Surface plasmon-enhanced photo-driven CO2 hydrogenation by hydroxy-terminated nickel nitride nanosheets

Abstract The majority of visible light-active plasmonic catalysts are often limited to Au, Ag, Cu, Al, etc., which have considerations in terms of costs, accessibility, and instability. Here, we show hydroxy-terminated nickel nitride (Ni3N) nanosheets as an alternative to these metals. The Ni3N nano...

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Main Authors: Saideep Singh, Rishi Verma, Nidhi Kaul, Jacinto Sa, Ajinkya Punjal, Shriganesh Prabhu, Vivek Polshettiwar
Format: Article
Language:English
Published: Nature Portfolio 2023-05-01
Series:Nature Communications
Online Access:https://doi.org/10.1038/s41467-023-38235-9
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author Saideep Singh
Rishi Verma
Nidhi Kaul
Jacinto Sa
Ajinkya Punjal
Shriganesh Prabhu
Vivek Polshettiwar
author_facet Saideep Singh
Rishi Verma
Nidhi Kaul
Jacinto Sa
Ajinkya Punjal
Shriganesh Prabhu
Vivek Polshettiwar
author_sort Saideep Singh
collection DOAJ
description Abstract The majority of visible light-active plasmonic catalysts are often limited to Au, Ag, Cu, Al, etc., which have considerations in terms of costs, accessibility, and instability. Here, we show hydroxy-terminated nickel nitride (Ni3N) nanosheets as an alternative to these metals. The Ni3N nanosheets catalyze CO2 hydrogenation with a high CO production rate (1212 mmol g−1 h−1) and selectivity (99%) using visible light. Reaction rate shows super-linear power law dependence on the light intensity, while quantum efficiencies increase with an increase in light intensity and reaction temperature. The transient absorption experiments reveal that the hydroxyl groups increase the number of hot electrons available for photocatalysis. The in situ diffuse reflectance infrared Fourier transform spectroscopy shows that the CO2 hydrogenation proceeds via the direct dissociation pathway. The excellent photocatalytic performance of these Ni3N nanosheets (without co-catalysts or sacrificial agents) is suggestive of the use of metal nitrides instead of conventional plasmonic metal nanoparticles.
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spelling doaj.art-a02e0232be3c43b8a7b29e906986d3342023-05-07T11:17:08ZengNature PortfolioNature Communications2041-17232023-05-0114111810.1038/s41467-023-38235-9Surface plasmon-enhanced photo-driven CO2 hydrogenation by hydroxy-terminated nickel nitride nanosheetsSaideep Singh0Rishi Verma1Nidhi Kaul2Jacinto Sa3Ajinkya Punjal4Shriganesh Prabhu5Vivek Polshettiwar6Department of Chemical Sciences, Tata Institute of Fundamental ResearchDepartment of Chemical Sciences, Tata Institute of Fundamental ResearchDepartment of Chemistry-Ångström Laboratory, Uppsala UniversityDepartment of Chemistry-Ångström Laboratory, Uppsala UniversityDepartment of Condensed Matter Physics and Materials Science, Tata Institute of Fundamental ResearchDepartment of Condensed Matter Physics and Materials Science, Tata Institute of Fundamental ResearchDepartment of Chemical Sciences, Tata Institute of Fundamental ResearchAbstract The majority of visible light-active plasmonic catalysts are often limited to Au, Ag, Cu, Al, etc., which have considerations in terms of costs, accessibility, and instability. Here, we show hydroxy-terminated nickel nitride (Ni3N) nanosheets as an alternative to these metals. The Ni3N nanosheets catalyze CO2 hydrogenation with a high CO production rate (1212 mmol g−1 h−1) and selectivity (99%) using visible light. Reaction rate shows super-linear power law dependence on the light intensity, while quantum efficiencies increase with an increase in light intensity and reaction temperature. The transient absorption experiments reveal that the hydroxyl groups increase the number of hot electrons available for photocatalysis. The in situ diffuse reflectance infrared Fourier transform spectroscopy shows that the CO2 hydrogenation proceeds via the direct dissociation pathway. The excellent photocatalytic performance of these Ni3N nanosheets (without co-catalysts or sacrificial agents) is suggestive of the use of metal nitrides instead of conventional plasmonic metal nanoparticles.https://doi.org/10.1038/s41467-023-38235-9
spellingShingle Saideep Singh
Rishi Verma
Nidhi Kaul
Jacinto Sa
Ajinkya Punjal
Shriganesh Prabhu
Vivek Polshettiwar
Surface plasmon-enhanced photo-driven CO2 hydrogenation by hydroxy-terminated nickel nitride nanosheets
Nature Communications
title Surface plasmon-enhanced photo-driven CO2 hydrogenation by hydroxy-terminated nickel nitride nanosheets
title_full Surface plasmon-enhanced photo-driven CO2 hydrogenation by hydroxy-terminated nickel nitride nanosheets
title_fullStr Surface plasmon-enhanced photo-driven CO2 hydrogenation by hydroxy-terminated nickel nitride nanosheets
title_full_unstemmed Surface plasmon-enhanced photo-driven CO2 hydrogenation by hydroxy-terminated nickel nitride nanosheets
title_short Surface plasmon-enhanced photo-driven CO2 hydrogenation by hydroxy-terminated nickel nitride nanosheets
title_sort surface plasmon enhanced photo driven co2 hydrogenation by hydroxy terminated nickel nitride nanosheets
url https://doi.org/10.1038/s41467-023-38235-9
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