Abstract
Electrochemical reduction of CO2 into value-added chemicals should reduce the consumption of fossil fuels and counteract global warming caused by CO2 generation. Nonetheless, CO2 is rather stable and chemically inert, calling for effective electrocatalysts to avoid problems such as sluggish kinetics, low reaction efficiency and poor product selectivity during CO2 conversion. Recently, single-atom catalysts have shown maximum atom utilization and unique catalytic performance during electrochemical reactions. Catalysts used have been developed from poorly controlled nanoparticles or nanoclusters to isolated atomic structures. Herein, we review the preparation, characterization, anchoring strategies and electrochemical applications of single-atom catalysts. Concerning methods of preparation, the use of organometallic ligands shows high potential for synthesis and industrial applications. Both characterization and calculations using the density functional theory allow to assess the atomic distribution, the coordination environment and the catalytic mechanism. To improve synthesis, we present four anchoring strategies: defect engineering, atom coordination, spatial confinement and sacrifice template. Applications in electrochemical reduction of CO2 to liquid and gaseous products reveal Faraday efficiency higher than 90%, excellent activity, selectivity, stability and kinetic properties.
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Copyright 2017, American Chemical Society
Copyright 2017, American Chemical Society. Modified after Liu et al. (2017)
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Abbreviations
- CO:
-
Carbon monoxide
- CO2 :
-
Carbon dioxide
- CO2RR:
-
CO2 reduction reaction
- C:
-
Carbon
- N:
-
Nitrogen
- O:
-
Oxygen
- S:
-
Sulfur
- CH4 :
-
Methane
- ALD:
-
Atomic layer deposition
- NH3BH3 :
-
Ammonia borane
- H2 :
-
Hydrogen
- HCHO:
-
Formaldehyde
- OH:
-
Hydroxyl
- HCOOH:
-
Formic acid
- TS1:
-
Transition state 1
- TS2:
-
Transition state 2
- TS3:
-
Transition state 3
- MCM:
-
Multichannel carbon matrix
- HCNS:
-
Hollow carbon nitride microsphere
- TCNFs:
-
Through-hole carbon nanofibers
- PHMs:
-
Porous hollow microspheres
- FE:
-
Faraday efficiency
- HPC:
-
Hollow porous carbon
- PS:
-
Polystyrene
- N–C:
-
Nitrogen–doped carbon
- S–C:
-
Sulfur–doped carbon
- G:
-
Graphene
- N–G:
-
Nitrogen–doped graphene
- CNS:
-
Carbon nanosheets
- ISAS:
-
Isolated single-atom sites
- SA:
-
Single atom
- ISA:
-
Isolated single atom
- SAA:
-
Single-atom alloys
- Def:
-
Defective
- NP:
-
Nanoparticles
- NRR:
-
Nitrogen reduction reaction
- OER:
-
Oxygen evolution reaction
- HER:
-
Hydrogen evolution reaction
- STEM:
-
Scanning transmission electron microscopy
- HAADF-STEM:
-
High-angle annular dark-field scanning transmission electron microscopy
- XRD:
-
X-ray diffraction
- TEM:
-
Transmission electron microscopy
- XPS:
-
X-ray photoelectron spectroscopy
- XAS:
-
X-ray spectroscopy
- XANES:
-
X-ray absorption structure spectroscopy
- EXAFS:
-
Extended X-ray absorption fine structure spectroscopy
- DRIFTS:
-
Diffuse reflected Fourier transform infrared spectroscopy
- NMR:
-
Nuclear magnetic resonance
- DFT:
-
Density functional theory calculation
- EDS:
-
Energy dispersive X-ray spectroscopy
- EELS:
-
Electron energy loss spectroscopy
- PHMs:
-
Porous hollow microspheres
- E. coli :
-
Escherichia coli
- WT:
-
Wavelet transform
- ICP:
-
Inductively coupled plasma
- HAP:
-
Hydroxyapatite
- HNPCS:
-
Hollow N-doped porous carbon spheres
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We are very grateful for the financial support of the National Natural Science Foundation of China (Grant Nos. 21978043, U1662130), and we sincerely thank the reviewers for their valuable time and constructive comments.
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Sun, JF., Wu, JT., Xu, QQ. et al. CO2 electrochemical reduction using single-atom catalysts. Preparation, characterization and anchoring strategies: a review. Environ Chem Lett 18, 1593–1623 (2020). https://doi.org/10.1007/s10311-020-01023-8
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DOI: https://doi.org/10.1007/s10311-020-01023-8