Silicon-based materials, particularly at the microscale, are prone to rapid capacity fade due to substantial volume fluctuations during the charge-discharge cycles, significantly impeding their commercial viability. Constructing a stable solid electrolyte interface (SEI) is an effective means to improve the performances of silicon-based anodes. Here small biomolecules, tryptophan (Trp) and phytic acid (PA), are introduced as interface modifiers to optimize the interfacial chemistry of micron-silicon anodes. By engaging in the SEI formation process, these small biomolecules effectively regulate the chemical composition and mechanical properties of the formed SEI, fostering a more cohesive and durable interface. The simultaneous addition of PA and Trp has been observed to yield a synergistic effect, creating a tightly bonded and resilient SEI that confers markedly improved battery performances upon the co-modified micron silicon anodes. Density functional theory calculations reveal charge interactions between these small biomolecules and silicon particles, facilitating effective adsorption onto the silicon surface. Simultaneous adsorption of Trp and PA on silicon surface can significantly enhance adsorption strength, providing a compelling explanation for the observed synergistic effect of Trp and PA co-modification.
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