Pd3Au 上 CO2 还原成 HCOOH 的理论研究：显式溶剂模型必不可少,Journal of Materials Chemistry A

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Pd3Au 上 CO2 还原成 HCOOH 的理论研究：显式溶剂模型必不可少
Journal of Materials Chemistry A ( IF 10.7 ) Pub Date : 2023-02-20 , DOI: 10.1039/d2ta08552f
Ming Zheng ₁ , Xin Zhou ₁ , Yixin Wang ₁ , Gang Chen ₁ , Mingxia Li ₂

Affiliation

由于原子排列和电子结构的差异，具有不同晶面的固体催化剂具有不同的催化性能。因此，在原子水平上研究催化剂在不同晶面上的反应机理，有助于更好地理解构效关系，提高催化剂的活性。_{在这项工作中，CO 2在Pd}₃的不同表面上还原为甲酸的机理利用密度泛函理论对金合金进行了研究，揭示了催化剂功函数和d带中心的差异与过电位之间的潜在关系。电子结构计算结果表明，催化剂的表面粗糙度和电子结构共同决定了CO ₂还原为甲酸的催化活性。同时发现催化剂的表面净电荷与HER活性之间存在良好的线性关系。钯₃Au(110)表面净电荷较少，可以有效抑制HER。水溶液的动态氢键网络是决定反应机理的关键，反映了水分子在催化反应中不可或缺的作用，表明了在反应机理计算中使用显式溶剂模型模拟溶剂化作用的重要性.

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Theoretical study on the reduction mechanism of CO2 to HCOOH on Pd3Au: an explicit solvent model is essential

Due to the differences in atomic arrangement and electronic structures, solid catalysts with different crystal planes have different catalytic properties. Therefore, studying the reaction mechanism on different crystal planes of catalysts at the atomic level is helpful to better understand the structure–activity relationship and improve the activity of catalysts. In this work, the mechanism of reduction of CO₂ to formic acid on different surfaces of the Pd₃Au alloy is investigated by using density functional theory, and the potential relationship between the difference in the work function and d-band center of the catalyst and the overpotential is revealed. The electronic structure calculation results show that the surface roughness and the electronic structure of the catalyst together determine the catalytic activity of CO₂ reduction to formic acid. At the same time, a good linear relationship was found between the surface net charge of the catalyst and the HER activity. The Pd₃Au (110) surface with less net surface charge can effectively suppress the HER. The dynamic hydrogen bonding network of water solution is the key to determine the reaction mechanism, which reflects the indispensable role of water molecules in the catalytic reaction and indicates the importance of using an explicit solvent model to simulate solvation effects in the calculation of the reaction mechanism.

更新日期：2023-02-20

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