在Pt上通过Nano-Confinement的界面水调节进化反应活动和机制
Yang Tao1, Keegan A Lorenz-Ochoa1, Lei Pan1
1Department of Chemistry, The University of Texas at Austin, Austin, Texas 78712, United States.
Journal of the American Chemical Society
|August 9, 2025
概括
在电催化剂中添加二甲基硫化物 (DMSO) 会改变水的结构,影响演变反应 (HER) 动力学. DMSO的界面水封闭阻碍了质子传递,减缓了HER,特别是在水覆盖率低的情况下.
科学领域:
- 电催化
- 物理化学
- 表面科学
背景情况:
- 水结构对于水性电催化是至关重要的.
- 介面水在电极运动中的作用尚不清楚.
- 甲基硫化物 (DMSO) 可以改变水网.
研究的目的:
- 研究DMSO如何影响 (Pt) 上的演变反应 (HER) 动力学.
- 阐明散装和界面水网修改对HER的影响.
- 了解界面水封闭对电催化活动的影响.
主要方法:
- 超微电极测量以隔离内在的HER动力学.
- 在酸性介质中的DMSO度的系统变化.
- 分子动力学 (MD) 模拟探测水结构和键.
主要成果:
- 通过阻断活性部位来抑制DMSO吸附.
- 在水资源丰富的地区,HER活动保持稳定,直到水覆盖率降至30%以下.
- 在水覆盖率低于30%的情况下,HER动力学急剧下降,吸附率变得有限.
- MD模拟显示DMSO限制了水界,并破坏了结,阻碍了质子传递.
结论:
- 像DMSO这样的吸附物种对水的界面限制显著调节了电催化动力学.
- 水网络的破坏和阻碍质子传递是活动变化的关键机制.
- 接口水结构提供了一种超越传统表面改造的电催化调节策略.
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