Facile synthesis of defect-rich nitrogen and sulfur Co-doped graphene quantum dots as metal-free electrocatalyst for the oxygen reduction reaction

Tianju Fan; Guangxing Zhang; Lingfeng Jian; Imran Murtaza; Hong Meng; Yidong Liu; Yong Min

doi:10.1016/j.jallcom.2019.04.097

Facile synthesis of defect-rich nitrogen and sulfur Co-doped graphene quantum dots as metal-free electrocatalyst for the oxygen reduction reaction

Tianju Fan, Guangxing Zhang, Lingfeng Jian, Imran Murtaza, Hong Meng, Yidong Liu, Yong Min

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

82 Scopus citations

Abstract

Carbon-based metal-free nanomaterials have attracted immense and persistent attention as electrocatalysts for oxygen reduction reaction (ORR) in fuel cells, due to their high electrocatalytic activity, long-term stability and low cost. Here, a facile hydrothermal treatment in the presence of ammonium hydroxide (NH₄OH) and sodium sulfide (Na₂S), as precursors, has been developed to synthesize heteroatom-doped graphene quantum dots (GQDs). For comparison, undoped graphene quantum dots (GQDs), nitrogen doped graphene quantum dots (N-GQDs), sulfur doped graphene quantum dots (S-GQDs) and nitrogen and sulfur co-doped graphene quantum dots (N,S-GQDs) have been synthesized with the same method. The as-obtained N,S-GQDs possess a high N-doping content up to 9.36% and low S-doping content up to 0.78%, with a uniform size distribution similar to that of GQDs, N-GQDs and S-GQDs. Interestingly, the multi-types of N[sbnd]C or C[sbnd]S[sbnd]C bonding in metal free N,S-GQDs can significantly enhance the electrocatalytic activity for the oxygen reduction reaction (ORR), with the electron transfer number as good as 3.82, which verify the importance of our facile synthesis method to fabricate metal-free electrocatalysts for ORR and other electrochemical applications.

Original language	English
Pages (from-to)	844-850
Number of pages	7
Journal	Journal of Alloys and Compounds
Volume	792
DOIs	https://doi.org/10.1016/j.jallcom.2019.04.097
State	Published - 5 Jul 2019
Externally published	Yes

Bibliographical note

Publisher Copyright:
© 2019 Elsevier B.V.

Funding

The authors gratefully acknowledge financial support of Guangdong Innovative and Entrepreneurial Research Team Program (No. 2016ZT06C412 ), the International Cooperation and Exchange Program under grant between the National Natural Science Foundation of China and Pakistan Science Foundation (No. 5161101159 and PSF-NSFC-II/Eng/C-IIUI-06 ), the National Basic Research Program of China (973 Program, No. 2015CB856505 ), Shenzhen Science and Technology Research Grants ( GJHZ20160229122304608 ), and Shenzhen Maker Special Project Program ( GRCK20170424144331753 ). The authors gratefully acknowledge financial support of Guangdong Innovative and Entrepreneurial Research Team Program (No. 2016ZT06C412), the International Cooperation and Exchange Program under grant between the National Natural Science Foundation of China and Pakistan Science Foundation (No. 5161101159 and PSF-NSFC-II/Eng/C-IIUI-06), the National Basic Research Program of China (973 Program, No. 2015CB856505), Shenzhen Science and Technology Research Grants (GJHZ20160229122304608), and Shenzhen Maker Special Project Program (GRCK20170424144331753).

Funders	Funder number
Shenzhen Maker Special Project Program	GRCK20170424144331753
Shenzhen Science and Technology Research Grants	GJHZ20160229122304608
Pakistan Science Foundation
Guangdong Innovative and Entrepreneurial Research Team Program	2016ZT06C412
National Natural Science Foundation of China	PSF-NSFC-II/Eng/C-IIUI-06, 5161101159
International Cooperation and Exchange Programme
National Basic Research Program of China (973 Program)	2015CB856505

Keywords

Metal-free electrocatalyst
Nitrogen and sulfur Co-doped graphene quantum dots
Oxygen reduction reaction

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10.1016/j.jallcom.2019.04.097

