Applying statistical modeling strategies to sparse datasets in synthetic chemistry

Science Advances, Journal Year: 2025, Volume and Issue: 11(1)

Published: Jan. 1, 2025

The application of statistical modeling in organic chemistry is emerging as a standard practice for probing structure-activity relationships and predictive tool many optimization objectives. This review aimed tutorial those entering the area chemistry. We provide case studies to highlight considerations approaches that can be used successfully analyze datasets low data regimes, common situation encountered given experimental demands Statistical hinges on (what being modeled), descriptors (how are represented), algorithms modeled). Herein, we focus how various reaction outputs (e.g., yield, rate, selectivity, solubility, stability, turnover number) structures binned, heavily skewed, distributed) influence choice algorithm constructing chemically insightful models.

Language: Английский

---

Ligand-Induced Activation of Single-Atom Palladium Heterogeneous Catalysts for Cross-Coupling Reactions

ACS Nano, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 2, 2025

Single-atom heterogeneous catalysts (SACs) are potential, recoverable alternatives to soluble organometallic complexes for cross-coupling reactions in fine-chemical synthesis. When developing SACs these applications, it is often expected that the need ligands, which essential catalysts, can be bypassed. Contrary that, ligands remain almost always required palladium atoms stabilized on commonly used functionalized carbon and nitride supports, as otherwise show limited activity. Despite this, ligand optimization has received little attention, their role activating poorly understood. Here, we explore impact of structurally diverse phosphine performance nitrogen-doped supported single-atoms (Pd1@NC) Sonogashira–Hagihara (SH) reaction, using X-ray absorption spectroscopy density functional theory simulations rationalize observed trends. Compared ligand-free SAC, SH activity enhanced all ligand-assisted systems, with reactivity varying by up 8 orders magnitude depending choice. Distinct trends emerge based free volume class. Unlike molecular electronic effects less significant due modulating influence support. Instead, SAC-ligand systems governed a balance between deformation energy during coordination metal centers, resulting accessibility reagents. These findings offer key insights into optimizing Pd-SACs leveraging activate centers tailor 3D environment.

Language: Английский

---

COBRA web application to benchmark linear regression models for catalyst optimization with few-entry datasets

Cell Reports Physical Science, Journal Year: 2024, Volume and Issue: unknown, P. 102348 - 102348

Published: Dec. 1, 2024

Language: Английский

---

NHC-Cracker: A Platform for the In Silico Engineering of N-Heterocyclic Carbenes for Diverse Chemical Applications

ACS Catalysis, Journal Year: 2025, Volume and Issue: unknown, P. 5915 - 5927

Published: March 27, 2025

Language: Английский

---