Changes of Structure and Functional Group of Reduction of Graphene Oxide with p-Phenylene Diamine†

doi:10.7503/cjcu20150682

Abstract

Abstract:

The p-phenylene diamine(PPD) were selected as reducion and modification agent to prepare functionalized and reduced graphene(GOP-X) by one-step simple refluxing method. Infrared spectrum(FTIR), X-ray photoelectron spectroscopy(XPS), X-ray diffraction(XRD) and UV-Vis absorption spectrum were used to investigate the reaction types and structure changes between PPD and graphene oxide(GO). The results show that the d-spacing of GOP-X layers increases firstly and then decreases with the increase of X(the mass ratio of PPD and GO), and the conjugated structure gradually restored; when the solvent molecular interaction, the amplification of the d-spacing decrease to a steady figure. Three types of bonds between PPD and GO were proposed: (Ⅰ) hydrogen-bonding interaction between the oxygen-containing functional groups of GO and the PPD molecules(C—OH…H₂N—X); (Ⅱ) ionic bonding in protonating amine by the weakly acidic sites of the GO layers(—COO^- $H 3 +$ N—X); (Ⅲ) covalent bonding from amidation and nucleophilic addition reactions between the amie in PPD(NH₂) and the oxygen containing groups of GO. Furthermore, the NH₂ prefers to react first with the carboxyl group(COOH) and then with the epoxide group(C—O—C), and the relative action mechanisms were also described.

Key words: p-Phenylene diamine, Functionalization and reduction of grapheme, Protonation, d-Spacing, Reaction sequence

CLC Number:

O641
O613.71

TrendMD:

ZHAO Xiaolong, SUN Hongjuan, PENG Tongjiang. Changes of Structure and Functional Group of Reduction of Graphene Oxide with p-Phenylene Diamine^†[J]. Chem. J. Chinese Universities, 2016, 37(4): 728.

Figures/Tables 8

Fig.1 FTIR spectra of membranesa. GO; b. GOP-2; c. GOP-4; d. GOP-6; e. GOP-8.

Fig.2 XPS(A) and N1s spectra(B) of the samples a. GO; b. GOPJ-2; c. GOPJ-4; d. GOPJ-6; e. GOPJ-8.

Fig.3 C1s spectra of GO(A), GOPJ-2(B), GOPJ-4(C) and GOPJ-6(D)

Fig.4 XRD patterns of membrane presoaked in 90% EtOH-H2O(A) Dry state; (B) wet state. a. GO; b. GOP-2; c. GOP-4; d. GOP-6; e. GOP-8.

Fig.5 Change in d-spacing for GO and GOP-X membranes in dry(a) and wet(b) state(A) and schematic of d-spacing change(B)

Fig.6 SEM images of GO(A), GOP-2(B), GOP-4(C) and GOP-6(D)

Fig.7 UV-Vis absorption of membranesa. GO; b. GOP-2; c. GOP-4; d. GOP-6; e. GOP-8.

Fig.8 Process of the functionalization and reduction of grahene preparation with PPD(A) and schematic representation of covalent interaction(B)

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