Abstract
Copper nanostructures are promising catalysts for the electrochemical reduction of CO2 because of their unique ability to produce a large proportion of multi-carbon products. Despite great progress, the selectivity and stability of such catalysts still need to be substantially improved. Here, we demonstrate that controlling the surface oxidation of Cu nanowires (CuNWs) can greatly improve their C2+ selectivity and stability. Specifically, we achieve a faradaic efficiency as high as 57.7 and 52.0 % for ethylene when the CuNWs are oxidized by the O2 from air and aqueous H2O2, respectively, and both of them show hydrogen selectivity below 12 %. The high yields of C2+ products can be mainly attributed to the increase in surface roughness and the generation of defects and cavities during the electrochemical reduction of the oxide layer. Our results also indicate that the formation of a relatively thick, smooth oxide sheath can improve the catalytic stability by mitigating the fragmentation issue.
| Original language | English |
|---|---|
| Pages (from-to) | 1909-1915 |
| Number of pages | 7 |
| Journal | Angewandte Chemie - International Edition |
| Volume | 60 |
| Issue number | 4 |
| DOIs | |
| State | Published - Jan 25 2021 |
Funding
This work was supported in part by a grant from the NSF (CHE 1804970), start‐up funds from the Georgia Institute of Technology, two grants from the Research Grant Council of Hong Kong SAR (26206115 and 16309418), and one from Hong Kong Branch of Southern Marine Science and Engineering Guangdong Laboratory (SMSEGL20SC01). TEM and STEM imaging were performed at the Materials Characterization Facilities of the GT's Institute of Electronics and Nanotechnology (IEN), a member of the National Nanotechnology Coordinated Infrastructure (NNCI) and supported by the National Science Foundation (ECCS‐1542174). Part of the STEM imaging and EELS mapping in this research were completed at the Center for Nanophase Materials Sciences, which is a DOE Office of Science User Facility. S. Zhu thanks the financial support from Research Grant Council Postdoctoral Fellowship Scheme (PDFS2021‐6S08). We thank Prof. Mingjie Zhang and Mr. Rui Feng from HKUST for providing the NMR facility. This work was supported in part by a grant from the NSF (CHE 1804970), start-up funds from the Georgia Institute of Technology, two grants from the Research Grant Council of Hong Kong SAR (26206115 and 16309418), and one from Hong Kong Branch of Southern Marine Science and Engineering Guangdong Laboratory (SMSEGL20SC01). TEM and STEM imaging were performed at the Materials Characterization Facilities of the GT's Institute of Electronics and Nanotechnology (IEN), a member of the National Nanotechnology Coordinated Infrastructure (NNCI) and supported by the National Science Foundation (ECCS-1542174). Part of the STEM imaging and EELS mapping in this research were completed at the Center for Nanophase Materials Sciences, which is a DOE Office of Science User Facility. S. Zhu thanks the financial support from Research Grant Council Postdoctoral Fellowship Scheme (PDFS2021-6S08). We thank Prof. Mingjie Zhang and Mr. Rui Feng from HKUST for providing the NMR facility.
| Funders | Funder number |
|---|---|
| Center for Nanophase Materials Sciences | |
| Research Grant Council | |
| Research Grant Council of Hong Kong | |
| National Science Foundation | CHE 1804970, ECCS‐1542174, 1804970 |
| Office of Science | |
| Georgia Institute of Technology | |
| Research Grants Council, University Grants Committee | 16309418, 26206115 |
| Hong Kong Branch of Southern Laboratory of Ocean Science and Engineering Guangdong Laboratory | SMSEGL20SC01 |
Keywords
- C selectivity
- copper nanowires
- electrochemical CO reduction
- nanocatalysis
- surface oxidation
