Unzipping carbon nanotubes to nanoribbons for revealing the mechanism of nonradical oxidation by carbocatalysis

Qi Yang; Yidi Chen; Xiaoguang Duan; Shanke Zhou; Yue Niu; Hongqi Sun; Linjie Zhi; Shaobin Wang

doi:10.1016/j.apcatb.2020.119146

Unzipping carbon nanotubes to nanoribbons for revealing the mechanism of nonradical oxidation by carbocatalysis

Qi Yang, Yidi Chen, Xiaoguang Duan, Shanke Zhou, Yue Niu, Hongqi Sun, Linjie Zhi, Shaobin Wang

Research output: Contribution to journal › Article › peer-review

144 Citations (Scopus)

Abstract

Graphitic multi-walled carbon nanotubes (MWCNTs) are controllably unzipped into edge-rich graphene nanoribbons to reveal the roles of edges and defects in persulfate activation for bisphenol A (BPA) oxidation. Enriched carbon edges remarkably enhance the catalytic performance and can serve as hosting sites for heteroatom (N, S) doping to promote carbocatalysis. A sample (NS-2) presented a complete BPA removal in 20 min at a rate constant of 0.182 min^-1. The rate constants were relating to the defect speciation in a negative correlation to an indicator (I_D/I_D’) from Raman spectra. Excessive edges induce defects and structure transformation of sp² to sp³, resulting in deterioration of the organic oxidation. Furthermore, unzipped MWCNTs were clarified to follow a nonradical electron transfer pathway by radical screening tests, in situ Raman and electrochemical characterizations. The unveiled mechanism emphasizes the importance of an essential graphitic degree and conductivity in the edge-enriched carbocatalysts for better catalytic performance.

Original language	English
Article number	119146
Journal	Applied Catalysis B: Environmental
Volume	276
DOIs	https://doi.org/10.1016/j.apcatb.2020.119146
Publication status	Published - 5 Nov 2020
Externally published	Yes

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@article{e42af056be0641869dde7f2d31f84ff0,

title = "Unzipping carbon nanotubes to nanoribbons for revealing the mechanism of nonradical oxidation by carbocatalysis",

abstract = "Graphitic multi-walled carbon nanotubes (MWCNTs) are controllably unzipped into edge-rich graphene nanoribbons to reveal the roles of edges and defects in persulfate activation for bisphenol A (BPA) oxidation. Enriched carbon edges remarkably enhance the catalytic performance and can serve as hosting sites for heteroatom (N, S) doping to promote carbocatalysis. A sample (NS-2) presented a complete BPA removal in 20 min at a rate constant of 0.182 min-1. The rate constants were relating to the defect speciation in a negative correlation to an indicator (ID/ID{\textquoteright}) from Raman spectra. Excessive edges induce defects and structure transformation of sp2 to sp3, resulting in deterioration of the organic oxidation. Furthermore, unzipped MWCNTs were clarified to follow a nonradical electron transfer pathway by radical screening tests, in situ Raman and electrochemical characterizations. The unveiled mechanism emphasizes the importance of an essential graphitic degree and conductivity in the edge-enriched carbocatalysts for better catalytic performance.",

keywords = "carbocatalysis, Carbon edge, defect, nonradical pathway, persulfate activation",

author = "Qi Yang and Yidi Chen and Xiaoguang Duan and Shanke Zhou and Yue Niu and Hongqi Sun and Linjie Zhi and Shaobin Wang",

note = "Funding Information: The authors acknowledge the financial support from the National Natural Science Foundation of China (Grant No. 51425302 , 51702062 ) and the Chinese Academy of Sciences . X.D., H.S. and S.W. also appreciate the partial support from the Australian Research Council ( DP190103548 ). Publisher Copyright: {\textcopyright} 2020 Elsevier B.V.",

year = "2020",

month = nov,

day = "5",

doi = "10.1016/j.apcatb.2020.119146",

language = "English",

volume = "276",

journal = "Applied Catalysis B: Environmental",

issn = "0926-3373",

publisher = "Elsevier",

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T1 - Unzipping carbon nanotubes to nanoribbons for revealing the mechanism of nonradical oxidation by carbocatalysis

AU - Yang, Qi

AU - Chen, Yidi

AU - Duan, Xiaoguang

AU - Zhou, Shanke

AU - Niu, Yue

AU - Sun, Hongqi

AU - Zhi, Linjie

AU - Wang, Shaobin

N1 - Funding Information: The authors acknowledge the financial support from the National Natural Science Foundation of China (Grant No. 51425302 , 51702062 ) and the Chinese Academy of Sciences . X.D., H.S. and S.W. also appreciate the partial support from the Australian Research Council ( DP190103548 ). Publisher Copyright: © 2020 Elsevier B.V.

PY - 2020/11/5

Y1 - 2020/11/5

N2 - Graphitic multi-walled carbon nanotubes (MWCNTs) are controllably unzipped into edge-rich graphene nanoribbons to reveal the roles of edges and defects in persulfate activation for bisphenol A (BPA) oxidation. Enriched carbon edges remarkably enhance the catalytic performance and can serve as hosting sites for heteroatom (N, S) doping to promote carbocatalysis. A sample (NS-2) presented a complete BPA removal in 20 min at a rate constant of 0.182 min-1. The rate constants were relating to the defect speciation in a negative correlation to an indicator (ID/ID’) from Raman spectra. Excessive edges induce defects and structure transformation of sp2 to sp3, resulting in deterioration of the organic oxidation. Furthermore, unzipped MWCNTs were clarified to follow a nonradical electron transfer pathway by radical screening tests, in situ Raman and electrochemical characterizations. The unveiled mechanism emphasizes the importance of an essential graphitic degree and conductivity in the edge-enriched carbocatalysts for better catalytic performance.

AB - Graphitic multi-walled carbon nanotubes (MWCNTs) are controllably unzipped into edge-rich graphene nanoribbons to reveal the roles of edges and defects in persulfate activation for bisphenol A (BPA) oxidation. Enriched carbon edges remarkably enhance the catalytic performance and can serve as hosting sites for heteroatom (N, S) doping to promote carbocatalysis. A sample (NS-2) presented a complete BPA removal in 20 min at a rate constant of 0.182 min-1. The rate constants were relating to the defect speciation in a negative correlation to an indicator (ID/ID’) from Raman spectra. Excessive edges induce defects and structure transformation of sp2 to sp3, resulting in deterioration of the organic oxidation. Furthermore, unzipped MWCNTs were clarified to follow a nonradical electron transfer pathway by radical screening tests, in situ Raman and electrochemical characterizations. The unveiled mechanism emphasizes the importance of an essential graphitic degree and conductivity in the edge-enriched carbocatalysts for better catalytic performance.

KW - carbocatalysis

KW - Carbon edge

KW - defect

KW - nonradical pathway

KW - persulfate activation

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JO - Applied Catalysis B: Environmental

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Unzipping carbon nanotubes to nanoribbons for revealing the mechanism of nonradical oxidation by carbocatalysis

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