Synthesis of carbon nitride in potassium hydroxide molten salt for efficient uranium extraction from radioactive wastewater

doi:10.1007/s11783-024-1859-5

2024, Vol. 18

Issue (8) : 99 https://doi.org/10.1007/s11783-024-1859-5

Synthesis of carbon nitride in potassium hydroxide molten salt for efficient uranium extraction from radioactive wastewater

Shuang Liu^1,², Junhan Luo¹, Daniel-James Maguire³, Liyuan Zheng⁴, Zhe Wang¹(

), Yuexiang Lu¹(

)

¹. Institute of Nuclear and New Energy Technology, Tsinghua University, Beijing 100084, China
². Nuclear Research Institute for Future Technology and Policy, Seoul National University, Seoul 08826, Republic of Korea
³. Department of Earth Sciences, University of Cambridge, Cambridge CB23EQ, UK
⁴. The MOE Key Laboratory of Resources and Environmental System Optimization, College of Environmental Science and Engineering, North China Electric Power University, Beijing 102206, China

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Abstract

● Develop a one-step unary KOH molten salt carbon nitride synthesis method.

● Enhance light absorption and separation efficiency of electron-hole pair of K-CN-80.

● Improve photocatalytic activity and kinetics of U(VI) extraction onto K-CN-80.

● Separated U(VI) from wastewater as metastudtite by the photocatalytic extraction.

Photocatalysis-assisted removal of uranium has been proven as an effective method for the elimination of radioactive pollution from wastewater. In this work, carbon nitride materials were synthesized in potassium hydroxide (KOH) molten salt and applied to photocatalytic uranyl extraction. Obtained materials were confirmed to possess the triazine-s-heptazine structure by NMR, XPS and UV-Vis characterization, and exhibited a wider visible light absorption than graphitic carbon nitride (g-C₃N₄). The photocatalytic activity of the carbon nitride materials was tailored by varying the precursor mass fractions. The carbon nitride obtained at 80% melamine as precursor (K-CN-80) exhibited the highest photocatalytic extraction ability and its photocatalytic reaction rate is 6.6 times faster than that of g-C₃N₄. The influence of sacrificial agents was studied and the results showed that triethanolamine inhibited U(VI) photoreduction, but methanol can accelerate U(VI) photoreduction by consuming photogenerated holes. This unary KOH molten salt synthesis method has exceptional potential applications in the preparation of carbon nitrides, and the obtained products showed potential in extracting U(VI) from aqueous solutions for use in nuclear fuel industry and for U(VI) environmental pollution cleanup.

Keywords Uranium Carbon nitride Molten salt Photocatalysis Radioactive wastewater

Corresponding Author(s): Zhe Wang,Yuexiang Lu

Issue Date: 17 June 2024

Cite this article:

Shuang Liu,Junhan Luo,Daniel-James Maguire, et al. Synthesis of carbon nitride in potassium hydroxide molten salt for efficient uranium extraction from radioactive wastewater[J]. Front. Environ. Sci. Eng., 2024, 18(8): 99.

URL:

https://academic.hep.com.cn/fese/EN/10.1007/s11783-024-1859-5
https://academic.hep.com.cn/fese/EN/Y2024/V18/I8/99

Scheme1 The formation of K-CN-w from melamine and picture of the synthesized K-CN-w.

Fig.1 The photos and SEM images of (a) g-C₃N₄, (b) K-CN-70, (c) K-CN-80, and (d) K-CN-90.

Fig.2 N₂ adsorption-desorption curves of (a) g-C₃N₄, (b) K-CN-70, (c) K-CN-80, and (d) K-CN-90.

Fig.3 (a) The XRD patterns, (b) local enlarged XRD image and fitting of FWHM, (c) solid-state ¹³C NMR spectra and (d) FT-IR spectra of the synthetic g-C₃N₄, K-CN-70, K-CN-80, and K-CN-90.

Fig.4 (a) XPS survey spectra of g-C₃N₄, K-CN-70, K-CN-80, and K-CN-90; (b) high resolution C 1s of g-C₃N₄, K-CN-70, K-CN-80, and K-CN-90; (c) high resolution N 1s of g-C₃N₄, K-CN-70, K-CN-80, and K-CN-90; (d) high resolution K 2p of g-C₃N₄, K-CN-70, K-CN-80, and K-CN-90.

Tab.1 The element composition of g-C₃N₄, K-CN-70, K-CN-80, and K-CN-90

Fig.5 (a) PL spectra, (b) TR-PL fitting, (c) UV-vis absorption spectra, (d) illustration of energy level diagrams, (e) the time dependent photocurrent responses under light irradiation, (f) EIS Nyquist plots of g-C₃N₄, K-CN-70, K-CN-80, and K-CN-90.

Fig.6 (a) The photocatalytic U(VI) extraction performance using g-C₃N₄, K-CN-70, K-CN-80, and K-CN-90 as catalysts with initial uranium concentration of 200 mg/L, solid/liquid = 0.75, pH = 4.0 and (b) the calculated first-order kinetics rate constant for the photocatalytic reaction, (c) the powder XRD pattern and (d) U 4f XPS spectrum after uranium photocatalytic reaction.

Fig.7 The photocatalytic performance of K-CN-80 for the uranium extraction with different sacrificial agent compared with blank.

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