在电解质与基于Pt的核心外纳米晶体中的进化反应动力学的理论和实验理解
Jeonghyeon Kim1, Haesol Kim2, Won-Jae Lee1
1Department of Chemistry and Green-Nano Materials Research Center , Kyungpook National University , Daegu 41566 , Korea.
Journal of the American Chemical Society
|October 18, 2019
概括
这项研究探讨了基介质中的进化反应 (HER) 的吸附自由能量 (ΔGH). 核心Pd@Pt和PdH@Pt催化剂显示了提高的HER活性,由工作功能和接口电场模型解释.
科学领域:
- 材料科学
- 电化学
- 催化剂
背景情况:
- 吸附自由能量 (ΔGH) 是演化反应 (HER) 动学的关键描述器.
- 它在性介质中的应用有限,需要进一步研究.
- 核心外纳米结构为催化应用提供可调节的特性.
研究的目的:
- 调查 ΔGH 作为基介质中的 HER 描述物的适用性.
- 合成和描述具有控制Pt外厚度的Pd@Pt和PdH@Pt核心外催化剂
- 阐明影响电解质中的HER活性的因素.
主要方法:
- 具有不同Pt外厚度 (1-5个原子层) 的Pd@Pt核心外八面体的合成.
- 在性电解质中对HER活性进行电化学评估.
- 使用复杂的表面应力核心板模型进行密度函数理论计算.
主要成果:
- 随着核心外的构造和Pt外厚度的增加,核心外催化剂的HER活性得到改善.
- 实验结果与计算的 ΔGH 值一致.
- 增强的HER活性更好地通过考虑界面电场的工作函数和明显的ΔGH模型来解释.
结论:
- 单独的热力学 ΔGH 缩放关系不足以解释性介质中增强的 HER 活性.
- 工作功能和界面电场效应在调整 HER 动力学方面发挥着至关重要的作用.
- Pd@Pt和Pd@Pt核心外纳米晶体显示出有效的HER催化潜力.
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