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Environ Sci Technol. 2017 Dec 19;51(24):14209-14216. doi: 10.1021/acs.est.7b04213. Epub 2017 Dec 1.

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

Author information

1
SHU Center of Green Urban Mining & Industry Ecology, School of Environmental and Chemical Engineering, Shanghai University , No. 333 Nanchen Road, Shanghai 200444, P. R. China.
2
Shanghai Institute of Materials Genome , Shanghai, No. 99 Shangda Road, Shanghai 200444, P. R. China.
3
ARC Centre of Excellence for Functional Nanomaterials, Australian Institute for Bioengineering and Nanotechnology, the University of Queensland , Brisbane, Queensland 4072, Australia.

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 N2 at 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.

PMID:
29156130
DOI:
10.1021/acs.est.7b04213
[Indexed for MEDLINE]

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