Cuprous oxide/copper oxide interpenetrated into ordered mesoporous cellulose-based carbon aerogels for efficient photocatalytic degradation of methylene blue

doi:10.1007/s11705-023-2305-0

Front. Chem. Sci. Eng.

2023, Vol. 17

Issue (7) : 918-929 https://doi.org/10.1007/s11705-023-2305-0

RESEARCH ARTICLE

Cuprous oxide/copper oxide interpenetrated into ordered mesoporous cellulose-based carbon aerogels for efficient photocatalytic degradation of methylene blue

Rui Cui, Dongnv Jin, Gaojie Jiao, Zhendong Liu, Jiliang Ma(

), Runcang Sun(

)

Liaoning Key Lab of Lignocellulose Chemistry and Biomaterials, Liaoning Collaborative Innovation Center for Lignocellulosic Biorefinery, College of Light Industry and Chemical Engineering, Dalian Polytechnic University, Dalian 116034, China

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Abstract

The casual discharge of dyes from industrial settings has seriously polluted global water systems. Owing to the abundance of biomass resources, preparing photocatalysts for photocatalytic degradation of dyes is significant; however, it still remains challenging. In this work, a cuprous oxide/copper oxide composite was interpenetrated onto carbon nanosheets of cellulose-based flexible carbon aerogels (Cu₂O/CuO@CA_x) via a simple freeze-drying-calcination method. The introduction of the carbon aerogel effectively prevents the aggregation of the cuprous oxide/copper oxide composite. In addition, Cu₂O/CuO@CA_0.2 has a larger specific surface area, stronger charge transfer capacity, and lower recombination rate of photogenerated carriers than copper oxide. Moreover, Cu₂O/CuO@CA_0.2 exhibited high photocatalytic activity in decomposing methylene blue, with a degradation rate reaching up to 99.09% in 60 min. The active oxidation species in the photocatalytic degradation process were systematically investigated by electron spin resonance characterization and poisoning experiments, among which singlet oxygen played a major role. In conclusion, this work provides an effective method for preparing photocatalysts using biomass resources in combination with different metal oxides. It also promotes the development of photocatalytic degradation of dyes.

Keywords carbon aerogel photocatalysis dye degradation biomass cuprous oxide/copper oxide

Corresponding Author(s): Jiliang Ma,Runcang Sun

About author:

^* These authors contributed equally to this work.

Online First Date: 17 May 2023 Issue Date: 05 July 2023

Cite this article:

Rui Cui,Dongnv Jin,Gaojie Jiao, et al. Cuprous oxide/copper oxide interpenetrated into ordered mesoporous cellulose-based carbon aerogels for efficient photocatalytic degradation of methylene blue[J]. Front. Chem. Sci. Eng., 2023, 17(7): 918-929.

URL:

https://academic.hep.com.cn/fcse/EN/10.1007/s11705-023-2305-0
https://academic.hep.com.cn/fcse/EN/Y2023/V17/I7/918

Fig.1 (a) Schematic of Cu₂O/CuO@CA_x preparation. (b–e) Scanning electron microscopy images of Cu₂O/CuO@CA_0.2. Elemental mapping images of Cu₂O/CuO@CA_0.2: (f) C, (g) N, (h) O and (i) Cu. (j) Energy-dispersive X-ray spectroscopy of Cu₂O/CuO@CA_0.2.

Fig.2 (a) N₂ adsorption?desorption isotherms and (b) Barret?Joyner?Halenda pore size distributions of copper oxide (CuO) and Cu₂O/CuO@CA_0.2; (c) Fourier transform infrared (FTIR) spectra of CuO and Cu₂O/CuO@CA_0.2 and (d) its local zoom of FTIR spectrum for Cu₂O/CuO@CA_0.2.

Fig.3 (a) X-ray diffraction patterns of copper oxide and Cu₂O/CuO@CA_0.2; X-ray photoelectron spectroscopy (XPS) spectra of Cu₂O/CuO@CA_0.2: (b) XPS survey spectrum, (c) C 1s, (d) N 1s, (e) O 1s and (f) Cu 2p.

Fig.4 Mott?Schottky plots of (a) copper oxide (CuO) and (b) Cu₂O/CuO@CA_0.2; (c, d) ultraviolet photoelectron spectroscopy of CuO and Cu₂O/CuO@CA_0.2; (e) periodic ON/OFF photocurrent response of CuO and Cu₂O/CuO@CA_0.2 in 0.1 mol·L^?1 Na₂SO₄ electrolyte under visible light irradiation (λ > 420 nm) at 0.5 V vs. Ag/AgCl electrode; (f) electrochemical impedance spectroscopy Nyquist plots in the visible light illumination of CuO and Cu₂O/CuO@CA_0.2.

Fig.5 The effects of (a) pH and (b) catalyst dosage on the photocatalytic degradation of methylene blue using Cu₂O/CuO@CA_0.2; the effect of (c) reaction time on the photocatalytic degradation of methylene blue using Cu₂O/CuO@CA_x; photocatalytic degradation kinetics of methylene blue using (d, g) Cu₂O/CuO@CA_0.1, (e, h) Cu₂O/CuO@CA_0.2 and (f, i) Cu₂O/CuO@CA_0.3.

Fig.6 2,2,6,6-Tetramethylpiperidine-N-oxide electron spin resonance (ESR) spin labeling for (a) electrons and (b) holes, 5,5-dimethyl-1-pyrroline-N-oxide ESR spin trapping for (c) superoxide radical and (d) hydroxyl radical as well as 2,2,6,6-tetramethyl-4-piperidone-1-yloxy ESR spin labeling for (e) singlet oxygen (control: under the dark conditions or irradiation without samples); (f) the effect of different active oxidation species on methylene blue’s degradation.

Fig.7 The possible photocatalytic mechanism for degradation of methylene blue using Cu₂O/CuO@CA_0.2.

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