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Self-Assembled Monolayer Interface with Reconstructed Hydrogen-Bond Network for Enhanced CO2 Electroreduction.
Yuantao Wei1, Jianrui Zhang1, Boyang Li1
1Engineering Research Center of Energy Storage Materials and Devices, Ministry of Education, School of Chemistry, Xi'an Jiaotong University, Xi'an, 710049, China.
Advanced Materials (Deerfield Beach, Fla.)
|May 7, 2025
Summary
Interface engineering with self-assembled monolayers enhances carbon dioxide electrolysis (CO2RR) for producing valuable multi-carbon products. This strategy optimizes mass transport and ion-electron transfer, boosting catalyst performance and selectivity for C2+ products.
Area of Science:
- Electrochemistry and Catalysis
- Materials Science
- Chemical Engineering
Background:
- Carbon dioxide electrolysis (CO2RR) is crucial for reducing CO2 emissions and producing high-value multi-carbon (C2+) products.
- Catalyst performance in CO2RR is significantly influenced by the reaction microenvironment, in addition to the electrocatalyst itself.
- Optimizing the interface between the catalyst and reactants is key to improving efficiency and selectivity.
Purpose of the Study:
- To develop an interface engineering strategy for enhancing CO2 electrolysis performance.
- To investigate the role of a reconstructed hydrogen-bond network in facilitating mass transport and ion-electron transfer.
- To improve the selectivity towards C2+ products in CO2RR.
Main Methods:
- Fabrication of a composite catalyst (Cu@F-Si) using co-assembly of fluorinated self-assembled monolayers (F-SAM) and siloxane on a commercial Cu catalyst.
- Molecular dynamics simulations (MDS) to analyze mass transport and interfacial properties.
- Density functional theory (DFT) calculations to elucidate reaction mechanisms and optimize surface coverages.
Main Results:
- The Cu@F-Si catalyst demonstrated facilitated CO2 mass transport and maintained ideal H+/e- transfer pathways.
- Optimized *H/*CO coverage was identified as a key factor for enhancing C2+ product selectivity.
- Achieved high current density (502.5 mA cm-2) with over 85% C2+ Faradaic efficiency and stable operation (>100 h).
Conclusions:
- Interface engineering using SAMs with reconstructed hydrogen-bond networks is an effective strategy for CO2RR.
- This approach significantly improves mass transport, ion-electron transfer, and C2+ selectivity.
- The developed strategy offers a promising solution for efficient CO2 conversion with broad applicability in multiphase catalysis.
