Oxygen Vacancy-rich Porous Co3O4 Nanosheets toward Boosted NO Reduction by CO and CO Oxidation: Insights into the Structure-Activity Relationship and Performance Enhancement Mechanism

Copyright © 2019 American Chemical Society. Oxygen vacancy-rich porous Co3O4 nanosheets (OV-Co3O4) with diverse surface oxygen vacancy contents were synthesized via facile surface reduction and applied to NO reduction by CO and CO oxidation. The structure-activity relationship between surface ox...

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Main Authors: Wang, X., Li, Xinyong, Mu, J., Fan, S., Chen, X., Wang, L., Yin, Z., Tade, Moses, Liu, Shaomin
Format: Journal Article
Language:English
Published: AMER CHEMICAL SOC 2019
Subjects:
Online Access:http://hdl.handle.net/20.500.11937/79347
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author Wang, X.
Li, Xinyong
Mu, J.
Fan, S.
Chen, X.
Wang, L.
Yin, Z.
Tade, Moses
Liu, Shaomin
author_facet Wang, X.
Li, Xinyong
Mu, J.
Fan, S.
Chen, X.
Wang, L.
Yin, Z.
Tade, Moses
Liu, Shaomin
author_sort Wang, X.
building Curtin Institutional Repository
collection Online Access
description Copyright © 2019 American Chemical Society. Oxygen vacancy-rich porous Co3O4 nanosheets (OV-Co3O4) with diverse surface oxygen vacancy contents were synthesized via facile surface reduction and applied to NO reduction by CO and CO oxidation. The structure-activity relationship between surface oxygen vacancies and catalytic performance was systematically investigated. By combining Raman, X-ray diffraction, transmission electron microscopy, X-ray photoelectron spectroscopy, and O2-temperature programmed desorption, it was found that the efficient surface reduction leads to the presence of more surface oxygen vacancies and thus distinctly enhance the surface oxygen amount and mobility of OV-Co3O4. The electron transfer towards Co sites was promoted by surface oxygen vacancies with higher content. Compared with the pristine porous Co3O4 nanosheets, the presence of more surface oxygen vacancies is beneficial for the catalytic performance enhancement for NO reduction by CO and CO oxidation. The OV-Co3O4 obtained in 0.05 mol L-1 NaBH4 solution (Co3O4-0.05) exhibited the best catalytic activity, achieving 100% NO conversion at 175 °C in NO reduction by CO and 100% CO conversion at 100 °C in CO oxidation, respectively. Co3O4-0.05 exhibited outstanding catalytic stability and resistance to high gas hour space velocity in both reactions. Combining in situ DRIFTS results, the enhanced performance of OV-Co3O4 for NO reduction by CO should be attributed to the promoted formation and transformation of dinitrosyl species and -NCO species at lower and higher temperatures. The enhanced performance of OV-Co3O4 for CO oxidation is due to the promotion of oxygen activation ability, surface oxygen mobility, as well as the enhanced CO2 desorption ability. The results indicate that the direct regulation of surface oxygen vacancies could be an efficient way to evidently enhance the catalytic performance for NO reduction by CO and CO oxidation.
