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在金属表面上对水吸附的基准测试与ab initio分子动力学

Mianle Xu¹, Sihang Liu¹, Sudarshan Vijay¹

¹Catalysis Theory Center, Department of Physics, Technical University of Denmark, Kongens Lyngby, Denmark.

The Journal of chemical physics

|June 26, 2024

概括

密度函数理论 (DFT) 对金属表面水的模拟需要仔细选择参数. 与PBE-D3相比,RPBE-D3和BEEF-vdW函数提供了更准确的水吸附能量,这对于理解固体水接口至关重要.

科学领域:

计算材料科学科学计算材料科学
表面科学是一门学科.
物理化学物理化学

背景情况:

固态水接口在自然现象和技术应用中至关重要,特别是在绿色转型技术中,如电催化剂.
密度函数理论 (DFT) 是电解质-电极接口的原子模拟的标准,需要对固体/水相互作用进行验证.
准确的模拟设置对于防止理解接口过程中的系统错误至关重要.

研究的目的:

开发和应用一个严格的协议,用于对DFT对金属表面水吸附/脱附能量的模拟进行基准测试.
评估水与金属相互作用的常见交换相关函数 (PBE-D3,RPBE-D3,BEEF-vdW) 的性能.
通过评估系统错误,为未来的 DFT 模拟索尔瓦特固体接口提供指导.

主要方法:

与实验数据对比的DFT计算:温度编程脱落,单晶吸附热量计和热能原子散射.
在各种过渡金属表面上选DFT质量,使用PBE-D3,RPBE-D3和BEEF-vdW交换相关函数.
分析水吸附强度和与水-金属和水-水相互作用相关的变化.

主要成果:

所有测试的函数 (PBE-D3,RPBE-D3,BEEF-vdW) 都捕获了水的伪零级脱吸.
与实验数据相比,RPBE-D3和BEEF-vdW函数能产生更准确的水吸附强度.
PBE-D3功能系统地覆盖了近地表水,导致模拟中的潜在不准确性.

结论:

交换相关函数的选择对模拟固体水界面的水吸附能量的准确性产生重大影响.
建议使用RPBE-D3和BEEF-vdW来进行更可靠的水金属相互作用的DFT模拟.
这项研究提供了对水吸附平衡的原子洞察力,并为DFT模拟中的错误评估提供了一个框架.

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