Structure Sensitive Reaction Kinetics of Chiral Molecules on Intrinsically Chiral Surfaces

Area of Science:

• Heterogeneous catalysis
• Surface chemistry
• Chiral materials science

Background:

• Enantiospecific heterogeneous catalysis relies on chiral surfaces to separate enantiomers through structure-sensitive surface chemistry.
• Designing effective catalysts requires identifying chiral surface structures that enhance enantiospecificity.

Purpose of the Study:

• Develop data-driven models to predict the enantiospecificity of tartaric acid reactions on chiral copper (Cu) surfaces.
• Identify key structural features governing enantiospecificity in catalysis.

Main Methods:

• Utilized curved Cu(hkl) surfaces for kinetic measurements across diverse chiral orientations.
• Developed two data-driven models: one using generalized coordination numbers and another employing chiral cubic harmonic functions to describe surface structure.
• Correlated surface structure descriptors with measured enantiospecific rate constants.

Main Results:

• Both models achieved similar fitting errors, indicating comparable predictive power.
• The generalized coordination number model used 58 descriptors, while the cubic harmonic model used only 5.
• Both models predicted maximum enantiospecificity on closely related surface orientations.

Conclusions:

• Data-driven models, particularly those using symmetry-based descriptors like cubic harmonics, can effectively predict enantiospecificity.
• The findings are applicable to various enantiospecific reactions on chiral materials with cubic lattices.
• This work provides a pathway to understanding and optimizing structure-sensitive enantiospecific reaction kinetics.