Electrostatically Embedded Many-Body Expansion for Neutral and Charged Metalloenzyme Model Systems

Area of Science:

• Computational Chemistry
• Quantum Chemistry
• Inorganic Chemistry

Background:

• The electrostatically embedded many-body (EE-MB) method is established for cluster energy calculations.
• EE-MB has been extended to metal-ligand bonds in positively charged inorganic complexes.
• Accurate calculation of bond dissociation energies is crucial for understanding chemical reactivity and designing new materials.

Purpose of the Study:

• To present guidelines for optimizing EE-MB calculations on metal centers.
• To validate the EE-MB method for bond dissociation energies in neutral and negatively charged inorganic systems.
• To assess the performance of EE-MB for metalloenzyme active site models.

Main Methods:

• Development and application of four key guidelines for EE-MB calculations.
• Utilizing the electrostatically embedded three-body (EE-3B) variant of the method.
• Testing on a range of pentacoordinate and hexacoordinate zinc-containing systems.

Main Results:

• The EE-MB method, following the proposed guidelines, performs well for diverse inorganic coordination systems.
• The EE-3B method accurately reproduces bond dissociation energies.
• An average absolute error of 0.98 kcal/mol was achieved across 25 test cases.

Conclusions:

• The EE-MB method is a reliable and efficient approach for calculating bond dissociation energies in various inorganic coordination complexes.
• The developed guidelines enhance the accuracy and efficiency of EE-MB for metal-centered systems.
• This method shows promise for studying metalloenzyme active sites and related drug targets.