董姝楠, 夏继红, 王为木, 刘慧, 盛丽婷. 水体离子强度、pH值和腐殖酸浓度对石墨相氮化碳沉降的影响[J]. 农业工程学报, 2021, 37(17): 218-224. DOI: 10.11975/j.issn.1002-6819.2021.17.025
    引用本文: 董姝楠, 夏继红, 王为木, 刘慧, 盛丽婷. 水体离子强度、pH值和腐殖酸浓度对石墨相氮化碳沉降的影响[J]. 农业工程学报, 2021, 37(17): 218-224. DOI: 10.11975/j.issn.1002-6819.2021.17.025
    Dong Shunan, Xia Jihong, Wang Weimu, Liu Hui, Sheng Liting. Effects of ionic strength, pH value and humic acid on the settlement of graphitic carbon nitride[J]. Transactions of the Chinese Society of Agricultural Engineering (Transactions of the CSAE), 2021, 37(17): 218-224. DOI: 10.11975/j.issn.1002-6819.2021.17.025
    Citation: Dong Shunan, Xia Jihong, Wang Weimu, Liu Hui, Sheng Liting. Effects of ionic strength, pH value and humic acid on the settlement of graphitic carbon nitride[J]. Transactions of the Chinese Society of Agricultural Engineering (Transactions of the CSAE), 2021, 37(17): 218-224. DOI: 10.11975/j.issn.1002-6819.2021.17.025

    水体离子强度、pH值和腐殖酸浓度对石墨相氮化碳沉降的影响

    Effects of ionic strength, pH value and humic acid on the settlement of graphitic carbon nitride

    • 摘要: 为解决农业环境中石墨相氮化碳(g-C3N4)的风险评估、污染预测等问题,该研究以g-C3N4为研究对象,通过室内沉降试验、沉降模型计算、DLVO(Derjaguine Landaue Verweye Overbeek)理论计算相结合的研究方法,考察离子强度(Ionic Strength,IS)、pH值和腐殖酸(Humic Acid,HA)3种典型水环境因素对g-C3N4沉降与分散稳定性的影响。研究结果表明,g-C3N4的沉降随水环境IS升高而明显增强,IS由0上升至50.0 mmol/L,360 min后g-C3N4悬液的终点标准化浓度(C/C0)由0.86变为0.58。水环境pH值变化对g-C3N4沉降与分散稳定性影响较小,pH值由2上升至4,360 min后g-C3N4悬液的终点C/C0由0.63变为0.57;而pH值由4上升至10,360 min后g-C3N4悬液的终点C/C0由0.57变为0.78。水环境中HA的存在能够增强g-C3N4的分散稳定性,HA浓度由0提升至10.0 mg/L,360 min后g-C3N4悬液的终点C/C0由0.60变为0.91。一阶动力学沉降模型能够有效模拟水体中g-C3N4的沉降动力学曲线,DLVO理论的计算结果能够反映出不同条件下g-C3N4颗粒间的势能分布。研究结果对于准确分析评估农业环境中g-C3N4的环境风险和生态安全具有重要意义。

       

      Abstract: Graphitic Carbon Nitride (g-C3N4) has widely been used on the photocatalytic degradation of agricultural organic pollutants (e.g. pesticides, polycyclic aromatic hydrocarbons, and antibiotics). Therefore, it is inevitably entering into the agricultural environment soil, leading to potential risks. This study aims to better evaluate and then predict the photocatalytic efficiency and environmental risk of g-C3N4 application. Experiment, simulation, and theoretical calculation were conducted to investigate the settlement and dispersion stability of g-C3N4 in the aqueous environment. Three typical water factors were also considered, including ionic strength, pH values, and humic acid concentration. Experimental data showed that the water ionic strength was the most important factor in the settlement and dispersion stability of g-C3N4. A one-site kinetic settlement model was also well established to fit the settlement rate data of g-C3N4 from the experimental measurement. The extended DLVO theory was selected to explain the energy distribution between g-C3N4 particles in the aqueous environment. The settlement of g-C3N4 was remarkably enhanced with the increasing ionic strength, thereby reducing the dispersion stability. Specifically, the final standardized concentration (after 360 min) of g-C3N4 suspension decreased from 0.86 to 0.58, while the fitted settlement rate increased from 0.014 4 to 0.019 1 cm/min, as well as the Zeta potential of g-C3N4 particles increased from -37.1 to -12.7 mV, with the ionic strength increased from 0 to 50 mmol/L. The variation of Zeta potential indicated that the charge shielding of g-C3N4 particles increased with the increasing ionic strength, leading to the compressed electrical double layer and enhanced aggregation of g-C3N4 for better settlement and reduced dispersion stability. Additionally, the water pH showed a relatively low impact on the settlement and dispersion stability of g-C3N4. The settlement of g-C3N4 was firstly enhanced and then reduced with the increasing pH values. Specifically, the final standardized concentration (after 360 min) of g-C3N4 suspension firstly decreased from 0.63 to 0.57, as the pH values increased from 2 to 4, and then increased from 0.57 to 0.78 with the pH values further increased from 4 to 10. Particularly, the tendency of fitted settlement rate was well consistent with the experimental measurement. By contrast, the hydrodynamic radius of g-C3N4 also firstly increased from 1 116 to 1 271 nm, as the pH values increased from 2 to 4, whereas, then decreased from 1 271 to 862 nm with the pH values further increased from 4 to 10. The Zeta potential of g-C3N4 particles decreased from 18.6 to -57.0 mV with the increasing pH values. Correspondingly, the highest settlement and lowest dispersion stability of g-C3N4 were achieved in the aqueous environment, when the pH value approached the isoelectric point (pH was 4). Furthermore, the electrostatic repulsion and steric hindrance between g-C3N4 particles increased in the presence of humic acid, leading to the reduced settlement and enhanced dispersion stability of g-C3N4 with the increasing concentrations. However, there was a critical point for the enhanced efficiency. More importantly, the final standardized concentration (after 360 min) of g-C3N4 suspension significantly increased from 0.60 to 0.87, as the humic acid concentrations increased from 0 to 5 mg/L, but remained at 0.91 with the humic acid concentrations further increased to 10 mg/L. Anyway, the finding can be expected to well elucidate the settlement and dispersion stability of g-C3N4 in the aqueous environment under typical conditions, particularly for the better understanding of potential behaviors of graphitic carbon nitride in modern agriculture.

       

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