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Unraveling Entropic Rate Acceleration Induced by Solvent Dynamics in Membrane Enzymes

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Accelerating the discovery of multicatalytic cooperativity.

Marcus H Sak¹, Richard Y Liu², Eugene E Kwan³

¹Department of Chemistry and Chemical Biology, Harvard University, Cambridge, MA, USA.

|November 3, 2025

Summary

A new algorithm identifies cooperative catalysts by pooling and deconvoluting candidates, reducing experimental costs. This method discovered synergistic ligand pairs for palladium-catalyzed cross-coupling reactions, enabling lower catalyst loading and temperatures.

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Area of Science:

Catalysis
Organic Chemistry
Computational Chemistry

Background:

Cooperative catalysis, where multiple catalysts work together, is vital for many organic reactions.
Discovering new cooperative catalysts is challenging due to combinatorial complexity and reliance on serendipity or prior knowledge.

Purpose of the Study:

To develop a systematic and cost-effective algorithm for discovering novel cooperative catalytic behaviors.
To identify synergistic catalyst combinations for challenging organic transformations.

Main Methods:

A pooling-deconvolution algorithm inspired by group testing was developed to identify cooperative catalyst behaviors.
The algorithm was validated using simulated data and experimentally on organocatalytic enantioselective oxetane-opening reactions.
The approach was applied to discover catalysts for palladium-catalyzed decarbonylative cross-coupling.

Main Results:

The algorithm efficiently identifies cooperative catalyst behaviors with reduced experimental effort.
Previously unknown cooperativity was validated in organocatalysis.
Several ligand pairs were identified for palladium-catalyzed decarbonylative cross-coupling, significantly improving efficiency.

Conclusions:

The pooling-deconvolution algorithm offers a powerful, systematic approach to catalyst discovery.
This method enables the identification of cooperative catalysts that operate at lower loadings and temperatures.
The findings open new avenues for designing efficient catalytic systems.