Electrical double layer and capacitance of TiO2 electrolyte interfaces from first principles simulations
arxiv(2024)
摘要
The electrical double layer (EDL) at aqueous solution-metal oxide interfaces
critically affects many fundamental processes in electrochemistry, geology and
biology, yet understanding its microscopic structure is challenging for both
theory and experiments. Here we employ ab initio-based machine learning
potentials including long-range electrostatics in large-scale atomistic
simulations of the EDL at the TiO2-electrolyte interface. Our simulations
provide a molecular-scale picture of the EDL that demonstrates the limitations
of standard mean-field models. We further develop a method to accurately
calculate the electrostatic potential drop at the interface. The computed
capacitance originating from the adsorbed charges and the potential drop agrees
with experiments, supporting the reliability of our description of the EDL. The
larger interfacial capacitance of basic relative to acidic solutions originates
from the higher affinity of the cations for the oxide surface and gives rise to
distinct charging mechanisms on negative and positive surfaces.
更多查看译文
AI 理解论文
溯源树
样例
![](https://originalfileserver.aminer.cn/sys/aminer/pubs/mrt_preview.jpeg)
生成溯源树,研究论文发展脉络
Chat Paper
正在生成论文摘要