Mechanism-Guided, Data-Driven Discovery of a Dinuclear Gold Catalyst for Promoting Oxidative Addition
Yulong Fu1, Kelin Zhu2, Zhensheng Jia1
1State Key Laboratory of Coordination Chemistry, Jiangsu Key Laboratory of Advanced Organic Materials, Chemistry and Biomedicine Innovation Center (ChemBIC), School of Chemistry and Chemical Engineering, Nanjing University, Nanjing, China.
Angewandte Chemie (International Ed. in English)
|July 6, 2026
Summary
Researchers designed new dinuclear gold catalysts using machine learning to improve gold catalysis for aryl halide reactions. This strategy accelerates the design of efficient catalysts by exploring numerous ligand possibilities.
Area of Science:
- Organometallic Chemistry
- Catalysis
- Computational Chemistry
Background:
- Gold catalysis is limited by the accessibility of Au(I)/Au(III) redox pathways, hindering reactions like aryl halide oxidative addition (OA).
- Developing efficient gold catalysts requires understanding and overcoming these redox limitations.
Purpose of the Study:
- To design dinuclear gold complexes for facile oxidative addition of aryl halides.
- To develop a mechanism-guided, data-driven strategy for catalyst design using machine learning.
Main Methods:
- Mechanistic Density Functional Theory (DFT) calculations to identify favorable reaction pathways.
- High-throughput virtual screening and multiobjective Bayesian optimization to screen 42,398 bidentate ligands.
- Machine learning and energy decomposition analyses to understand ligand effects.
Main Results:
- Identified pyridine-phosphine (di-PN) ligands as privileged scaffolds that significantly lower the OA activation barrier.
- Revealed a favorable cationic Au(III)-Au(I) OA pathway within a bimetallic framework.
- Demonstrated enhanced reactivity due to geometric pre-distortion, electronic polarization, and Au-Au interactions.
Conclusions:
- The developed strategy successfully designs dinuclear gold catalysts with enhanced reactivity for aryl halide OA.
- Synthesized and validated a predicted dinuclear gold catalyst in a sulfonylation reaction.
- Established a broadly applicable workflow for designing multinuclear transition-metal catalysts.
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