Catalytic NO Oxidation in the Presence of Moisture Using Porous ...

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Catalytic NO Oxidation in the Presence of Moisture Using Porous Polymers and Activated Carbon Mohsen Ghafari and John D. Atkinson* Department of Civil, Structural, and Environmental Engineering, State University of New York at Buffalo, Buffalo, New York 14260, United States ABSTRACT: NO oxidation catalyzed by porous materials is difficult to implement under industrial conditions because moisture in combustion exhaust streams blocks oxidation sites, decreasing NO conversion. In this work, hydrophobic crosslinked polymers are tested as NO oxidation catalysts to overcome these negative impacts associated with moisture. Although activated carbons (ACs) outperform hyper-cross-linked polymers by >88% and low-cross-linked polymers by >463% under dry conditions, their NO conversion drops to 0% when 50% relative humidity is added. Performance of hyper-cross-linked and lowcross-linked polymers, however, decreases by only 19−35% and 40 yr ago,12,13 NOx absorption has gained research traction over the past 5 yr due to continued need for improved stationary source NOx control.14−19 NO, which comprises >90% of NOx in combustion flue gas, has low solubility in water ( XAD4 (0.21 mmol/g) > XAD16N (0.17 mmol/g). The small amount of adsorbed NO for the low-cross-linked polymers justifies their small hydrophilicity increase after NO oxidation (Table 2). However, total NO2 reduction by low-cross-linked polymers remains much lower than hyper-cross-linked polymers (>71% lower) and ACs (>92% lower). Differences in performance of the three classes of catalysts are attributed to differences in their chemical properties, causing different interactions with water (Table 2) and different reactivity with NO2 (Figure 4). AC contains reactive sites at the edges of graphene sheets64 that chemisorb NOx and become oxidized (NO2 reduction with oxygen deposition).62 This is attributed to AC’s structure, which contains unpaired electrons due to the breaking of bonds at the edges of the aromatic sheets that can interact with heteroatoms such as oxygen and nitrogen.47 Polymers do not have similar reactive edge sites. This is an important result, with wide-reaching implications, because industrial AC performance can be hindered by its notable reactivity with other gas components. For example, AC chemisorbs O2 (increasing hydrophilicity), reduces NO2 to NO (generating surface oxygen groups and increasing hydrophilicity), and reacts with SO2 (potentially resulting in the formation and deposition of sulfur complexes on the carbon surface).47,61,65 This is the first study to compare surface reactivity of polymeric materials and AC in an air pollution control application. Identifying the opportunity to wield a

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AUTHOR INFORMATION

Corresponding Author

*Phone: 716-645-4001; fax: 716-645-3667; e-mail: AtkJDW@ buffalo.edu (J.D.A.). Notes

The authors declare no competing financial interest.

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ACKNOWLEDGMENTS The authors gratefully acknowledge the State University of New York at Buffalo’s Furnas Hall Materials Characterization Laboratory for providing access to the nitrogen adsorption analyzer and technical assistance with operation and analysis.

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REFERENCES

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DOI: 10.1021/acs.est.5b05443 Environ. Sci. Technol. 2016, 50, 5189−5196

Article

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