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

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 reducibili...

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Main Authors: Li, J., Wang, Y., Song, J., Gao, Q., Zhang, J., Zhai, D., Zhou, J., Liu, Jian, Xu, Z., Qian, G., Liu, Y.
Format: Journal Article
Published: American Chemical Society 2017
Online Access:http://hdl.handle.net/20.500.11937/71146
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author Li, J.
Wang, Y.
Song, J.
Gao, Q.
Zhang, J.
Zhang, J.
Zhai, D.
Zhou, J.
Liu, Jian
Xu, Z.
Qian, G.
Liu, Y.
author_facet Li, J.
Wang, Y.
Song, J.
Gao, Q.
Zhang, J.
Zhang, J.
Zhai, D.
Zhou, J.
Liu, Jian
Xu, Z.
Qian, G.
Liu, Y.
author_sort Li, J.
building Curtin Institutional Repository
collection Online Access
description 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.
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publishDate 2017
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spelling curtin-20.500.11937-711462019-01-31T03:21:36Z Theoretical and Experimental Evidence for the Carbon-Oxygen Group Enhancement of NO Reduction Li, J. Wang, Y. Song, J. Gao, Q. Zhang, J. Zhang, J. Zhai, D. Zhou, J. Liu, Jian Xu, Z. Qian, G. Liu, Y. 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. 2017 Journal Article http://hdl.handle.net/20.500.11937/71146 10.1021/acs.est.7b04213 American Chemical Society restricted
spellingShingle Li, J.
Wang, Y.
Song, J.
Gao, Q.
Zhang, J.
Zhang, J.
Zhai, D.
Zhou, J.
Liu, Jian
Xu, Z.
Qian, G.
Liu, Y.
Theoretical and Experimental Evidence for the Carbon-Oxygen Group Enhancement of NO Reduction
title Theoretical and Experimental Evidence for the Carbon-Oxygen Group Enhancement of NO Reduction
title_full Theoretical and Experimental Evidence for the Carbon-Oxygen Group Enhancement of NO Reduction
title_fullStr Theoretical and Experimental Evidence for the Carbon-Oxygen Group Enhancement of NO Reduction
title_full_unstemmed Theoretical and Experimental Evidence for the Carbon-Oxygen Group Enhancement of NO Reduction
title_short Theoretical and Experimental Evidence for the Carbon-Oxygen Group Enhancement of NO Reduction
title_sort theoretical and experimental evidence for the carbon-oxygen group enhancement of no reduction
url http://hdl.handle.net/20.500.11937/71146