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混合RPA:DFT在过渡金属表面上吸附的方法:甲和乙在 (111) 上

Christopher Sheldon^1,2, Joachim Paier^1,3, Denis Usvyat¹

¹Institut für Chemie, Humboldt-Universität zu Berlin, Unter den Linden 6, Berlin 10099, Germany.

Journal of chemical theory and computation

|February 8, 2024

概括

这项研究增强了量子力学:量子力学 (QM:QM) 对于过渡金属表面的方法. 混合方法准确地预测了 Pt{111} 上甲和乙的吸附能量,特别是在多体分散 (MBD) 时.

科学领域:

计算化学的计算化学
表面科学是一门学科.
材料科学材料科学材料科学

背景情况:

对过渡金属表面吸附的准确理论建模对于理解催化和材料特性至关重要.
对于复杂的表面相互作用,以前的方法在平衡精度和计算成本方面经常面临局限性.

研究的目的:

扩展混合量子力学:在过渡金属表面进行吸附研究的量子力学 (QM:QM) 方法.
调查随机相近似 (RPA) 的性能,作为一种嵌入密度函数理论 (DFT) 的高级方法,用于表面吸附.
评估不同DFT函数 (PBE和PBE+MBD) 与RPA相结合的准确性,以预测甲和乙在Pt上的吸附能量.

主要方法:

一种混合QM:QM方法,将集群模型的随机相近似 (RPA) 与使用减法方案的周期模型的密度函数理论 (DFT) 结合起来.
应用PBE功能,无论没有和多体分散 (MBD) 校正.
在Pt{111}表面上计算甲和乙的吸附能量.

主要成果:

混合RPA:PBE和RPA:PBE+MBD方法在显著降低的计算成本下实现了接近Pt{111}上甲吸附周期RPA计算的结果.
对于甲和乙,RPA:PBE方法与实验性脱吸障碍相比显示出低结合.
混合RPA:PBE+MBD方法与Pt{111}上的甲和乙的实验吸附能量表现出很好的一致性,并且在实验不确定性范围内.

结论:

混合QM:QM方法,特别是包括多体分散 (MBD),为研究过渡金属表面吸附提供了计算效率高和准确的方法.
选择DFT功能和表现表面集群对于基于RPA的QM:QM方案在金属表面的成功至关重要.
这种方法为表面化学和催化学的高精度理论预测提供了有希望的途径.

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