Lanthanide-Bridged Dual-Atom Catalysts for Efficient Chlorine Electrosynthesis
Wen-Da Zhang1,2, Lulu Chen3, Yongbiao Mu4
1Key Laboratory of Synthetic and Biological Colloids, School of Chemical and Material Engineering, Ministry of Education, Jiangnan University, Wuxi, P. R. China.
Researchers developed a novel "mortise-and-tenon" strategy using a tulip-shaped covalent organic framework (Tu-COF) to create heteronuclear dual-atom catalysts (DACs). The Ru-Ce catalyst shows exceptional performance in the chlorine evolution reaction (CER), offering high efficiency and stability.
Area of Science:
- Materials Science and Engineering
- Electrochemistry
- Catalysis
Background:
- The chlorine evolution reaction (CER) is crucial for industrial chlor-alkali processes and water treatment.
- Current CER methods face challenges with high energy consumption and limited selectivity.
- Developing efficient and selective electrocatalysts is essential for advancing CER technologies.
Purpose of the Study:
- To design and synthesize novel heteronuclear dual-atom catalysts (DACs) for improved CER performance.
- To investigate the structure-activity relationship of these DACs using experimental and computational methods.
- To demonstrate a generalizable strategy for constructing advanced electrocatalysts.
Main Methods:
- Synthesis of a tulip-shaped covalent organic framework (Tu-COF) precursor.
- Construction of heteronuclear Ru-Ln dual-atom catalysts (DACs) via a "mortise-and-tenon" strategy.
- Electrocatalytic performance evaluation in a flow cell, including chronoamperometry and Faradaic efficiency measurements.
- Mechanistic studies using in situ characterization and Density Functional Theory (DFT) calculations.
Main Results:
- The Ru-Ce catalyst, synthesized using the Tu-COF precursor, exhibited superior CER performance.
- Achieved high current density (150 mA cm⁻²) at a low overpotential (1.45 V vs. RHE) with near 100% Faradaic efficiency for Cl₂ evolution.
- Demonstrated excellent long-term stability (>500 h) in a flow cell.
- DFT calculations revealed that the Ce atom modulates the electronic structure of the Ru center, optimizing Cl adsorption and facilitating Cl-Cl coupling while suppressing competing reactions.
Conclusions:
- The "mortise-and-tenon" strategy using Tu-COF is effective for precise construction of heteronuclear DACs.
- The Ru-Ce catalyst shows significant potential for efficient and selective chlorine evolution.
- Lanthanide-mediated electronic engineering is a promising approach for designing high-performance electrocatalysts.
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