Ge Bingqing, Wei Fenfei, Wan Qiang, Zhang Hongwei, Yuan Pei, Lin Sen
State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou 350002, China.
National Engineering Research Center of Chemical Fertilizer Catalyst, College of Chemical Engineering, Fuzhou University, Fuzhou 350002, China.
Precis Chem. 2023 Apr 13;1(7):429-436. doi: 10.1021/prechem.3c00015. eCollection 2023 Sep 25.
Selective adsorption of α,β-unsaturated aldehydes (α,β-UALs) is a prerequisite for the hydrogenation of α,β-UALs to high-value unsaturated alcohols, but a quantitative description of the interactions between the CC/CO bond of α,β-UALs and the catalysts is still lacking. Herein, based on comprehensive density functional theory calculations, we developed a descriptor that combines the near-frontier molecular orbitals of the CC/CO bonds of α,β-UALs with the fundamental physical properties of single-atom catalysts (SACs) and considers the inner/outer coordination environment. All of the parameters used in this descriptor are easily accessible and interpretable, enabling an efficient assessment of the selectivity of SACs for the CC/CO bonds of α,β-UALs.
选择性吸附α,β-不饱和醛（α,β-UALs）是将α,β-UALs氢化为高价值不饱和醇的前提条件，但目前仍缺乏对α,β-UALs的CC/CO键与催化剂之间相互作用的定量描述。在此，基于全面的密度泛函理论计算，我们开发了一种描述符，该描述符将α,β-UALs的CC/CO键的近前沿分子轨道与单原子催化剂（SACs）的基本物理性质相结合，并考虑了内/外配位环境。该描述符中使用的所有参数都易于获取和解释，能够有效地评估SACs对α,β-UALs的CC/CO键的选择性。
