缺陷捕获的Pt单位电催化剂的结构-属性关系,用于进化反应
Peng Tang1, Po-Yuan Huang1, Jack E N Swallow1
1Department of Materials, University of Oxford, Parks Road, Oxford OX1 3PH, United Kingdom.
概括
单位催化剂 (SSCs) 对进化反应 (HER) 是有前途的. 然而,被困单位催化剂 (Pt-SSCs) 由于不利的结合,其活性低于预期,这限制了它们的商业用途.
科学领域:
- 材料科学 材料科学 材料科学
- 电化学 电化学 电化学
- 催化剂是一种催化剂.
背景情况:
- 单位催化剂 (SSCs) 提供高金属原子利用率,单位被困在碳缺陷 (Pt-SSCs) 中,显示出进化反应 (HER) 的潜力.
- 了解Pt结合,其操作演变和Pt-SSC中的催化性能之间的关系至关重要,但仍然不清楚.
研究的目的:
- 在聚亚尼林基板上合成和表征一个被困的单位催化剂 (Pt-SSC).
- 研究Pt在合成过程中的结构演变及其对HER活性的影响.
- 为了阐明结构-属性关系,控制受困Pt-SSCs的性能.
主要方法:
- 在聚氨上通过H2PtCl6的热解合成Pt-SSC.
- 在现场加热扫描传输电子显微镜 (STEM) 和取决于温度的X射线光电子谱 (XPS) 用于结构分析.
- 操作X射线吸收光谱 (XAS) 来评估在HER条件下的稳定性.
- 第一个原则计算,以确定的化学吸收能量.
主要成果:
- 聚氨酸中的与Pt离子协调,使得在热解前的原子分散,并在石墨化后的pyridinic N缺陷中捕获.
- 被困的Pt-SSC在HER操作期间表现出稳定性.
- 与金属Pt纳米粒子相比,被困的Pt-SSC表现出较低的电催化活性.
- 第一个原则的计算表明,受困的Pt-SSCs对不良的化学吸收.
结论:
- 这项研究澄清了合成过程中被困的Pt-SSCs的结构演变和结合环境.
- 被困的Pt-SSCs的劣质HER活性归因于不利的化学吸收.
- 建议进行进一步的技术经济分析,以评估这些催化剂的商业可行性.
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