在SnO2(110)/H2O界面上以水为媒介的质子跳跃机制从Ab Initio深潜在分子动力学界面开始
Mei Jia1,2, Yong-Bin Zhuang2, Feng Wang2
1Henan Key Laboratory of Biomolecular Recognition and Sensing, Henan Joint International Research Laboratory of Chemo/Biosensing and Early Diagnosis of Major Diseases, College of Chemistry and Chemical Engineering, Shangqiu Normal University, Shangqiu 476000, China.
调查金属氧化物表面的质子转移 (PT) 显示,以水为媒介的路径在鲁氧化物上表现出最低的能量障碍. 这一发现对于理解水分和储存过程至关重要.
科学领域:
- 表面化学 表面化学
- 计算材料科学科学 计算材料科学
- 电化学 电化学 电化学
背景情况:
- 介面质子转移 (PT) 对于光电催化水分裂,脱和储存等过程至关重要.
- 了解PT在金属氧化物表面上的热力学和动力学至关重要,但具体路径的详细自由能量障碍和溶剂效应仍然难以捉摸.
研究的目的:
- 为了研究面交界质子转移 (PT) 机制在鲁SnO2{\displaystyle S_{O}{2}{1}{10}}/H2O界面上.
- 阐明溶剂效应的作用,并确定具有最低能量障碍的 PT 途径.
- 探索深度神经网络在氧化物/液体界面的 PT 建模中的适用性.
主要方法:
- 结合了初始计算和深潜分子动力学.
- 模拟的PT路径在鲁SnO2(110) / H2O接口上.
- 在一系列氧化物 (SnO2,TiO2,IrO2) 中分析了PT机制.
主要成果:
- 确定了三个PT路径:表面PT,介导PT和附加层PT.
- 涉及溶剂水的中介PT表现出最低的能量屏障和最快的速度,这是由于最佳的H结合.
- 完全溶解显著影响水媒介PT,但对直接PT的影响很小.
结论:
- 溶解环境对氧化物界面的水介导质子传导具有关键的影响.
- 深度神经网络可以准确地复制PT研究的初始潜在能量表面.
- 这项研究提供了有关电化学,光电催化和地球化学的PT机制的关键见解.
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