The regulation mechanism of a zero-dimensional interface towards a catalytic reaction in the setting of a single-atom catalyst has been elusive to researchers. In a recent article published in Journal of the American Chemical Society, Zeng and Zhou et al. differentiated the electronic and steric effects on the oxygen evolution reaction at two distinct zero-dimensional interfaces. The steric interaction resulted in the desired adsorption behavior of intermediates at the interface, which lowered the energy barrier to the rate-determining step (RDS) and thus facilitated the oxygen evolution reaction. For the first time, this work validated the impacts of electronic and steric effects on the atomic interface of catalysts by delicately designing the anchoring site of single atoms on the support. The elegant design concept presented in this work pushes the research field of interface engineering to the atomic level and blazes a trail for the rational development of high-performing catalysts.
The regulation mechanism of a zero-dimensional interface towards a catalytic reaction in the setting of a single-atom catalyst has been elusive to researchers. In a recent article published in Journal of the American Chemical Society, Zeng and Zhou et al. differentiated the electronic and steric effects on the oxygen evolution reaction at two distinct zero-dimensional interfaces. The steric interaction resulted in the desired adsorption behavior of intermediates at the interface, which lowered the energy barrier to the rate-determining step (RDS) and thus facilitated the oxygen evolution reaction. For the first time, this work validated the impacts of electronic and steric effects on the atomic interface of catalysts by delicately designing the anchoring site of single atoms on the support. The elegant design concept presented in this work pushes the research field of interface engineering to the atomic level and blazes a trail for the rational development of high-performing catalysts.
[1] |
Huang W X, Li W X. Surface and interface design for heterogeneous catalysis. Phys. Chem. Chem. Phys., 2019, 21: 523–536. doi: 10.1039/C8CP05717F
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[2] |
Kim D, Resasco J, Yu Y, et al. Synergistic geometric and electronic effects for electrochemical reduction of carbon dioxide using gold-copper bimetallic nanoparticles. Nat. Commun., 2014, 5: 4948. doi: 10.1038/ncomms5948
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van Deelen T W, Hernández Mejía C, de Jong K P. Control of metal-support interactions in heterogeneous catalysts to enhance activity and selectivity. Nat. Catal., 2019, 2: 955–970. doi: 10.1038/s41929-019-0364-x
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[4] |
Wang H, Wang L, Lin D, et al. Strong metal-support interactions on gold nanoparticle catalysts achieved through Le Chatelier’s principle. Nat. Catal., 2021, 4: 418–424. doi: 10.1038/s41929-021-00611-3
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[5] |
Wang Y, Su H, He Y, et al. Advanced electrocatalysts with single-metal-atom active sites. Chem. Rev., 2020, 120: 12217–12314. doi: 10.1021/acs.chemrev.0c00594
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[6] |
Lang R, Du X R, Huang Y K, et al. Single-atom catalysts based on the metal–oxide interaction. Chem. Rev., 2020, 120: 11986–12043. doi: 10.1021/acs.chemrev.0c00797
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[7] |
Feng C, Zhang Z R, Wang D D, et al. Tuning the electronic and steric interaction at the atomic interface for enhanced oxygen evolution. J. Am. Chem. Soc., 2022, 144: 9271–9279. doi: 10.1021/jacs.2c00533
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[8] |
Pérez-Ramírez J, López N. Strategies to break linear scaling relationships. Nat. Catal., 2019, 2: 971–976. doi: 10.1038/s41929-019-0376-6
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[9] |
Man I C, Su H Y, Calle-Vallejo F, et al. Universality in oxygen evolution electrocatalysis on oxide surfaces. ChemCatChem, 2011, 3: 1159–1165. doi: 10.1002/cctc.201000397
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[10] |
Seh Z W, Kibsgaard J, Dickens C F, et al. Combining theory and experiment in electrocatalysis: Insights into materials design. Science, 2017, 355: eaad4998. doi: 10.1126/science.aad4998
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Figure 1. Regulating the steric effect at the zero-dimensional interface. (a) The side view and (b) top view of Ir1/CoOOHlat; (c) the side view and (d) top view of Ir1/CoOOHsur. (e) The free energy diagrams of Ir1/CoOOHlat and Ir1/CoOOHsur towards OER. (f) The specific activities of Ir1/CoOOHlat and Ir1/CoOOHsur at an overpotential of 300 mV. Adapted with permission from Ref. [7]. Copyright 2022, American Chemical Society.
[1] |
Huang W X, Li W X. Surface and interface design for heterogeneous catalysis. Phys. Chem. Chem. Phys., 2019, 21: 523–536. doi: 10.1039/C8CP05717F
|
[2] |
Kim D, Resasco J, Yu Y, et al. Synergistic geometric and electronic effects for electrochemical reduction of carbon dioxide using gold-copper bimetallic nanoparticles. Nat. Commun., 2014, 5: 4948. doi: 10.1038/ncomms5948
|
[3] |
van Deelen T W, Hernández Mejía C, de Jong K P. Control of metal-support interactions in heterogeneous catalysts to enhance activity and selectivity. Nat. Catal., 2019, 2: 955–970. doi: 10.1038/s41929-019-0364-x
|
[4] |
Wang H, Wang L, Lin D, et al. Strong metal-support interactions on gold nanoparticle catalysts achieved through Le Chatelier’s principle. Nat. Catal., 2021, 4: 418–424. doi: 10.1038/s41929-021-00611-3
|
[5] |
Wang Y, Su H, He Y, et al. Advanced electrocatalysts with single-metal-atom active sites. Chem. Rev., 2020, 120: 12217–12314. doi: 10.1021/acs.chemrev.0c00594
|
[6] |
Lang R, Du X R, Huang Y K, et al. Single-atom catalysts based on the metal–oxide interaction. Chem. Rev., 2020, 120: 11986–12043. doi: 10.1021/acs.chemrev.0c00797
|
[7] |
Feng C, Zhang Z R, Wang D D, et al. Tuning the electronic and steric interaction at the atomic interface for enhanced oxygen evolution. J. Am. Chem. Soc., 2022, 144: 9271–9279. doi: 10.1021/jacs.2c00533
|
[8] |
Pérez-Ramírez J, López N. Strategies to break linear scaling relationships. Nat. Catal., 2019, 2: 971–976. doi: 10.1038/s41929-019-0376-6
|
[9] |
Man I C, Su H Y, Calle-Vallejo F, et al. Universality in oxygen evolution electrocatalysis on oxide surfaces. ChemCatChem, 2011, 3: 1159–1165. doi: 10.1002/cctc.201000397
|
[10] |
Seh Z W, Kibsgaard J, Dickens C F, et al. Combining theory and experiment in electrocatalysis: Insights into materials design. Science, 2017, 355: eaad4998. doi: 10.1126/science.aad4998
|