Insights into nitrogen and boron-co-doped graphene toward high-performance peroxymonosulfate activation : maneuverable N-B bonding configurations and oxidation pathways

Nitrogen and boron-co-doped graphene was synthesized through two-step thermal annealing (2sNBG) which was employed as a PMS activator to degrade sulfacetamide (SAM). The concentration of the main reactive functionalities (pyridinic N and substitutional B (BC3)) as well as catalytic activity of 2sNBG...

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Main Authors: Chen, Xiao, Duan, Xiaoguang, Oh, Wen-Da, Zhang, Peng-Hui, Guan, Chao-Ting, Zhu, Yi-An, Lim, Teik Thye
Other Authors: School of Civil and Environmental Engineering
Format: Article
Language:English
Published: 2021
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Online Access:https://hdl.handle.net/10356/151364
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spelling sg-ntu-dr.10356-1513642021-07-09T02:11:44Z Insights into nitrogen and boron-co-doped graphene toward high-performance peroxymonosulfate activation : maneuverable N-B bonding configurations and oxidation pathways Chen, Xiao Duan, Xiaoguang Oh, Wen-Da Zhang, Peng-Hui Guan, Chao-Ting Zhu, Yi-An Lim, Teik Thye School of Civil and Environmental Engineering School of Chemical and Biomedical Engineering Nanyang Environment and Water Research Institute Environmental Chemistry and Materials Centre Engineering::Environmental engineering Nitrogen and Boron-co-doped Graphene Radical Pathway Nitrogen and boron-co-doped graphene was synthesized through two-step thermal annealing (2sNBG) which was employed as a PMS activator to degrade sulfacetamide (SAM). The concentration of the main reactive functionalities (pyridinic N and substitutional B (BC3)) as well as catalytic activity of 2sNBGs were delicately maneuvered through tuning the thermal annealing temperatures. The catalytic performances of the doped graphene in this study followed the order of 2sNBG800 > 2sNBG900 > 2sNBG700 > 2sNBG600 > NG600 > 1sNBGs > BG800. 30.4 at.% N of h-BN (Nh-NB/Ntotal) and 32.8 at.% B of h-BN (Bh-NB/Btotal) were detected in the 1sNBG800, which hampered the catalytic oxidation of SAM via PMS activation by 1sNBG. Among all the 2sNBGs, 2sNBG800 (2sNBG prepared at 800 °C) possessed the highest level of N (13.8 at.%) and B (16.3 at.%), the highest content of pyridinic N (73.4 at.%, Npyridinic-N/Ntotal) and BC3 (43.4 at.%, BBC3/Btotal), the lowest B-C–O (56.6 at.% BC2O, BBC2O/Btotal) content and none of h-BN. 2sNBG800 performed best to activate PMS for catalytic oxidation of SAM. Both radical quenching experiment and DFT calculation revealed that the introduction of B into NG can facilitate the transition from a non-radical oxidation dominating in the NG/PMS system to the coexistence of non-radical and radical oxidation in the 2sNBG/PMS system. The synergistic coupling effect between pyridinic N and BC3 (bonding configuration of B-C-C-C-pyridinic N) was the main reason for the enhanced catalytic activity of 2sNBG800. The transformation of the amine group and subsequent mineralization can effectively minimize the hazardous potentials of sulfonamides to the environment. The SAM degradation was negligibly influenced by NO3− in the 2sNBG800/PMS/SAM system, while Cl− and humic acid led to 33% and 64% decrease in kapp, respectively. The adsorbed intermediates mainly accounted for the deactivation of 2sNBG. This study provides an insight into the function of different N-B bonding configurations in NBG for metal-free catalytic oxidation. Ministry of Education (MOE) This research is supported by Ministry of Education, Singapore, under the Academic Research Grant RG96/16. X. D. appreciate the partial support from Open Research Projects of State Key Laboratory (SKL-ChE-16C05 and QAK201808). 2021-07-09T02:11:44Z 2021-07-09T02:11:44Z 2019 Journal Article Chen, X., Duan, X., Oh, W., Zhang, P., Guan, C., Zhu, Y. & Lim, T. T. (2019). Insights into nitrogen and boron-co-doped graphene toward high-performance peroxymonosulfate activation : maneuverable N-B bonding configurations and oxidation pathways. Applied Catalysis B: Environmental, 253, 419-432. https://dx.doi.org/10.1016/j.apcatb.2019.04.018 0926-3373 0000-0001-9129-9105 0000-0001-9635-5807 0000-0002-1848-7617 0000-0001-6226-0711 https://hdl.handle.net/10356/151364 10.1016/j.apcatb.2019.04.018 2-s2.0-85064894487 253 419 432 en RG96/16 Applied Catalysis B: Environmental © 2019 Elsevier B.V. All rights reserved.
