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Copper nanoparticle ensembles for selective electroreduction of CO2 to C2–C3 products
| Content Provider | eScholarship Repository: University of California |
|---|---|
| Author | Kim, Dohyung Kley, Christopher S Li, Yifan Yang, Peidong |
| Abstract | Direct conversion of carbon dioxide to multicarbon products remains as a grand challenge in electrochemical CO2 reduction. Various forms of oxidized copper have been demonstrated as electrocatalysts that still require large overpotentials. Here, we show that an ensemble of Cu nanoparticles (NPs) enables selective formation of C2-C3 products at low overpotentials. Densely packed Cu NP ensembles underwent structural transformation during electrolysis into electrocatalytically active cube-like particles intermixed with smaller nanoparticles. Ethylene, ethanol, and n-propanol are the major C2-C3 products with onset potential at -0.53 V (vs. reversible hydrogen electrode, RHE) and C2-C3 faradaic efficiency (FE) reaching 50% at only -0.75 V. Thus, the catalyst exhibits selective generation of C2-C3 hydrocarbons and oxygenates at considerably lowered overpotentials in neutral pH aqueous media. In addition, this approach suggests new opportunities in realizing multicarbon product formation from CO2, where the majority of efforts has been to use oxidized copper-based materials. Robust catalytic performance is demonstrated by 10 h of stable operation with C2-C3 current density 10 mA/cm2 (at -0.75 V), rendering it attractive for solar-to-fuel applications. Tafel analysis suggests reductive CO coupling as a rate determining step for C2 products, while n-propanol (C3) production seems to have a discrete pathway. |
| File Format | |
| ISSN | 00278424 |
| Conference Proceedings | Proceedings of the National Academy of Sciences of the United States of America |
| DOI | 10.1073/pnas.1711493114 |
| Alternate Webpage(s) | https://escholarship.org/uc/item/4kw2z3hf |
| Issue Number | 40 |
| Volume Number | 114 |
| Language | English |
| Publisher Date | 2017-10-03 |
| Access Restriction | Open |
| Subject Keyword | Heterogeneous Catalysis Electrocatalysis Copper Nanoparticles In Situ Structural Transformation Engineering Chemical Sciences Nanotechnology Bioengineering Affordable and Clean Energy CO2 reduction CSD-02-CAT-A |
| Content Type | Text |
| Resource Type | Article |