Enhanced Catalytic Hydrogen Peroxide Production from Hydroxylamine Oxidation on Modified Activated Carbon Fibers: The Role of Surface Chemistry

Herein, direct production of hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) through hydroxylamine (NH<sub>2</sub>OH) oxidation by molecular oxygen was greatly enhanced over modified activated carbon fiber (ACF) catalysts. We revealed that the higher content of pyr...

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Main Authors: Wei Song, Ran Zhao, Lin Yu, Xiaowei Xie, Ming Sun, Yongfeng Li
Format: Article
Language:English
Published: MDPI AG 2021-12-01
Series:Catalysts
Subjects:
Online Access:https://www.mdpi.com/2073-4344/11/12/1515
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author Wei Song
Ran Zhao
Lin Yu
Xiaowei Xie
Ming Sun
Yongfeng Li
author_facet Wei Song
Ran Zhao
Lin Yu
Xiaowei Xie
Ming Sun
Yongfeng Li
author_sort Wei Song
collection DOAJ
description Herein, direct production of hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) through hydroxylamine (NH<sub>2</sub>OH) oxidation by molecular oxygen was greatly enhanced over modified activated carbon fiber (ACF) catalysts. We revealed that the higher content of pyrrolic/pyridone nitrogen (N5) and carboxyl-anhydride oxygen could effectively promote the higher selectivity and yield of H<sub>2</sub>O<sub>2</sub>. By changing the volume ratio of the concentrated H<sub>2</sub>SO<sub>4</sub> and HNO<sub>3</sub>, the content of N5 and surface oxygen containing groups on ACF were selectively tuned. The ACF catalyst with the highest N5 content and abundant carboxyl-anhydride oxygen containing groups was demonstrated to have the highest activity toward catalytic H<sub>2</sub>O<sub>2</sub> production, enabling the selectivity of H<sub>2</sub>O<sub>2</sub> over 99.3% and the concentration of H<sub>2</sub>O<sub>2</sub> reaching 123 mmol/L. The crucial effects of nitrogen species were expounded by the correlation of the selectivity of H<sub>2</sub>O<sub>2</sub> with the content of N5 from X-ray photoelectron spectroscopy (XPS). The possible reaction pathway over ACF catalysts promoted by N5 was also shown.
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spelling doaj.art-b016a54a4b8a412b8515b99c31ea54a72023-11-23T07:34:45ZengMDPI AGCatalysts2073-43442021-12-011112151510.3390/catal11121515Enhanced Catalytic Hydrogen Peroxide Production from Hydroxylamine Oxidation on Modified Activated Carbon Fibers: The Role of Surface ChemistryWei Song0Ran Zhao1Lin Yu2Xiaowei Xie3Ming Sun4Yongfeng Li5School of Chemical Engineering and Light Industry, Guangdong University of Technology, Guangzhou Higher Education Mega Centre, Guangzhou 510006, ChinaSchool of Chemical Engineering and Light Industry, Guangdong University of Technology, Guangzhou Higher Education Mega Centre, Guangzhou 510006, ChinaSchool of Chemical Engineering and Light Industry, Guangdong University of Technology, Guangzhou Higher Education Mega Centre, Guangzhou 510006, ChinaSchool of Chemical Engineering and Light Industry, Guangdong University of Technology, Guangzhou Higher Education Mega Centre, Guangzhou 510006, ChinaSchool of Chemical Engineering and Light Industry, Guangdong University of Technology, Guangzhou Higher Education Mega Centre, Guangzhou 510006, ChinaSchool of Chemical Engineering and Light Industry, Guangdong University of Technology, Guangzhou Higher Education Mega Centre, Guangzhou 510006, ChinaHerein, direct production of hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) through hydroxylamine (NH<sub>2</sub>OH) oxidation by molecular oxygen was greatly enhanced over modified activated carbon fiber (ACF) catalysts. We revealed that the higher content of pyrrolic/pyridone nitrogen (N5) and carboxyl-anhydride oxygen could effectively promote the higher selectivity and yield of H<sub>2</sub>O<sub>2</sub>. By changing the volume ratio of the concentrated H<sub>2</sub>SO<sub>4</sub> and HNO<sub>3</sub>, the content of N5 and surface oxygen containing groups on ACF were selectively tuned. The ACF catalyst with the highest N5 content and abundant carboxyl-anhydride oxygen containing groups was demonstrated to have the highest activity toward catalytic H<sub>2</sub>O<sub>2</sub> production, enabling the selectivity of H<sub>2</sub>O<sub>2</sub> over 99.3% and the concentration of H<sub>2</sub>O<sub>2</sub> reaching 123 mmol/L. The crucial effects of nitrogen species were expounded by the correlation of the selectivity of H<sub>2</sub>O<sub>2</sub> with the content of N5 from X-ray photoelectron spectroscopy (XPS). The possible reaction pathway over ACF catalysts promoted by N5 was also shown.https://www.mdpi.com/2073-4344/11/12/1515activated carbon fibersurface modificationhydrogen peroxidehydroxylaminepyrrolic/pyridone nitrogen
spellingShingle Wei Song
Ran Zhao
Lin Yu
Xiaowei Xie
Ming Sun
Yongfeng Li
Enhanced Catalytic Hydrogen Peroxide Production from Hydroxylamine Oxidation on Modified Activated Carbon Fibers: The Role of Surface Chemistry
Catalysts
activated carbon fiber
surface modification
hydrogen peroxide
hydroxylamine
pyrrolic/pyridone nitrogen
title Enhanced Catalytic Hydrogen Peroxide Production from Hydroxylamine Oxidation on Modified Activated Carbon Fibers: The Role of Surface Chemistry
title_full Enhanced Catalytic Hydrogen Peroxide Production from Hydroxylamine Oxidation on Modified Activated Carbon Fibers: The Role of Surface Chemistry
title_fullStr Enhanced Catalytic Hydrogen Peroxide Production from Hydroxylamine Oxidation on Modified Activated Carbon Fibers: The Role of Surface Chemistry
title_full_unstemmed Enhanced Catalytic Hydrogen Peroxide Production from Hydroxylamine Oxidation on Modified Activated Carbon Fibers: The Role of Surface Chemistry
title_short Enhanced Catalytic Hydrogen Peroxide Production from Hydroxylamine Oxidation on Modified Activated Carbon Fibers: The Role of Surface Chemistry
title_sort enhanced catalytic hydrogen peroxide production from hydroxylamine oxidation on modified activated carbon fibers the role of surface chemistry
topic activated carbon fiber
surface modification
hydrogen peroxide
hydroxylamine
pyrrolic/pyridone nitrogen
url https://www.mdpi.com/2073-4344/11/12/1515
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AT yongfengli enhancedcatalytichydrogenperoxideproductionfromhydroxylamineoxidationonmodifiedactivatedcarbonfiberstheroleofsurfacechemistry