Stabilized Cuδ+-OH species on in situ reconstructed Cu nanoparticles for CO2-to-C2H4 conversion in neutral media
Achieving large-scale electrochemical CO<sub>2</sub> reduction to multicarbon products with high selectivity using membrane electrode assembly (MEA) electrolyzers in neutral electrolyte is promising for carbon neutrality. However, the unsatisfactory multicarbon products selectivity and unclear reaction mechanisms in an MEA have hindered its further development. Here, we report a strategy that manipulates the interfacial microenvironment of Cu nanoparticles in an MEA to suppress hydrogen evolution reaction and enhance C<sub>2</sub>H<sub>4</sub> conversion. In situ multimodal characterizations consistently reveal well-stabilized Cu<sup>δ+</sup>-OH species as active sites during MEA testing. The OH radicals generated in situ from water create a locally oxidative microenvironment on the copper surface, stabilizing the Cu<sup>δ+</sup> species and leading to an irreversible and asynchronous change in morphology and valence, yielding high-curvature nanowhiskers. Consequently, we deliver a selective C<sub>2</sub>H<sub>4</sub> production with a Faradaic efficiency of 55.6% ± 2.8 at 316 mA cm<sup>-2</sup> in neutral media.
Authors
- Rodney D. L. Smith (ORCID: https://orcid.org/0000-0003-1209-9653)
- Yimin A. Wu (ORCID: https://orcid.org/0000-0002-3807-8431)
- Ning Chen (ORCID: https://orcid.org/0000-0002-1269-6119)
- Holly M. Fruehwald (ORCID: https://orcid.org/0000-0002-4822-4359)
- Dmitry Akhmetzyanov (ORCID: https://orcid.org/0009-0003-4632-0288)
- Zhiwen Chen (ORCID: https://orcid.org/0000-0002-0155-2101)
- Zhongchao Tan (ORCID: https://orcid.org/0000-0001-7922-8291)
- Lei Wang (ORCID: https://orcid.org/0000-0001-7275-4846)
- Yi Feng Xiao (ORCID: https://orcid.org/0000-0001-6318-8010)
- Brant Billinghurst (ORCID: https://orcid.org/0000-0002-5346-5317)
- Chandra Veer Singh (ORCID: https://orcid.org/0000-0002-6644-0178)
- Xiyang Wang (ORCID: https://orcid.org/0000-0002-7591-6676)
- Linke Huang
- Zuolong Chen
- Mathew Hanson
Institutions
- University of Waterloo (CA)
- University of Toronto (CA)
- Zhejiang Business Technology Institute (CN)
- Canadian Light Source (Canada) (CA)
Publication Details
- Journal
- Nature Communications
- Published
- 2024-08-29
- DOI
- https://doi.org/10.1038/s41467-024-52004-2
- Citations
- 48
- Primary Topic
- CO2 Reduction Techniques and Catalysts
- Type
- article
- Field-Weighted Citation Impact
- 4.91
Funders
- Canadian Light Source
- Ontario Research Foundation
- University of Toronto
- Canada First Research Excellence Fund
- Canadian Institutes of Health Research
- Natural Sciences and Engineering Research Council of Canada