| Citation: |
SHAO Xiongbin, XIE Shuibo, MAI Yingqing, et al. Performance and mechanism of biochar loaded magnetic nanocarbon hydroxyapatite(CHAP-γ-Fe2O3/BC) for the removal of U(Ⅵ) from water[J]. Acta Materiae Compositae Sinica, 2024, 41(11): 6170-6182. DOI: 10.13801/j.cnki.fhclxb.20240201.001
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To address the efficiency of removing U(Ⅵ) from water using functional materials and the susceptibility of nanoparticles to agglomeration, biochar-loaded magnetic nanocarbon hydroxyapatite (CHAP-γ-Fe2O3/BC) composites were prepared by dynamic oil-heating and impregnation methods using corn stover, egg shells, and magnetic γ-Fe2O, and the experiments were carried out to investigate the performances and used for the removal of U(Ⅵ) from water. When the initial concentration of U(Ⅵ) is 5 mg/L, the dosage of CHAP-γ-Fe2O3/BC is 0.1 g/L, the pH value is 6, the temperature is 30℃, and the reaction time is 1 h, the experimental results show that the maximum adsorption capacity of CHAP-γ-Fe2O3/BC for U(Ⅵ) reaches 324.4 mg/g, and the removal rate reaches 95.93%. The proposed secondary kinetic model and Langmuir model could fit the adsorption process of CHAP-γ-Fe2O3/BC on U(Ⅵ) better, indicating that the monomolecular layer chemisorption is dominated. The materials are realized to attenuate the agglomeration by surface modification technique. The composite material shows good separation recovery and recyclability in the magnetic field. The characterization results of FTIR and XPS prove that the removal mechanism of uranium by this material mainly includes ion exchange, dissolution-precipitation chemisorption and surface complexation.
The easy agglomeration of carbon hydroxyapatite (CHAP) nanoparticles under the action of van der Waals forces and the insufficiency of biochar (BC)'s own functional groups severely restricted their respective removal performance of uranium-containing wastewater, and the two composites complemented each other's strengths through the surface modification technology, compensated for the shortcomings of both sides, and realized the efficient removal of uranium-containing wastewater. Meanwhile, the introduction of superparamagnetic γ-FeO enabled the composites to realize efficient separation recovery and recycling in the magnetic field. In addition, the use of common wastes as raw materials also realized the purpose of "green environmental protection" and "waste to cure pollution". Finally, in ordered to verify the efficiency of the functional materials in removing U(VI) from water and the recycling and reuse performance, the performance and mechanism of the materials before and after modification were investigated by characterization techniques.
Biochar-loaded magnetic nanocarbon hydroxyapatite (CHAP-γ-FeO/BC) composites were prepared by dynamic oil-heating and impregnation methods using corn stover, eggshells, and magnetic γ-FeO. Characterization and analysis techniques such as SEM-EDS, XRD, BET, VSM and FTIR were used to analyze the surface and internal micro-morphology, crystal structure, specific surface area and pore size distribution, magnetic saturation intensity and functional groups of the materials before and after modification, respectively. Batch static adsorption experiments were carried out to investigate the effects of pH, temperature, adsorbent material dosage, interfering ions, reaction time and different initial U(Ⅵ) concentrations on the removal of U(Ⅵ) from water. The cyclic regeneration performance of the adsorbent materials was investigated by adsorption-desorption experiments. Based on the results of adsorption experiments and characterization analyses, the separation, recovery and recycling performance of the adsorbent materials, as well as the main mechanism of removing U(Ⅵ) from water were investigated.
(1) SEM-EDS, XRD, BET, VSM and FTIR characterization and analysis results show that: nano-CHAP is uniformly filled between the BC layered porous structure after loading, the surface modification technique is successful, and BC as a support material achieves the purpose of attenuating the self-agglomeration of nano-CHAP particles; CO is successfully introduced, and the HAP aberration is transformed into a low-crystallinity CHAP; the CHAP- γ-FeO/BC possesses high specific surface area and rich and uniform mesoporous structure; there are abundant oxygen-containing functional groups on the surface of CHAP-γ-FeO/BC with sufficient active binding sites; CHAP-γ-FeO/BC possesses a magnetic saturation strength of 0.8 emu/g. (2) The results of batch static adsorption experiments show that when the mass ratio of CHAP, γ-Fe2O3 and biomass is 1:0.54:1, the initial U(Ⅵ) concentration is 5 mg/L, the dosage of CHAP-γ-FeO/BC is 0.1 g/L, the pH value is 6, the temperature is 30 °, and the reaction time is 1 h, the maximum adsorption capacity of U(Ⅵ) of CHAP-γ-FeO/BC reaches 324.4%. The maximum adsorption capacity of CHAP-γ-FeO/BC on U(Ⅵ) reaches 324.4 mg/g, which is better than most of the reported materials of the same kind, and the removal rate reaches 95.93%; the proposed two-stage kinetic model (R2=0.999, 1, 0.999) and Langmuir model (R2=0.988, 0.991, 0.0.983) can better fit the adsorption process of U(Ⅵ) on U(Ⅵ) by monolayer chemisorption. , indicating that the monomolecular layer chemisorption is dominated and the adsorption is a spontaneous heat adsorption process, and the high temperature is favorable for the reaction to proceed. (3) After five adsorption-desorption experiments, the removal rate of U(VI) is still maintained at about 85.19%, indicating that the material has good regeneration performance.Conclusions: The low crystallinity CHAP and γ-FeO are successfully loaded on BC, which both attenuates the self-agglomeration of CHAP nanoparticles and enhances the removal performance of CHAP-γ-FeO/BC on U(VI) in water; and also makes the composite materials have efficient separation recovery and recycling performance in the magnetic field. Meanwhile, CHAP-γ-FeO/BC can still realize the selective adsorption of U(VI) in the presence of multiple interfering ions, with strong anti-interference ability.CHAP-γ-FeO/BC also has good regeneration performance. However, in the adsorption and desorption experiments, there is a lack of in-depth investigation into the reasons for the decrease in the removal rate of CHAP-γ-FeO/BC after five adsorption-desorption experiments, which will be the research direction and focus of the subsequent study.
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