3D Graphene Preparation Via Covalent Amide Functionalization for Efficient Metal-free Electrocatalysis in Oxygen Reduction

Overview

Journal Sci Rep

Specialty Science

Date 2017 Feb 28

PMID 28240302

Citations 10

Authors

Mohammad Shamsuddin Ahmed

Young-Bae Kim

Affiliations

Soon will be listed here.

Abstract

3D and porous reduced graphene oxide (rGO) catalysts have been prepared with sp-hybridized 1,4-diaminobutane (sp-DABu, rGO-sp-rGO) and sp-hybridized 1,4-diaminobenzene (sp-DABe, rGO-sp-rGO) through a covalent amidation and have employed as a metal-free electrocatalyst for oxygen reduction reaction (ORR) in alkaline media. Both compounds have used as a junction between functionalized rGO layers to improve electrical conductivity and impart electrocatalytic activity to the ORR resulting from the interlayer charge transfer. The successful amidation and the subsequent reduction in the process of catalyst preparation have confirmed by X-ray photoelectron spectroscopy. A hierarchical porous structure is also confirmed by surface morphological analysis. Specific surface area and thermal stability have increased after successful the amidation by sp-DABu. The investigated ORR mechanism reveals that both functionalized rGO is better ORR active than nonfunctionalized rGO due to pyridinic-like N content and rGO-sp-rGO is better ORR active than rGO-sp-rGO due to higher pyridinic-like N content and π-electron interaction-free interlayer charge transfer. Thus, the rGO-sp-rGO has proven as an efficient metal-free electrocatalyst with better electrocatalytic activity, stability, and tolerance to the crossover effect than the commercially available Pt/C for ORR.

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References

Sanetuntikul J, Hang T, Shanmugam S . Hollow nitrogen-doped carbon spheres as efficient and durable electrocatalysts for oxygen reduction. Chem Commun (Camb). 2014; 50(67):9473-6. DOI: 10.1039/c4cc03437f. View

Kim O, Cho Y, Chung D, Kim M, Yoo J, Park J . Facile and gram-scale synthesis of metal-free catalysts: toward realistic applications for fuel cells. Sci Rep. 2015; 5:8376. PMC: 4345340. DOI: 10.1038/srep08376. View

Cote L, Kim F, Huang J . Langmuir-Blodgett assembly of graphite oxide single layers. J Am Chem Soc. 2008; 131(3):1043-9. DOI: 10.1021/ja806262m. View

Sun X, Song P, Zhang Y, Liu C, Xu W, Xing W . A class of high performance metal-free oxygen reduction electrocatalysts based on cheap carbon blacks. Sci Rep. 2013; 3:2505. PMC: 3752611. DOI: 10.1038/srep02505. View

Li X, Wang X, Zhang L, Lee S, Dai H . Chemically derived, ultrasmooth graphene nanoribbon semiconductors. Science. 2008; 319(5867):1229-32. DOI: 10.1126/science.1150878. View

Tao L, Wang Q, Dou S, Ma Z, Huo J, Wang S . Edge-rich and dopant-free graphene as a highly efficient metal-free electrocatalyst for the oxygen reduction reaction. Chem Commun (Camb). 2016; 52(13):2764-7. DOI: 10.1039/c5cc09173j. View

Wang X, Kholmanov I, Chou H, Ruoff R . Simultaneous Electrochemical Reduction and Delamination of Graphene Oxide Films. ACS Nano. 2015; 9(9):8737-43. DOI: 10.1021/acsnano.5b03814. View

Xu S, Yong L, Wu P . One-pot, green, rapid synthesis of flowerlike gold nanoparticles/reduced graphene oxide composite with regenerated silk fibroin as efficient oxygen reduction electrocatalysts. ACS Appl Mater Interfaces. 2013; 5(3):654-62. DOI: 10.1021/am302076x. View

Ahmed M, Kim D, Soon Han H, Jeong H, Jeon S . Covalent hybridization of thiolated graphene sheet and platinum nanoparticles for electrocatalytic oxygen reduction reaction. J Nanosci Nanotechnol. 2013; 12(11):8349-55. DOI: 10.1166/jnn.2012.6674. View

10.

Zhang S, Xiong P, Yang X, Wang X . Novel PEG functionalized graphene nanosheets: enhancement of dispersibility and thermal stability. Nanoscale. 2011; 3(5):2169-74. DOI: 10.1039/c0nr00923g. View

11.

Marcano D, Kosynkin D, Berlin J, Sinitskii A, Sun Z, Slesarev A . Improved synthesis of graphene oxide. ACS Nano. 2010; 4(8):4806-14. DOI: 10.1021/nn1006368. View

12.

Georgakilas V, Otyepka M, Bourlinos A, Chandra V, Kim N, Kemp K . Functionalization of graphene: covalent and non-covalent approaches, derivatives and applications. Chem Rev. 2012; 112(11):6156-214. DOI: 10.1021/cr3000412. View

13.

Wang B, Luo B, Liang M, Wang A, Wang J, Fang Y . Chemical amination of graphene oxides and their extraordinary properties in the detection of lead ions. Nanoscale. 2011; 3(12):5059-66. DOI: 10.1039/c1nr10901d. View

14.

Dai L, Xue Y, Qu L, Choi H, Baek J . Metal-free catalysts for oxygen reduction reaction. Chem Rev. 2015; 115(11):4823-92. DOI: 10.1021/cr5003563. View

15.

Park J, Jo S, Yu Y, Kim Y, Yang J, Lee W . Single-gate bandgap opening of bilayer graphene by dual molecular doping. Adv Mater. 2011; 24(3):407-11. DOI: 10.1002/adma.201103411. View

16.

Jiang W, Gu L, Li L, Zhang Y, Zhang X, Zhang L . Understanding the High Activity of Fe-N-C Electrocatalysts in Oxygen Reduction: Fe/Fe3C Nanoparticles Boost the Activity of Fe-N(x). J Am Chem Soc. 2016; 138(10):3570-8. DOI: 10.1021/jacs.6b00757. View

17.

Zhou K, Zhou W, Liu X, Wang Y, Wan J, Chen S . Nitrogen self-doped porous carbon from surplus sludge as metal-free electrocatalysts for oxygen reduction reactions. ACS Appl Mater Interfaces. 2014; 6(17):14911-8. DOI: 10.1021/am502215t. View

18.

Qi X, Pu K, Zhou X, Li H, Liu B, Boey F . Conjugated-polyelectrolyte-functionalized reduced graphene oxide with excellent solubility and stability in polar solvents. Small. 2010; 6(5):663-9. DOI: 10.1002/smll.200902221. View

19.

Ahmed M, Jeon S . The nanostructure of nitrogen atom linked carbon nanotubes with platinum employed to the electrocatalytic oxygen reduction. J Nanosci Nanotechnol. 2013; 13(1):306-14. DOI: 10.1166/jnn.2013.6851. View

20.

Gong K, Du F, Xia Z, Durstock M, Dai L . Nitrogen-doped carbon nanotube arrays with high electrocatalytic activity for oxygen reduction. Science. 2009; 323(5915):760-4. DOI: 10.1126/science.1168049. View