Synergistic Rh1-Cu1 Dual-Atom-Site Enhancing Performance of Ethane Low-Temperature Oxidation via Auto-Selective
Bin Li1, Siquan Feng1, Jiaqian Wang2
1Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, China.
Angewandte Chemie (International Ed. in English)
|February 4, 2026
Summary
This study introduces a novel dual-atom catalyst for efficient ethane conversion into valuable chemicals. The Rh-Cu catalyst demonstrates enhanced selectivity and productivity, offering a promising route for shale gas utilization.
Area of Science:
- Catalysis
- Materials Science
- Chemical Engineering
Background:
- Direct conversion of ethane is crucial for shale gas utilization.
- Dual-atom catalysts offer unique cooperative effects for enhanced reactivity.
- Selective oxidation of ethane to oxygenates is a challenging but important process.
Purpose of the Study:
- To develop a porous organic polymer-supported Rh-Cu dual-site catalyst for selective ethane oxidation.
- To investigate the auto-selective oxygen source mechanism in the catalytic process.
- To improve the productivity and selectivity of ethane conversion compared to single-atom catalysts.
Main Methods:
- Synthesis of a porous organic polymer-supported Rh1-Cu1 dual-site catalyst (Rh1-Cu1@POPs-PPh3).
- Characterization using isotopic labeling and in situ techniques.
- Density functional theory (DFT) calculations to elucidate the reaction mechanism and active site properties.
Main Results:
- The optimized Rh1-Cu1 catalyst achieved a productivity of ca. 250 mol molRh-1 h-1 with 65% acetaldehyde selectivity at 423 K.
- A four-fold improvement in performance was observed compared to a single-Rh-site catalyst.
- An auto-selective oxygen source mechanism was uncovered, involving distinct oxygen species for ethanol and acetaldehyde formation.
Conclusions:
- The Rh1-Cu1@POPs-PPh3 catalyst enables efficient and selective low-temperature direct conversion of ethane.
- The study reveals a novel auto-selective oxygen source mechanism governing the reaction pathways.
- DFT calculations confirm that the Rh-Cl-Cu configuration enhances ethane activation and facilitates the catalytic cycle.
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