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Published on: November 9, 2019
Atomically Asymmetric Pd1─O─Cu Interfaces Break the Activity-Selectivity Limit in CO-to-Acetate Conversion
Zhi-Xin Li1, Jia-Run Huang1, Zhen-Hua Zhao1
1MOE Key Laboratory of Bioinorganic and Synthetic Chemistry, GBRCE For Functional Molecular Engineering, School of Chemistry, IGCME, Sun Yat-Sen University, Guangzhou, China.
This study introduces a novel catalyst for electrochemical reduction of carbon monoxide (CO) to acetate, achieving high efficiency and stability. The atomically asymmetric Pd-Cu interface overcomes traditional limitations, paving the way for carbon neutrality.
Area of Science:
- Electrochemistry
- Catalysis
- Materials Science
Background:
- Electrochemical reduction of CO (eCORR) to acetate is crucial for carbon neutrality.
- Linear scaling relations and activity-selectivity trade-offs limit conventional alloy catalysts.
- Stabilizing key intermediates like C─C coupling species is challenging.
Purpose of the Study:
- To circumvent thermodynamic limits in eCORR by designing a novel catalyst.
- To improve activity and selectivity for acetate production.
- To provide a generalizable strategy for multi-electron electrocatalysis.
Main Methods:
- Construction of atomically asymmetric Pd₁─O─Cu interfaces from CuPd-THQ.
- Utilizing isolated Pd single atoms anchored on Cu₂O nanoislands (Pd/Cu₂O/CuPd-THQ).
- Investigating CO spillover effect and intermediate binding energetics.
Main Results:
- Achieved 82.3% Faradaic efficiency for acetate with 96% purity.
- Demonstrated sustained performance (>400 h) at 250 mA cm⁻² and -1.0 V vs RHE.
- Reported an acetate yield rate of 6367.7 mg L⁻¹ h⁻¹ in a membrane electrode assembly (MEA) system.
Conclusions:
- The atomically asymmetric interface successfully breaks scaling relations.
- Isolated Pd atoms on Cu₂O nanoislands enable independent optimization of binding energetics.
- This approach offers a scalable and viable strategy for efficient eCORR to acetate.
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