suppresses crystallization, with the stabilization of BO3-centered motifs identified as a critical structural descriptor that governs the amorphization propensity. Guided by these predictions, we first synthesize three representative FeCoNiMoBOx compositions with distinct boron contents within the theoretically identified composition window and perform synchrotron-based scattering and electron microscopy to verify compositional fidelity, structural homogeneity, and the targeted structural features, thereby experimentally validating our boron-assisted synthesis strategy. Building on this validation, we further extend the approach to abroader library of multimetal BOx amorphous compositions with diverse metal combinations and boron loadings, confirming the generality and transferability of the proposed method. Overall, these results demonstrate that this boron-assisted amorphization strategy provides a practical means to rationally design compositionally complex amorphous materials with tunable and potentially improved performance.