杨树落叶生物炭特性及其对污水中氧氟沙星的协同净化机制

Characteristics of poplar leaf biochar and its synergistic purification mechanism for ofloxacin in wastewater

  • 摘要: 为探究废弃生物质资源化利用在水体抗生素污染治理中的应用潜力,以杨树落叶为原料,在不同热解温度(300~700 ℃)条件下制备生物炭(记为BC300~BC700),通过考察不同温度制备生物炭对污水中氧氟沙星(OFX)的吸附效能,筛选最优热解温度;采用扫描电子显微镜、BET比表面积分析、X射线光电子能谱及密度泛函理论计算等手段,探讨杨树落叶生物炭对OFX吸附性能与其结构特征之间的关系。结果表明:热解温度显著影响生物炭孔隙结构与表面化学性质,随着热解温度由300 ℃升至600 ℃,制备的生物炭比表面积由22.711 m2/g增至379.656 m2/g,总孔体积由0.036 0 cm3/g增至0.368 2 cm3/g,微孔体积增至0.187 cm3/g,平均孔径降至2.734 4 nm,BC600综合性能最佳。模拟体系中,相较BC300,BC600对50 mg/L和100 mg/L OFX的去除率分别由42.2%和36.7%提高至78.4%和66.5%;实际污水中,BC600对OFX、化学需氧量、氨氮、硝氮、总氮和总磷的去除率分别达到73%、91%、82%、78%、88%和94%。落叶生物炭对OFX的等温吸附过程符合Langmuir模型(R2>0.97),在35 ℃条件下其最大吸附容量为80.9 mg/g。吸附动力学分析表明,该过程受物理扩散与化学吸附协同控制。DFT吸附能计算结果表明,生物炭的羟基和羧基通过增强氢键作用、π—π堆积及电子给体-受体相互作用,提高了生物炭对OFX的吸附能力。研究显示,杨树落叶生物炭在实际污水抗生素污染治理方面具有良好的应用潜力。

     

    Abstract: To explore the application potential of waste biomass valorization in the treatment of antibiotic pollution in water bodies, poplar leaf litter was used as the feedstock to prepare biochar (labeled BC300-BC700) at different pyrolysis temperatures (300-700 ℃). By evaluating the adsorption performance of biochar prepared at different temperatures for ofloxacin (OFX) in wastewater, the optimum pyrolysis temperature was identified. Scanning electron microscopy (SEM), Brunauer-Emmett-Teller (BET) specific surface area analysis, X-ray photoelectron spectroscopy (XPS), and density functional theory (DFT) calculations were employed to investigate the relationship between the adsorption performance of poplar leaf biochar for OFX and its structural characteristics. The results showed that the pyrolysis temperature significantly affected the pore structure and surface chemical properties of the biochar. As the pyrolysis temperature increased from 300 ℃ to 600 ℃, the specific surface area of the prepared biochar increased from 22.711 m2/g to 379.656 m2/g, the total pore volume increased from 0.036 0 cm3/g to 0.368 2 cm3/g, with the micropore volume reaching 0.187 cm3/g and the average pore diameter increasing to 2.734 4 nm. The comprehensive performance of BC600 was the best. In the simulation system, compared with BC300, the removal rates of OFX at 50 and 100 mg/L by BC600 increased from 42.2% and 36.7% to 78.4% and 66.5%, respectively. In actual wastewater, the removal efficiencies of BC600 for OFX, COD, \mathrmNH_4^+ -N, \mathrmNO_3^- -N, TN, and TP reached 73%, 91%, 82%, 78%, 88%, and 94%, respectively. The adsorption isotherms of OFX onto poplar leaf biochar were well described by the Langmuir model (R2>0.97), and the maximum adsorption capacity at 35 ℃ was 80.9 mg/g. Adsorption kinetic analysis indicated that the process was jointly controlled by physical diffusion and chemical adsorption. DFT-calculated adsorption energies further demonstrated that hydroxyl and carboxyl groups on the biochar enhanced OFX adsorption by strengthening hydrogen bonding, π—π stacking, and electron donor–acceptor interactions. These findings indicate that poplar leaf biochar has promising potential for the treatment of antibiotic pollution in actual wastewater.

     

/

返回文章
返回