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Metal–Organic Frameworks Mediate Cu Coordination for Selective CO2 Electroreduction
- Source :
- Journal of the American Chemical Society. 140:11378-11386
- Publication Year :
- 2018
- Publisher :
- American Chemical Society (ACS), 2018.
-
Abstract
- The electrochemical carbon dioxide reduction reaction (CO2RR) produces diverse chemical species. Cu clusters with a judiciously controlled surface coordination number (CN) provide active sites that simultaneously optimize selectivity, activity, and efficiency for CO2RR. Here we report a strategy involving metal–organic framework (MOF)-regulated Cu cluster formation that shifts CO2 electroreduction toward multiple-carbon product generation. Specifically, we promoted undercoordinated sites during the formation of Cu clusters by controlling the structure of the Cu dimer, the precursor for Cu clusters. We distorted the symmetric paddle-wheel Cu dimer secondary building block of HKUST-1 to an asymmetric motif by separating adjacent benzene tricarboxylate moieties using thermal treatment. By varying materials processing conditions, we modulated the asymmetric local atomic structure, oxidation state and bonding strain of Cu dimers. Using electron paramagnetic resonance (EPR) and in situ X-ray absorption spectros...
- Subjects :
- Dimer
Coordination number
02 engineering and technology
General Chemistry
010402 general chemistry
021001 nanoscience & nanotechnology
01 natural sciences
Biochemistry
Tricarboxylate
Catalysis
0104 chemical sciences
law.invention
chemistry.chemical_compound
Crystallography
Colloid and Surface Chemistry
chemistry
law
Oxidation state
Metal-organic framework
0210 nano-technology
Selectivity
Electron paramagnetic resonance
Electrochemical reduction of carbon dioxide
Subjects
Details
- ISSN :
- 15205126 and 00027863
- Volume :
- 140
- Database :
- OpenAIRE
- Journal :
- Journal of the American Chemical Society
- Accession number :
- edsair.doi...........37cd56502021f202d45323364093aa14