institution Nanyang Technological University
building NTU Library
continent Asia
country Singapore
Singapore
content_provider NTU Library
collection DR-NTU
language English
topic Engineering::Environmental engineering
Nitrogen and Boron-co-doped Graphene
Radical Pathway
spellingShingle Engineering::Environmental engineering
Nitrogen and Boron-co-doped Graphene
Radical Pathway
Chen, Xiao
Duan, Xiaoguang
Oh, Wen-Da
Zhang, Peng-Hui
Guan, Chao-Ting
Zhu, Yi-An
Lim, Teik Thye
Insights into nitrogen and boron-co-doped graphene toward high-performance peroxymonosulfate activation : maneuverable N-B bonding configurations and oxidation pathways
description Nitrogen and boron-co-doped graphene was synthesized through two-step thermal annealing (2sNBG) which was employed as a PMS activator to degrade sulfacetamide (SAM). The concentration of the main reactive functionalities (pyridinic N and substitutional B (BC3)) as well as catalytic activity of 2sNBGs were delicately maneuvered through tuning the thermal annealing temperatures. The catalytic performances of the doped graphene in this study followed the order of 2sNBG800 > 2sNBG900 > 2sNBG700 > 2sNBG600 > NG600 > 1sNBGs > BG800. 30.4 at.% N of h-BN (Nh-NB/Ntotal) and 32.8 at.% B of h-BN (Bh-NB/Btotal) were detected in the 1sNBG800, which hampered the catalytic oxidation of SAM via PMS activation by 1sNBG. Among all the 2sNBGs, 2sNBG800 (2sNBG prepared at 800 °C) possessed the highest level of N (13.8 at.%) and B (16.3 at.%), the highest content of pyridinic N (73.4 at.%, Npyridinic-N/Ntotal) and BC3 (43.4 at.%, BBC3/Btotal), the lowest B-C–O (56.6 at.% BC2O, BBC2O/Btotal) content and none of h-BN. 2sNBG800 performed best to activate PMS for catalytic oxidation of SAM. Both radical quenching experiment and DFT calculation revealed that the introduction of B into NG can facilitate the transition from a non-radical oxidation dominating in the NG/PMS system to the coexistence of non-radical and radical oxidation in the 2sNBG/PMS system. The synergistic coupling effect between pyridinic N and BC3 (bonding configuration of B-C-C-C-pyridinic N) was the main reason for the enhanced catalytic activity of 2sNBG800. The transformation of the amine group and subsequent mineralization can effectively minimize the hazardous potentials of sulfonamides to the environment. The SAM degradation was negligibly influenced by NO3− in the 2sNBG800/PMS/SAM system, while Cl− and humic acid led to 33% and 64% decrease in kapp, respectively. The adsorbed intermediates mainly accounted for the deactivation of 2sNBG. This study provides an insight into the function of different N-B bonding configurations in NBG for metal-free catalytic oxidation.
author2 School of Civil and Environmental Engineering
author_facet School of Civil and Environmental Engineering
Chen, Xiao
Duan, Xiaoguang
Oh, Wen-Da
Zhang, Peng-Hui
Guan, Chao-Ting
Zhu, Yi-An
Lim, Teik Thye
format Article
author Chen, Xiao
Duan, Xiaoguang
Oh, Wen-Da
Zhang, Peng-Hui
Guan, Chao-Ting
Zhu, Yi-An
Lim, Teik Thye
author_sort Chen, Xiao
title Insights into nitrogen and boron-co-doped graphene toward high-performance peroxymonosulfate activation : maneuverable N-B bonding configurations and oxidation pathways
title_short Insights into nitrogen and boron-co-doped graphene toward high-performance peroxymonosulfate activation : maneuverable N-B bonding configurations and oxidation pathways
title_full Insights into nitrogen and boron-co-doped graphene toward high-performance peroxymonosulfate activation : maneuverable N-B bonding configurations and oxidation pathways
title_fullStr Insights into nitrogen and boron-co-doped graphene toward high-performance peroxymonosulfate activation : maneuverable N-B bonding configurations and oxidation pathways
title_full_unstemmed Insights into nitrogen and boron-co-doped graphene toward high-performance peroxymonosulfate activation : maneuverable N-B bonding configurations and oxidation pathways
title_sort insights into nitrogen and boron-co-doped graphene toward high-performance peroxymonosulfate activation : maneuverable n-b bonding configurations and oxidation pathways
publishDate 2021
url https://hdl.handle.net/10356/151364
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