Unexpected Room-TemperatureSelective Catalytic Reductionof NO<sub><i>x</i></sub> with NH<sub>3</sub> over Metal-FreeCarbon-Based Catalysts

Catalysts operating at low temperatures are imperative for the denitrification of flue gases from various non-electric industries. Current catalysts typically exhibit significant activity for the selective catalytic reduction of NO<sub><i>x</i></sub> with NH<sub>3</sub> (NH<sub>3</sub>–SCR) at temperatures above 100 °C. Here, we observed for the first time remarkable room-temperature NH<sub>3</sub>–SCR activity on the surface of carbon-based catalysts. The oxidation of NO to NO<sub>2</sub> by surface C–O–C groups at room temperature serves as a key initial step, triggering a fast SCR reaction. The C–OH groups, as active sites, directly participate in the elementary reaction pathways of the SCR through an H migration process, significantly reducing the energy barrier of the rate-determining step to below 1 eV, thereby enabling fast SCR to occur at room temperature. The room-temperature SCR and its novel reaction mechanism reported in this study would inevitably expand the research boundaries of NO<sub><i>x</i></sub> abatement.

Publication Details

Journal
Figshare
Published
2025-03-24
DOI
https://doi.org/10.1021/acs.est.4c14482.s001
Primary Topic
Catalytic Processes in Materials Science
Type
article
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article

Unexpected Room-TemperatureSelective Catalytic Reductionof NOx with NH3 over Metal-FreeCarbon-Based Catalysts

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Catalytic Processes in Materials Science
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Unexpected Room-TemperatureSelective Catalytic Reductionof NOx with NH3 over Metal-FreeCarbon-Based Catalysts

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Abstract

Catalysts operating at low temperatures are imperative for the denitrification of flue gases from various non-electric industries. Current catalysts typically exhibit significant activity for the selective catalytic reduction of NO<sub><i>x</i></sub> with NH<sub>3</sub> (NH<sub>3</sub>–SCR) at temperatures above 100 °C. Here, we observed for the first time remarkable room-temperature NH<sub>3</sub>–SCR activity on the surface of carbon-based catalysts. The oxidation of NO to NO<sub>2</sub> by surface C–O–C groups at room temperature serves as a key initial step, triggering a fast SCR reaction. The C–OH groups, as active sites, directly participate in the elementary reaction pathways of the SCR through an H migration process, significantly reducing the energy barrier of the rate-determining step to below 1 eV, thereby enabling fast SCR to occur at room temperature. The room-temperature SCR and its novel reaction mechanism reported in this study would inevitably expand the research boundaries of NO<sub><i>x</i></sub> abatement.

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Unexpected Room-TemperatureSelective Catalytic Reductionof NO<sub><i>x</i></sub> with NH<sub>3</sub> over Metal-FreeCarbon-Based Catalysts · Figshare (2025) | TGRS Research Map | TGRS