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Synthesis and Performance Characterizations of Transition Metal Single Atom Catalyst for Electrochemical CO2 Reduction
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Curvature-Engineered Steering of Oxygen Electroreduction Pathways on Single-Atom Catalysts
Hongyin Xia1, Hounan Sun2, Dongyue Yang1
1State Key Laboratory of Electroanalytical Chemistry, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun, China.
Angewandte Chemie (International Ed. in English)
|March 18, 2026
Summary
Researchers engineered single-atom catalysts (SACs) using curvature engineering to control the oxygen reduction reaction (ORR) pathway. This breakthrough enables efficient hydrogen peroxide (H2O2) production and energy conversion, paving the way for advanced electrocatalysts.
Area of Science:
- Electrochemistry
- Materials Science
- Catalysis
Background:
- Single-atom catalysts (SACs) offer tunable pathways for the oxygen reduction reaction (ORR), producing either energy (4e-) or hydrogen peroxide (2e-).
- Controlling ORR selectivity in SACs is difficult due to challenges in fine-tuning coordination structures.
- Existing strategies lack precise methods for steering the ORR pathway between 2e- and 4e- reactions.
Purpose of the Study:
- To develop a curvature engineering strategy for continuous steering of the ORR pathway in copper-based SACs.
- To investigate the mechanism by which curvature influences ORR activity and selectivity.
- To demonstrate the application of engineered SACs in efficient hydrogen peroxide electrosynthesis.
Main Methods:
- Curvature engineering of carbon nanotubes (CNTs) to create SACs with varying substrate curvature.
- Theoretical calculations (e.g., DFT) to elucidate reaction mechanisms.
- In-situ spectroscopy to analyze active site behavior and interfacial water dynamics.
- Electrochemical testing in a solid-electrolyte electrolyzer for hydrogen peroxide production.
Main Results:
- A novel curvature engineering strategy successfully controlled the ORR pathway from 2e- to 4e- over Cu-SACs.
- High-curvature CNTs yielded 4e- ORR performance comparable to Pt/C, while low-curvature CNTs achieved 99.5% 2e- selectivity.
- Tensile strain and water restructuring at the active site were identified as key mechanistic factors.
- Proof-of-concept electrolyzer demonstrated high H2O2 Faradaic efficiencies (96.4% at 200 mA cm-2, 92.5% at 300 mA cm-2) and stability (>100 h).
Conclusions:
- Curvature engineering is established as a powerful descriptor for precisely regulating SACs in ORR.
- This strategy enables the rational design of advanced electrocatalysts for selective H2O2 production and energy conversion.
- The findings open new avenues for optimizing catalyst performance through substrate geometry control.
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