论文标题
热波动在电催化金属表面特性和共同结合趋势中的关键作用
The Critical Role of Thermal Fluctuations for Electrocatalytic Metal Surface Properties and CO Binding Trends
论文作者
论文摘要
这项工作解决了使用密度函数理论（DFT）的长期理论差异，并对CO2还原反应（CO2RR）的电催化金属的CO结合趋势进行了实验观察。 By introducing thermal fluctuations using appropriate statistical mechanical NVT and NPT ensembles, we show that DFT with universal dispersion interactions yields qualitatively better metal surface strain trends and CO binding energetics, consistently predicts the correct site preference for all metals due to thermally induced surface distortions that preferentially exposes the undercoordinated atop site for Cu(111) and Pt(111), and for the weak binding在有限温度下的AG（111）和AU（111）表面显示出是化学吸附和物理性物种的混合物。这项研究通过证明需要充分说明有限温度波动以与表面科学实验接触的有限温度波动，使理论更好地将理论视为实验性异质催化的平等伙伴。
This work addresses a longstanding theoretical discrepancy using Density Functional Theory (DFT) with experimental observations of CO binding trends on electrocatalytically relevant metals for the CO2 reduction reaction (CO2RR). By introducing thermal fluctuations using appropriate statistical mechanical NVT and NPT ensembles, we show that DFT with universal dispersion interactions yields qualitatively better metal surface strain trends and CO binding energetics, consistently predicts the correct site preference for all metals due to thermally induced surface distortions that preferentially exposes the undercoordinated atop site for Cu(111) and Pt(111), and for the weak binding Ag(111) and Au(111) surfaces at finite temperatures shows CO-metal interactions that are a mixture of chemisorbed and physisorbed species. This study better places theory as an equal partner to experimental heterogeneous catalysis by demonstrating the need to fully account for finite temperature fluctuations to make contact with surface science experiments.
