在甲酸盐酸溶液中乙醇电氧化时,的氧化特征和电催化活性之间的关系
Xinyu You1, Jiaxing Han1, Vinicius Del Colle2
1College of Chemical Engineering, China University of Mining and Technology, 221116, Xuzhou, People's Republic of China.
Communications chemistry
|May 29, 2023
概括
氧化物,特别是PtOHads和α-PtO2,是乙醇电氧化的主要催化中心. 这一发现得到了DFT计算的支持,有助于更好地理解用于能量转换的电化学反应.
科学领域:
- 表面科学是一门学科.
- 电化学 电化学 电化学
- 催化剂是一种催化剂.
背景情况:
- 水及其分离物种在催化过程中的固体-液体接口中至关重要.
- 人们越来越认识到氧物种在催化过程中从水解离中发挥的特定作用.
- 了解在乙醇电氧化中的作用对于能源转化技术至关重要.
研究的目的:
- 阐明白金氧化物身份及其在乙醇氧化中的电催化活性之间的关系.
- 为了确定作为催化中心的特定氧化物种.
- 开发一种以白金氧化物为媒介的乙醇电氧化综合反应机制.
主要方法:
- 电化学实验在高酸盐溶液中进行了广泛的电位范围 (高达1.5V RHE) 的实验.
- 该研究使用了各种晶表面,包括Pt{111},Pt{110}和Pt{100}电极.
- 用密度函数理论 (DFT) 的计算来确定反应机制.
主要成果:
- PtOHads和α-PtO2被确定为乙醇电氧化的活性催化中心,而PtOads不是.
- 这种催化活性关系在不同晶体方面是一致的.
- DFT计算支持了一种涉及氧化物,脱和双二醇中间体的机制,解释了实验观察如pH依赖和α-PtO2相对于PtOHads的相对活性等.
结论:
- 氧化物,特别是PtOHads和α-PtO2,对于有效的乙醇电氧化是必不可少的.
- 拟议的DFT衍生机制准确地解释了实验发现,包括产品选择性和α-PtO2的优越活性.
- 这些发现对设计用于能量转换和电化学合成的金属/合金电极具有广泛的影响.
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