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Theoretical and Experimental Evidence for the Carbon-Oxygen Group Enhancement of NO Reduction

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Authors
Li, J.
Wang, Y.
Song, J.
Gao, Q.
Zhang, J.
Zhang, J.
Zhai, D.
Zhou, J.
Liu, Jian
Xu, Z.
Qian, G.
Liu, Y.
Date
2017
Type
Journal Article

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Li, J. and Wang, Y. and Song, J. and Gao, Q. and Zhang, J. and Zhang, J. and Zhai, D. et al. 2017. Theoretical and Experimental Evidence for the Carbon-Oxygen Group Enhancement of NO Reduction. Environmental Science and Technology. 51 (24): pp. 14209-14216.
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Environmental Science and Technology
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WASM: Minerals, Energy and Chemical Engineering (WASM-MECE)
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Abstract

The relation between a catalytic center and the surrounding carbon-oxygen groups influences the catalytic activity in various reactions. However, the impact of this relation on catalysis is usually discussed separately. For the first time, we proved that carbon-oxygen groups increased the reducibility of Fe-C bonds toward NO reduction. Experimentally, we compared the reductive activities of materials with either one or both factors, i.e., carbon-oxygen groups and Fe-C bonds. As a result, graphene oxide-supported Fe (with both factors) showed the best activity, duration of activity, and selectivity. This material reduced 100% of NO to N2at 300 °C. Moreover, theoretical calculations revealed that the adsorption energy of graphene for NO increased from -13.51 (physical adsorption) to -327.88 kJ/mol (chemical adsorption) after modification with Fe-C. When the graphene-supported Fe was further modified with carboxylic acid groups, the ability to transfer charge increased dramatically from 0.109 to 0.180 |e-|. Therefore, the carbon-oxygen groups increased the reducibility of Fe-C. The main results will contribute to the understanding of NO reduction and the design of effective catalysts.