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spelling curtin-20.500.11937-793472020-08-04T05:57:31Z Oxygen Vacancy-rich Porous Co3O4 Nanosheets toward Boosted NO Reduction by CO and CO Oxidation: Insights into the Structure-Activity Relationship and Performance Enhancement Mechanism Wang, X. Li, Xinyong Mu, J. Fan, S. Chen, X. Wang, L. Yin, Z. Tade, Moses Liu, Shaomin Science & Technology Technology Nanoscience & Nanotechnology Materials Science, Multidisciplinary Science & Technology - Other Topics Materials Science Co3O4 nanosheets surface oxygen vacancy facile surface reduction NO reduction by CO CO oxidation ORDERED MESOPOROUS CO3O4 CATALYTIC PERFORMANCES N2O DECOMPOSITION MANGANESE OXIDE NITRIC-OXIDE SURFACE ACTIVATION CERIA MORPHOLOGY WATER Copyright © 2019 American Chemical Society. Oxygen vacancy-rich porous Co3O4 nanosheets (OV-Co3O4) with diverse surface oxygen vacancy contents were synthesized via facile surface reduction and applied to NO reduction by CO and CO oxidation. The structure-activity relationship between surface oxygen vacancies and catalytic performance was systematically investigated. By combining Raman, X-ray diffraction, transmission electron microscopy, X-ray photoelectron spectroscopy, and O2-temperature programmed desorption, it was found that the efficient surface reduction leads to the presence of more surface oxygen vacancies and thus distinctly enhance the surface oxygen amount and mobility of OV-Co3O4. The electron transfer towards Co sites was promoted by surface oxygen vacancies with higher content. Compared with the pristine porous Co3O4 nanosheets, the presence of more surface oxygen vacancies is beneficial for the catalytic performance enhancement for NO reduction by CO and CO oxidation. The OV-Co3O4 obtained in 0.05 mol L-1 NaBH4 solution (Co3O4-0.05) exhibited the best catalytic activity, achieving 100% NO conversion at 175 °C in NO reduction by CO and 100% CO conversion at 100 °C in CO oxidation, respectively. Co3O4-0.05 exhibited outstanding catalytic stability and resistance to high gas hour space velocity in both reactions. Combining in situ DRIFTS results, the enhanced performance of OV-Co3O4 for NO reduction by CO should be attributed to the promoted formation and transformation of dinitrosyl species and -NCO species at lower and higher temperatures. The enhanced performance of OV-Co3O4 for CO oxidation is due to the promotion of oxygen activation ability, surface oxygen mobility, as well as the enhanced CO2 desorption ability. The results indicate that the direct regulation of surface oxygen vacancies could be an efficient way to evidently enhance the catalytic performance for NO reduction by CO and CO oxidation. 2019 Journal Article http://hdl.handle.net/20.500.11937/79347 10.1021/acsami.9b08664 English AMER CHEMICAL SOC restricted
spellingShingle Science & Technology
Technology
Nanoscience & Nanotechnology
Materials Science, Multidisciplinary
Science & Technology - Other Topics
Materials Science
Co3O4 nanosheets
surface oxygen vacancy
facile surface reduction
NO reduction by CO
CO oxidation
ORDERED MESOPOROUS CO3O4
CATALYTIC PERFORMANCES
N2O DECOMPOSITION
MANGANESE OXIDE
NITRIC-OXIDE
SURFACE
ACTIVATION
CERIA
MORPHOLOGY
WATER
Wang, X.
Li, Xinyong
Mu, J.
Fan, S.
Chen, X.
Wang, L.
Yin, Z.
Tade, Moses
Liu, Shaomin
Oxygen Vacancy-rich Porous Co3O4 Nanosheets toward Boosted NO Reduction by CO and CO Oxidation: Insights into the Structure-Activity Relationship and Performance Enhancement Mechanism
title Oxygen Vacancy-rich Porous Co3O4 Nanosheets toward Boosted NO Reduction by CO and CO Oxidation: Insights into the Structure-Activity Relationship and Performance Enhancement Mechanism
title_full Oxygen Vacancy-rich Porous Co3O4 Nanosheets toward Boosted NO Reduction by CO and CO Oxidation: Insights into the Structure-Activity Relationship and Performance Enhancement Mechanism
title_fullStr Oxygen Vacancy-rich Porous Co3O4 Nanosheets toward Boosted NO Reduction by CO and CO Oxidation: Insights into the Structure-Activity Relationship and Performance Enhancement Mechanism
title_full_unstemmed Oxygen Vacancy-rich Porous Co3O4 Nanosheets toward Boosted NO Reduction by CO and CO Oxidation: Insights into the Structure-Activity Relationship and Performance Enhancement Mechanism
title_short Oxygen Vacancy-rich Porous Co3O4 Nanosheets toward Boosted NO Reduction by CO and CO Oxidation: Insights into the Structure-Activity Relationship and Performance Enhancement Mechanism
title_sort oxygen vacancy-rich porous co3o4 nanosheets toward boosted no reduction by co and co oxidation: insights into the structure-activity relationship and performance enhancement mechanism
topic Science & Technology
Technology
Nanoscience & Nanotechnology
Materials Science, Multidisciplinary
Science & Technology - Other Topics
Materials Science
Co3O4 nanosheets
surface oxygen vacancy
facile surface reduction
NO reduction by CO
CO oxidation
ORDERED MESOPOROUS CO3O4
CATALYTIC PERFORMANCES
N2O DECOMPOSITION
MANGANESE OXIDE
NITRIC-OXIDE
SURFACE
ACTIVATION
CERIA
MORPHOLOGY
WATER
url http://hdl.handle.net/20.500.11937/79347