周刚,栾国梁,李帅龙,等. 沙柳木粉基高效吸附材料对煤矿废水中Fe(II)和Mn(II)作用特性及机理[J]. 煤炭学报,2024,49(3):1570−1582. DOI: 10.13225/j.cnki.jccs.2023.1804
引用本文: 周刚,栾国梁,李帅龙,等. 沙柳木粉基高效吸附材料对煤矿废水中Fe(II)和Mn(II)作用特性及机理[J]. 煤炭学报,2024,49(3):1570−1582. DOI: 10.13225/j.cnki.jccs.2023.1804
ZHOU Gang,LUAN Guoliang,LI Shuailong,et al. Action characteristics and mechanism of Salix wood powder-based high-efficiency adsorption materials on Fe(II) and Mn(II) in coal mine wastewater[J]. Journal of China Coal Society,2024,49(3):1570−1582. DOI: 10.13225/j.cnki.jccs.2023.1804
Citation: ZHOU Gang,LUAN Guoliang,LI Shuailong,et al. Action characteristics and mechanism of Salix wood powder-based high-efficiency adsorption materials on Fe(II) and Mn(II) in coal mine wastewater[J]. Journal of China Coal Society,2024,49(3):1570−1582. DOI: 10.13225/j.cnki.jccs.2023.1804

沙柳木粉基高效吸附材料对煤矿废水中Fe(II)和Mn(II)作用特性及机理

Action characteristics and mechanism of Salix wood powder-based high-efficiency adsorption materials on Fe(II) and Mn(II) in coal mine wastewater

  • 摘要: 针对煤矿酸性废水中含有较高质量浓度铁离子和锰离子的问题,以沙柳木粉为主要原料,遵循农林废弃物提取再利用原则,经过NaOH、Na2SO3等溶液处理后获得脱木素木粉(DWF),通过微波辅助−原位合成的手段,制备了一种针对煤矿废水中Fe(II)和Mn(II)的吸附剂(AA-DWF-PAM)。借助扫描电子显微镜(SEM)、N2吸附−脱附、傅里叶变换红外光谱(FTIR)和红外热重联用(TG-FTIR)对产物的微观结构、反应机理、热稳定性进行了分析,探讨了AA-DWF-PAM的最佳吸附条件、吸附动力学、吸附等温线,研究了AA-DWF-PAM对Fe(II)和Mn(II)的吸附特性和吸附机理。表征实验结果表明:AA-DWF-PAM整体存在较多孔洞并呈现网状结构,且比表面积(BET)为150.83 m2/g,说明改性后的吸附剂具有较大的比表面积,能够为Fe(II)和Mn(II)吸附提供较多位点和空间;此外,AA-DWF-PAM热解气态产物主要有H2O、CO2以及少量CO,裂解温度较高,其结构稳定性较强。吸附特性实验研究表明:AA-DWF-PAM用量为4 g/L、溶液pH=4、吸附时间达到200 min,以及Fe(II)、Mn(II)初始质量浓度为100 mg/L和80 mg/L时,为AA-DWF-PAM的最佳吸附条件;经过计算得知,AA-DWF-PAM更接近于伪二级动力学假设,吸附主要控制过程为化学过程,且吸附过程更符合Langmuir方程的单层分子吸附,Fe(II)和Mn(II)的理论最大吸附量分别为192.29 mg/g和123.65 mg/g;通过Materials Studio对吸附过程进行分子模拟和量子化学计算得知,吸附过程中—NH2、—COOH以及—OH官能团起到静电吸附作用。因此,合理利用农林废弃物,为煤矿酸性废水治理提供了新途径,开发的AA-DWF-PAM吸附剂,能够有效处理煤矿酸性废水中的铁锰离子。

     

    Abstract: In response to the problem of acidic coal mine wastewater containing high concentrations of iron and manganese ions, Salix wood powder was used as the main raw material, following the principle of extraction and reuse of agricultural and forestry waste, the delignified wood powder (DWF) was obtained after the treatment with NaOH, Na2SO3 and other solutions. Through microwave assisted in-situ synthesis, an adsorbent (AA-DWF-PAM) for Fe(II) and Mn(II) in coal mine wastewater was prepared. The microstructure, reaction mechanism and thermal stability of the product were analyzed by scanning electron microscopy (SEM), N2 adsorption desorption, Fourier transform infrared spectroscopy (FTIR) and infrared thermogravimetry (TG-FTIR). The optimal adsorption conditions, adsorption kinetics and adsorption isotherms of AA-DWF-PAM were discussed. The adsorption characteristics and adsorption mechanism of AA-DWF-PAM for Fe(II) and Mn(II) were studied. The characterization experiment results show that the AA-DWF-PAM has many holes and presents a network structure, and the BET specific surface area is 150.83 m2/g, indicating that the modified adsorbent has a large specific surface area, which can provide more sites and spaces for the adsorption of Fe(II) and Mn(II). In addition, the gaseous products of AA-DWF-PAM pyrolysis mainly include H2O, CO2 and a small amount of CO, with high pyrolysis temperature and strong structural stability. The experimental study on adsorption characteristics shows that the best adsorption conditions for the AA-DWF-PAM are determined as follows: the AA-DWF-PAM dosage is 4 g/L, solution pH=4, and adsorption time is 200 min. According to the calculation, the AA-DWF-PAM is closer to the pseudo second order kinetic hypothesis, the main control process of adsorption is a chemical process, and the adsorption process is more consistent with the single-layer molecular adsorption of Langmuir equation. The theoretical maximum adsorption capacities of Fe(II) and Mn(II) are 192.29 mg/g and 123.65 mg/g respectively. According to the molecular simulation and quantum chemical calculation of the modified adsorption process in Materials Studio, the —NH2, —COOH and —OH functional groups play an electrostatic adsorption role in the adsorption process. Therefore, the rational utilization of agricultural and forestry waste provides a new approach for the treatment of acidic coal mine wastewater. The developed AA-DWF-PAM adsorbent can effectively treat iron and manganese ions in the acidic coal mine wastewater.

     

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