Co78Si8B14 metallic glass: A highly efficient and ultra-sustainable Fenton-like catalyst in degrading wastewater under universal pH conditions

doi:10.1016/j.jmst.2021.10.024

Abstract

Abstract:

Overcoming the pH limitation and increasing the catalyst reusability remain pressing demands for metallic glass (MG) in wastewater remediation. Herein, Co₇₈Si₈B₁₄ MG ribbons are used to degrade dye wastewater by activating hydrogen peroxide (H₂O₂) as Fenton-like catalysts. The Co-based MG catalysts exhibit high degradation efficiency under both acidic and alkaline conditions, and the kinetic reaction rate at pH 10 (0.176 min^-1) and pH 4 (0.089 min^-1) is 5.9 and 1.2 times higher than that of the extensively studied Fe-based MG catalysts, respectively. Impressively, the Co-based MG catalysts can be reused up to 20-60 times at universal pH conditions, demonstrating fairly good reusability. The newly discovered Co-based MG catalysts do not follow the classical Fenton reactions with H₂O₂ the way Fe-based MGs do. In an acid environment, hydroxyl radicals play a dominant role in the degradation, while in an alkaline environment, the effect of hydroxyl radicals is weakened, and Co³⁺ ions exert a relatively major function on the degradation. The excellent performance in catalytic activity and reusability at universal pH conditions of the Co-based MGs will inspire the development of MGs in wastewater treatment.

Key words: Metallic glass, Wastewater degradation, Catalytic applications

Xindong Qin, Jiliang Xu, Zhengwang Zhu, Zhengkun Li, Dawei Fang, Huameng Fu, Shiming Zhang, Haifeng Zhang. Co₇₈Si₈B₁₄ metallic glass: A highly efficient and ultra-sustainable Fenton-like catalyst in degrading wastewater under universal pH conditions[J]. J. Mater. Sci. Technol., 2022, 113: 105-116.

Figures/Tables 13

Fig. 1. (a) UV-vis spectra of AO II solution treated with Co78Si8B14 MG ribbons (pH = 10, H2O2 concentration: 2.5 mmol/L, Co78Si8B14 MG dosage: 4 g/L, temperature: 298 K and AO II concentration: 100 mg/L). (b) Effect of pH on AO II degradation using the as-received Co78Si8B14 MG ribbons. (c) Degradation process of AO II using Fe78Si8B14 MG ribbons at pH 4 and pH 10, respectively (H2O2 concentration: 2.5 mmol/L, Fe78Si8B14 MG dosage: 4 g/L, temperature: 298 K and AO II concentration: 100 mg/L). (d) Degradation efficiency and degradation rate of AO II using Co78Si8B14 and Fe78Si8B14 MG ribbons, respectively.

Fig. 2. Comparison of applicable range of pH. Degradation efficiency versus solution pH for the Co-based MGs in this work and the extensively studied Fe-based MG catalysts.

Fig. 3. (a) Effect of temperature on AO II degradation using Co78Si8B14 MG ribbons, the inset shows the plot of lnk versus 1000/RT, the solid line is the fitting using the Arrhenius equation to yield Ea. (b) UV-vis spectra of Rh B solution treated with Co78Si8B14 MG ribbons (pH = 4, H2O2 concentration: 2.5 mmol/L, Co78Si8B14 dosage: 4 g/L, temperature: 298 K and Rh B concentration: 50 mg/L). (c) Effect of pH on Rh B degradation using Co78Si8B14 MG ribbons. (d) TOC removals of AO II and Rh B by using Co78Si8B14 MG ribbons under acidic and alkaline conditions.

Fig. 4. Degradation efficiency and degradation rate of AO II treated by Co78Si8B14 MGs with different reused times with (a) pH = 4 and (b) pH = 10.

Fig. 5. XRD patterns of the Co78Si8B14 MG ribbons before and after reaction with AO II solution for different cycles.

Fig. 6. SEM images of Co78Si8B14 MGs: (a) before reaction and after the (b) 1st, (c) 5th, (d) 10th, (e) 20th and (f) 25th cycles with pH = 4.

Fig. 7. SEM image of the 10th run of Co78Si8B14 MGs and corresponding elemental mapping analysis on ribbon surface with pH = 4.

Fig. 8. High-resolution XPS results of Co 2p spectra of as-received and reused glassy ribbons with pH = 4.

Fig. 9. SEM images of Co78Si8B14 MGs after the (a) 1st, (b) 5th (with inset image of the enlarged view of the pits highlighted by a red square), (c) 10th, (d) 15th, (e) 20th, (f) 30th, (g) 40th, (h) 50th and (i) 60th cycles with pH = 10.

Fig. 10. SEM image of the 20th run of Co78Si8B14 MGs and corresponding element line scanning analysis on ribbon surface with pH = 10.

Fig. 11. High-resolution XPS results of Co 2p spectra of reused glassy ribbons with pH = 10.

Fig. 12. Effect of TBA concentration on AO II degradation with (a) pH = 4 and (b) pH = 10. Effect of (c) catalyst dosage and (d) H2O2 concentration on AO II degradation using as-received Co78Si8B14 MG ribbons. Effect of Co2+ and Co3+ on AO II degradation with (e) pH = 4 (Co2+ or Co3+ concentration: 16.9 mg/L, temperature: 298 K and AO II concentration: 100 mg/L) and (f) pH = 10 (Co2+ or Co3+ concentration: 6.1 mg/L, temperature: 298 K and AO II concentration: 100 mg/L).

Fig. 13. Schematic illustration of the degradation mechanism of organic dyes using Co78Si8B14 MG ribbons in acid and alkaline conditions.

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Co₇₈Si₈B₁₄ metallic glass: A highly efficient and ultra-sustainable Fenton-like catalyst in degrading wastewater under universal pH conditions

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