Theoretical modeling for interfacial catalysis

Abstract

Heterogeneous catalysis is vital in modern chemical industry. The development of next‐generation heterogeneous catalysts demands methodological shift from trial‐and‐error to theory‐guided design. However, heterogeneous catalysis usually involves complex surfaces/interfaces, which make it difficult to establish a reasonable model. Herein, we reviewed the recent progress in our group, and demonstrated a new research paradigm to successfully bridge the material gap between theory and experiment. Accordingly, three important interfacial effects of heterogeneous catalysts have been discussed in detail, that is, the support effect of oxide‐on‐metal catalysts, the coordination effect of atomically dispersed metal catalysts (ADCs) and the ligand effect of molecular modification. We addressed that the close cooperation of theory and experiment is essential to gain deep mechanistic insights and help to optimize heterogeneous catalysts in a more rational way. This article is categorized under: Structure and Mechanism > Reaction Mechanisms and Catalysis

Investigating the mechanism of propylene epoxidation over halogen (X = F, Cl, Br, I) modified Cu2O(110) surfaces: a theoretical study

“…The desire for developing a good catalyst with both excellent reactivity and selectivity requires an intricate understanding of the underlying molecular mechanisms and the roles of various catalyst constituents. 11…”

“…The desire for developing a good catalyst with both excellent reactivity and selectivity requires an intricate understanding of the underlying molecular mechanisms and the roles of various catalyst constituents. 11 Cu-based catalysts, endowed with unique electronic structures and surface properties, have attracted attention due to their suitability in a multitude of oxidation reactions, including the direct epoxidation of propylene using molecular O 2 (DEP). [12][13][14][15][16] Yet, the complex network of reactions in DEP often precludes Cu or Cu 2 O catalysts from reaching optimal activity and selectivity by themselves.…”

Local Magnetic Effect-Induced Electron Configuration Regulation: Spin Flipping of Iron Centers for Molecular Catalysis

“…26 However, under actual operating conditions, the application of a magnetic field may disrupt an energy conversion devices system, leading to energy consumption and reducing the energy conversion efficiency of the energy conversion devices. 27 Therefore, utilizing the inherent magnetic field of a material to enhance the performance of oxygen reduction catalysts is an attractive strategy; however, there is currently no known research on this approach. The uneven charge density distribution at the atomic steps of edge defects in metal oxide crystals may lead to electron polarization and local spin magnetic moments.…”

“…The uneven charge density distribution at the atomic steps of edge defects in metal oxide crystals may lead to electron polarization and local spin magnetic moments . TiO 2 , a prototypical catalyst support, boasts a wealth of atomic step sites.…”

Modelling Heterogeneous Catalysis using Quantum Computers: An academic and industry perspective

“…[10][11][12][13][14][15][16][17][18] Moreover, computational methods, ranging from various electronic structure methods for transition state characterization, ab initio molecular dynamics and advanced sampling, machine learning algorithms, multiscale modelling, etc., have emerged as powerful tools for elucidating reaction pathways, catalyst design, and high-throughput screening of new materials. [19][20][21][22][23][24][25][26][27][28][29][30][31] Density functional theory (DFT) has emerged as the workhorse for modelling heterogeneous catalysis, providing a powerful and efficient framework for understanding catalytic processes at the atomic and molecular level. 19,21 DFT offers a practical approach to calculate electronic structure and predict reaction energetics, allowing researchers to explore the activity, selectivity, and stability of catalysts.…”