Journal
NANOSCALE
Volume 11, Issue 5, Pages 2366-2373Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/c8nr09147a
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Funding
- National Natural Science Foundation of China [21822601, 21777011, 21501016]
- National Key RD Plan [2016YFC02047]
- Innovative Research Team of Chongqing [CXTDG201602014]
- Key Natural Science Foundation of Chongqing [cstc2017jcyjBX0052]
- Plan for National Youth Talents of the Organization Department of the Central Committee
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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 (O-2 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.
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