Cite this

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title = "Facile synthesis of defect-rich nitrogen and sulfur Co-doped graphene quantum dots as metal-free electrocatalyst for the oxygen reduction reaction",

abstract = "Carbon-based metal-free nanomaterials have attracted immense and persistent attention as electrocatalysts for oxygen reduction reaction (ORR) in fuel cells, due to their high electrocatalytic activity, long-term stability and low cost. Here, a facile hydrothermal treatment in the presence of ammonium hydroxide (NH4OH) and sodium sulfide (Na2S), as precursors, has been developed to synthesize heteroatom-doped graphene quantum dots (GQDs). For comparison, undoped graphene quantum dots (GQDs), nitrogen doped graphene quantum dots (N-GQDs), sulfur doped graphene quantum dots (S-GQDs) and nitrogen and sulfur co-doped graphene quantum dots (N,S-GQDs) have been synthesized with the same method. The as-obtained N,S-GQDs possess a high N-doping content up to 9.36% and low S-doping content up to 0.78%, with a uniform size distribution similar to that of GQDs, N-GQDs and S-GQDs. Interestingly, the multi-types of N[sbnd]C or C[sbnd]S[sbnd]C bonding in metal free N,S-GQDs can significantly enhance the electrocatalytic activity for the oxygen reduction reaction (ORR), with the electron transfer number as good as 3.82, which verify the importance of our facile synthesis method to fabricate metal-free electrocatalysts for ORR and other electrochemical applications.",

keywords = "Metal-free electrocatalyst, Nitrogen and sulfur Co-doped graphene quantum dots, Oxygen reduction reaction",

author = "Tianju Fan and Guangxing Zhang and Lingfeng Jian and Imran Murtaza and Hong Meng and Yidong Liu and Yong Min",

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doi = "10.1016/j.jallcom.2019.04.097",

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T1 - Facile synthesis of defect-rich nitrogen and sulfur Co-doped graphene quantum dots as metal-free electrocatalyst for the oxygen reduction reaction

AU - Fan, Tianju

AU - Zhang, Guangxing

AU - Jian, Lingfeng

AU - Murtaza, Imran

AU - Meng, Hong

AU - Liu, Yidong

AU - Min, Yong

PY - 2019/7/5

Y1 - 2019/7/5

N2 - Carbon-based metal-free nanomaterials have attracted immense and persistent attention as electrocatalysts for oxygen reduction reaction (ORR) in fuel cells, due to their high electrocatalytic activity, long-term stability and low cost. Here, a facile hydrothermal treatment in the presence of ammonium hydroxide (NH4OH) and sodium sulfide (Na2S), as precursors, has been developed to synthesize heteroatom-doped graphene quantum dots (GQDs). For comparison, undoped graphene quantum dots (GQDs), nitrogen doped graphene quantum dots (N-GQDs), sulfur doped graphene quantum dots (S-GQDs) and nitrogen and sulfur co-doped graphene quantum dots (N,S-GQDs) have been synthesized with the same method. The as-obtained N,S-GQDs possess a high N-doping content up to 9.36% and low S-doping content up to 0.78%, with a uniform size distribution similar to that of GQDs, N-GQDs and S-GQDs. Interestingly, the multi-types of N[sbnd]C or C[sbnd]S[sbnd]C bonding in metal free N,S-GQDs can significantly enhance the electrocatalytic activity for the oxygen reduction reaction (ORR), with the electron transfer number as good as 3.82, which verify the importance of our facile synthesis method to fabricate metal-free electrocatalysts for ORR and other electrochemical applications.

AB - Carbon-based metal-free nanomaterials have attracted immense and persistent attention as electrocatalysts for oxygen reduction reaction (ORR) in fuel cells, due to their high electrocatalytic activity, long-term stability and low cost. Here, a facile hydrothermal treatment in the presence of ammonium hydroxide (NH4OH) and sodium sulfide (Na2S), as precursors, has been developed to synthesize heteroatom-doped graphene quantum dots (GQDs). For comparison, undoped graphene quantum dots (GQDs), nitrogen doped graphene quantum dots (N-GQDs), sulfur doped graphene quantum dots (S-GQDs) and nitrogen and sulfur co-doped graphene quantum dots (N,S-GQDs) have been synthesized with the same method. The as-obtained N,S-GQDs possess a high N-doping content up to 9.36% and low S-doping content up to 0.78%, with a uniform size distribution similar to that of GQDs, N-GQDs and S-GQDs. Interestingly, the multi-types of N[sbnd]C or C[sbnd]S[sbnd]C bonding in metal free N,S-GQDs can significantly enhance the electrocatalytic activity for the oxygen reduction reaction (ORR), with the electron transfer number as good as 3.82, which verify the importance of our facile synthesis method to fabricate metal-free electrocatalysts for ORR and other electrochemical applications.

KW - Metal-free electrocatalyst

KW - Nitrogen and sulfur Co-doped graphene quantum dots

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Facile synthesis of defect-rich nitrogen and sulfur Co-doped graphene quantum dots as metal-free electrocatalyst for the oxygen reduction reaction

Abstract

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