Chemical Reaction Networks from Scratch with Reaction Prediction and Kinetics-Guided Exploration

Journal of Chemical Theory and Computation, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 30, 2025

Algorithmic reaction explorations based on transition state searches can now routinely predict relatively short sequences involving small molecules. However, applying these algorithms to deeper chemical network (CRN) exploration still requires the development of more efficient and accurate policies. Here, an algorithm, which we name yet another kinetic strategy (YAKS), is demonstrated that uses microkinetic simulations nascent achieve cost-effective, deep exploration. Key features algorithm are automatic incorporation bimolecular reactions between intermediates, compatibility with short-lived but kinetically important species, rate uncertainty into policy. In validation case studies glucose pyrolysis, rediscovers pathways previously discovered by heuristic policies elucidates new for experimentally obtained products. The resulting CRN first connect all major experimental pyrolysis products glucose. Additional presented investigate role rules, uncertainty, reactions. These show naïve exponential growth estimates vastly overestimate actual number relevant in physical networks. light this, further improvements prediction make it feasible CRNs might soon be predictable some contexts.

Language: Английский

Chemical Networks from Scratch with Reaction Prediction and Kinetics-Guided Exploration

Published: June 17, 2024

Algorithmic reaction explorations based on transition state searches can now routinely predict relatively short sequences involving small molecules. However, applying these algorithms to deeper chemical network (CRN) exploration still requires the development of more efficient and accurate policies. Here, an al- gorithm, which we name Yet Another Kinetic Strategy (YAKS), is demonstrated that uses microkinetic simulations nascent achieve cost-effective deep exploration. Key features algorithm are automatic incorporation bimolecular reactions between intermediates, compatibility with short-lived but kinetically important species, rate uncertainty into policy. In validation case studies glucose pyrolysis, rediscovers pathways previously discovered by heuristic policies also elucidates new experimentally obtained products. The resulting CRN first connect all major experimental pyrolysis products glucose. Additional presented investigate role rules, uncertainty, reactions. These show naive exponential growth estimates vastly overestimate actual number relevant in physical networks. light this, further improvements prediction make it feasible CRNs might soon be predictable many contexts.

Language: Английский