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Experimental and Computational Investigation of Au25 Clusters and CO2: A Unique Interaction and Enhanced Electrocatalytic Activity
Open accessAbstract
Atomically precise, inherently charged Au(25) clusters are an exciting prospect for promoting catalytically challenging reactions, and we have studied the interaction between CO(2) and Au(25). Experimental results indicate a reversible Au(25)-CO(2) interaction that produced spectroscopic and electrochemical changes similar to those seen with cluster oxidation. Density functional theory (DFT) modeling indicates these changes stem from a CO(2)-induced redistribution of charge within the cluster. Identification of this spontaneous coupling led to the application of Au(25) as a catalyst for the electrochemical reduction of CO(2) in aqueous media. Au(25) promoted the CO(2) → CO reaction within 90 mV of the formal potential (thermodynamic limit), representing an approximate 200-300 mV improvement over larger Au nanoparticles and bulk Au. Peak CO(2) conversion occurred at -1 V (vs RHE) with approximately 100% efficiency and a rate 7-700 times higher than that for larger Au catalysts and 10-100 times higher than those for current state-of-the-art processes.
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Metadata
- Authors
- Kauffman, D. R., Alfonso, D., Matranga, C., Qian, H., & Jin, R.
- Venue
- Journal of the American Chemical Society
- Publisher
- American Chemical Society (ACS)
- Published
- 2012-06-06
- Volume
- 134
- Issue
- 24
- Pages
- 10237-10243
- ISSN
- 0002-7863 (ISSN-L)
- 1520-5126
- OpenAlex
- W2002516293
- Cited by
- 451
- References
- 43
- FWCI
- 8.87
- Type
- journal article
- Language
- en
- Open access
- bronze
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