Facet-dependent photocatalytic NO conversion pathways predetermined by adsorption activation patterns
Photocatalysts with different exposed facets generally exhibit different physicochemical properties, but the underlying mechanism has not been revealed. In this study, we synthesized nanoflake-assembled flower-like Bi2O2CO3 and homodisperse nanoflakes Bi2O2CO3 with exposed {110} and {001} facets (110-BOC and 001-BOC), respectively, to probe the activation and reaction mechanism of facet-dependent reactants. The results showed that Bi2O2CO3 with exposed {001} facets exhibited superior photocatalytic activity for photocatalytic abatement of NO in the air in comparison with 110-BOC. According to the combined results of ESR spectra and DFT calculation, the superior photocatalytic activity of 001-BOC stemmed from its enhanced capability to activate the reactants (O2 and H2O), which facilitated the formation of reactive radicals to participate in the photocatalytic NO oxidation. Most significantly, the time-dependent in situ DRIFTS spectra and DFT simulation results reveal that the adsorption activation of pollutants and desorption mechanisms of products were different for 110-BOC and 001-BOC in photocatalytic NO oxidation. Due to the differences in the atomic arrangement on the {110} and {001} facets, 001-BOC enabled the transformation of NO into NO- or cis-N2O22- during adsorption activation, while 110-BOC induces the adsorption activation of NO into NO+ or N2O3. The {001} facet of Bi2O2CO3 could promote the oxidation of intermediates to final products (NO3-) and enhance NO3- desorption. These different adsorption activation patterns on {110} and {001} facets essentially predetermined the facet-dependent conversion pathways of photocatalytic NO oxidation on different facets. The findings of this work would have critical implications for the understanding of the facet-dependent reaction mechanism and the design of novel efficient catalysts.
| Medienart: |
E-Artikel |
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| Erscheinungsjahr: |
2019 |
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| Erschienen: |
2019 |
| Enthalten in: |
Zur Gesamtaufnahme - volume:11 |
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| Enthalten in: |
Nanoscale - 11(2019), 5 vom: 31. Jan., Seite 2366-2373 |
| Sprache: |
Englisch |
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| Beteiligte Personen: |
Chen, Peng [VerfasserIn] |
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| Themen: |
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| Anmerkungen: |
Date Completed 31.01.2019 Date Revised 31.01.2019 published: Print Citation Status PubMed-not-MEDLINE |
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| doi: |
10.1039/c8nr09147a |
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| funding: |
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| Förderinstitution / Projekttitel: |
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NLM292940068 |
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| 500 | |a Date Revised 31.01.2019 | ||
| 500 | |a published: Print | ||
| 500 | |a Citation Status PubMed-not-MEDLINE | ||
| 520 | |a Photocatalysts with different exposed facets generally exhibit different physicochemical properties, but the underlying mechanism has not been revealed. In this study, we synthesized nanoflake-assembled flower-like Bi2O2CO3 and homodisperse nanoflakes Bi2O2CO3 with exposed {110} and {001} facets (110-BOC and 001-BOC), respectively, to probe the activation and reaction mechanism of facet-dependent reactants. The results showed that Bi2O2CO3 with exposed {001} facets exhibited superior photocatalytic activity for photocatalytic abatement of NO in the air in comparison with 110-BOC. According to the combined results of ESR spectra and DFT calculation, the superior photocatalytic activity of 001-BOC stemmed from its enhanced capability to activate the reactants (O2 and H2O), which facilitated the formation of reactive radicals to participate in the photocatalytic NO oxidation. Most significantly, the time-dependent in situ DRIFTS spectra and DFT simulation results reveal that the adsorption activation of pollutants and desorption mechanisms of products were different for 110-BOC and 001-BOC in photocatalytic NO oxidation. Due to the differences in the atomic arrangement on the {110} and {001} facets, 001-BOC enabled the transformation of NO into NO- or cis-N2O22- during adsorption activation, while 110-BOC induces the adsorption activation of NO into NO+ or N2O3. The {001} facet of Bi2O2CO3 could promote the oxidation of intermediates to final products (NO3-) and enhance NO3- desorption. These different adsorption activation patterns on {110} and {001} facets essentially predetermined the facet-dependent conversion pathways of photocatalytic NO oxidation on different facets. The findings of this work would have critical implications for the understanding of the facet-dependent reaction mechanism and the design of novel efficient catalysts | ||
| 650 | 4 | |a Journal Article | |
| 700 | 1 | |a Sun, Yanjuan |e verfasserin |4 aut | |
| 700 | 1 | |a Liu, Hongjing |e verfasserin |4 aut | |
| 700 | 1 | |a Zhou, Ying |e verfasserin |4 aut | |
| 700 | 1 | |a Jiang, Guangming |e verfasserin |4 aut | |
| 700 | 1 | |a Lee, S C |e verfasserin |4 aut | |
| 700 | 1 | |a Zhang, Yuxin |e verfasserin |4 aut | |
| 700 | 1 | |a Dong, Fan |e verfasserin |4 aut | |
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| 773 | 1 | 8 | |g volume:11 |g year:2019 |g number:5 |g day:31 |g month:01 |g pages:2366-2373 |
| 856 | 4 | 0 | |u http://dx.doi.org/10.1039/c8nr09147a |3 Volltext |
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