Study on the Migration and Transformation Mechanism of Graphene Oxide in Aqueous Solutions

doi:10.6023/A19070276

Abstract

Graphene oxide (GO) is widely used in energy chemical, environmental restoration, nanomaterials, liquid phase catalysis, etc. due to its excellent physical and chemical properties. At the same time, GO is inevitably discharged into nature during the application process, and the toxicity released into the environment may lead to instability of the biological system. Therefore, this paper systematically studied several common cations (Na⁺, K⁺, Ca²⁺, Mg²⁺), anions (PO₄^3-, SO₄^2-, CO₃^2-, HCO₃^-, Cl^-) and clay minerals (montmorillonite, kaolin, bentonite, nano-alumina) on GO coagulation at different concentrations. And FTIR is used to characterize the clay minerals before and after the precipitation of GO. The experimental results show that the cations have strong GO coagulation ability, and the coagulation ability of different valence cations has a large difference. After analysis, the electrical properties of GO in aqueous solution are negative, the cation acts as a counter ion, and the coagulation behavior conforms to the Schulze-Hardy rule. The main reason for the difference in coagulation ability between isovalent cations is electronegativity and ionic hydration. The anion acts to increase the stability of GO, and the coagulation ability of the cation is more effective than the stabilization ability of the anion. The ability of sodium salts with the same valence anion to coagulate GO also differs, mainly because the hydrolysis of HCO₃^- and CO₃^2- causes a decrease in the negative charges, resulting in a decrease in the ability to stabilize GO. The clay minerals contain hydroxyl and metal-oxygen bonds that interact with GO. According to the maximum removal rate, the clay minerals have the coagulation ability:nano-alumina > kaolin > bentonite > montmorillonite. The main influencing factors are the electrical properties of clay minerals in aqueous solution. This paper is helpful to understand the coagulation behavior of GO in different water environments, and it is of great significance for the future application of graphene engineering in pollution control.

Key words: graphene oxide, coagulation, cation, anion, clay mineral

Cite this article

Shi Lei, Pang Hongwei, Wang Xiangxue, Zhang Pan, Yu Shujun. Study on the Migration and Transformation Mechanism of Graphene Oxide in Aqueous Solutions[J]. Acta Chimica Sinica, 2019, 77(11): 1177-1183.

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Fig. & Tab. 5

Figure 1. FTIR spectrum of GO

Figure 2. (A) Removal rate of GO as a function of the cation concentration. (B) Photograph illustration of the influence of cations on GO coagulation. All experiments were carried out at pH＝6±0.1, C0(GO)＝22 mg/L, and T＝298 K

Figure 3. (A) Removal rate of GO as a function of the anion concentration. (B) Photograph illustration of the influence of anions on GO coagulation. All experiments were carried out at pH＝6±0.1, C0(GO)＝22 mg/L, and T＝298 K

Figure 4. (A) Removal rate of GO as a function of the clay minerals concentration. (B) Photograph illustration of the influence of clay minerals on GO coagulation. All experiments were carried out at pH＝6±0.1, C0(GO)＝22 mg/L, and T＝298 K

Figure 5. FTIR spectrum of clay minerals before and after GO coagulation: (A) kaolin; (B) nano-Al2O3; (C) montmorillonite; (D) bentonite

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