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Quantum Mechanical Screening of Single-Atom Bimetallic Alloys for the Selective Reduction of CO2 to C1 Hydrocarbons
Open accessAbstract
Electrocatalytic reduction of CO 2 to energy-rich hydrocarbons such as alkanes, alkenes, and alcohols is a very challenging task. So far, only copper has proven to be capable of such a conversion. We report density functional theory (DFT) calculations combined with the Poisson–Boltzmann implicit solvation model to show that single-atom alloys (SAAs) are promising electrocatalysts for CO 2 reduction to C 1 hydrocarbons in aqueous solution. The majority component of the SAAs studied is either gold or silver, in combination with isolated single atoms, M (M = Cu, Ni, Pd, Pt, Co, Rh, and Ir), replacing surface atoms. We envision that the SAA behaves as a one-pot tandem catalyst: first gold (or silver) reduces CO 2 to CO, and the newly formed CO is then captured by M and is further reduced to C 1 hydrocarbons such as methane or methanol. We studied 28 SAAs, and found about half of them selectively favor the CO 2 reduction reaction over the competing hydrogen evolution reaction. Most of those promising SAAs contain M = Co, Rh, or Ir. The reaction mechanism of two SAAs, Rh@Au(100) and Rh@Ag(100), is explored in detail. Both of them reduce CO 2 to methane but via different pathways. For Rh@Au(100), reduction occurs through the pathway *CO → *CHO → *CHOH → *CH + H 2 O ( l ) → *CH 2 + H 2 O ( l ) → *CH 3 + H 2 O ( l ) → * + H 2 O ( l ) + CH 4( g ); whereas, for Rh@Ag(100), the pathway is *CO → *CHO → *CH 2 O→ *OCH 3 → *O + CH 4( g ) → *OH + CH 4( g ) → * + H 2 O ( l ) + CH 4( g ) . The minimum applied voltages to drive the two electrocatalytic systems are −1.01 and −1.12 V RHE for Rh@Au(100) and Rh@Ag(100), respectively, at which the Faradaic efficiencies for CO 2 reduction to CO are 60% for gold and 90% for silver. This suggests that SAA can efficiently reduce CO 2 to methane with as small as 40% loss to the hydrogen evolution reaction for Rh@Au(100) and as small as 10% for Rh@Ag(100). We hope these computational results can stimulate experimental efforts to explore the use of SAA to catalyze CO 2 electrochemical reduction to hydrocarbons.
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Metadata
- Authors
- Cheng, M.-J., Clark, E. L., Pham, H. H., Bell, A. T., & Head-Gordon, M.
- Venue
- ACS Catalysis
- Publisher
- American Chemical Society (ACS)
- Published
- 2016-10-17
- Volume
- 6
- Issue
- 11
- Pages
- 7769-7777
- ISSN
- 2155-5435 (ISSN-L)
- OpenAlex
- W2522872739
- Cited by
- 233
- References
- 15
- FWCI
- 5.45
- Type
- journal article
- Language
- en
- Open access
- green
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