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Creating High Regioselectivity by Electronic Metal-Support Interaction of a Single-Atomic-Site Catalyst
Wen-Hao Li1, Jiarui Yang1, Hongyu Jing1
1Department of Chemistry, Tsinghua University, Beijing, 100084, China.
Researchers developed a novel single-atomic-site catalyst (Cu1-TiC) that precisely controls organic reaction regioselectivity. This catalyst enhances electronic metal-support interactions (EMSI) for highly linear-E-type alkyne conversion, avoiding branched isomers.
Area of Science:
- Catalysis
- Organic Chemistry
- Materials Science
Background:
- Ligands are traditionally used to control regioselectivity in organic synthesis.
- Developing novel regioselective control methods is crucial for advancing organic synthesis.
Purpose of the Study:
- To design and synthesize a single-atomic-site catalyst (SAC) for enhanced regioselective control.
- To investigate the role of electronic metal-support interaction (EMSI) in regulating reaction selectivity.
Main Methods:
- Designed and synthesized a single-atomic-site catalyst, Cu1-TiC, leveraging EMSI effects.
- Studied reaction mechanisms to understand the catalyst's performance.
- Utilized transient electron-rich characteristics to enhance π cloud back-donation.
Main Results:
- Achieved highly linear-E-type regioselective conversion of electronically unbiased alkynes (linear:branched ratio >100:1).
- Completely avoided the formation of branched isomers.
- Demonstrated a turnover number (TON) up to 612, three times higher than previously recorded.
- Showcased the critical role of each element in the SAC's synthesis mechanism.
Conclusions:
- Single-atomic-site catalysts (SACs) with strong EMSI can effectively regulate regioselectivity in homogeneous catalysis.
- EMSI, previously known for enhancing catalytic efficiency and durability, shows significant potential for controlling reaction selectivity.
- The designed Cu1-TiC catalyst offers a new paradigm for regioselective organic synthesis.
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