原子与过渡金属表面的相互作用:一个高通量计算研究
Miquel Allés1, Ling Meng1, Ismael Beltrán1
1Departament de Ciència de Materials i Química Física and Institut de Química Teòrica i Computacional (IQTCUB), Universitat de Barcelona, c/Martí i Franquès 1-11, Barcelona 08028, Spain.
The journal of physical chemistry. C, Nanomaterials and interfaces
|December 5, 2024
概括
这项研究揭示了过渡金属表面有利于解离或H2吸附. 计算模型显示相互作用的趋势,有助于关键工业反应的催化剂设计.
科学领域:
- 表面科学是一门学科.
- 计算化学计算化学
- 材料科学 材料科学 材料科学
- 催化剂是一种催化剂.
背景情况:
- 原子在过渡金属 (TM) 催化反应中至关重要,如哈伯-博什过程.
- 了解原子水平上的金属相互作用对于催化剂改进至关重要.
- 基于现实模型的第一原则计算是实现这种原子知识的关键.
研究的目的:
- 为了评估与各种过渡金属的低覆盖,稳定的表面的相互作用.
- 研究不同TM表面结构上的吸附和解离行为.
- 识别用于预测相互作用强度和趋势的描述符.
主要方法:
- 使用密度函数理论 (DFT) 的计算.
- 研究了27种BCC,FCC和HCP过渡金属的81个稳定表面的低覆盖相互作用.
- 分析了吸附能量,高度,并将它们与电子描述符相关联,如d频段中心.
主要成果:
- TM表面被分为两组:那些有利于H2解离和那些有利于没有解离的H2吸附 (通常是d10配置的晚期TM).
- 在离散表面上,在约0.5或1.0 Å的高度发现了原子.
- d频段中心与H吸附能量的强有力的线性相关性,特别是对于FCC和HCP表面 (MAE为0.15 eV).
- 基于吉布斯自由吸附能量的理论火山图表表明FCCTM是最佳的,尽管Pt的峰值性能被分散力所转移.
- 计算火山图与实验催化活性数据有质的相关性,但不具有数量.
结论:
- 该研究提供了对金属相互作用的全面原子学理解,涉及广泛的过渡金属.
- 确定了相互作用的关键趋势和描述符 (d带中心),对于催化剂的计算选有用.
- 虽然通过计算获得的火山图提供了定性见解,但对催化性能的定量预测需要进一步改进.
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