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腐殖酸负载对萘和1-萘酚在生物炭上吸附动力学的影响

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张萌, 吕耀斌, 朱一滔, 施羲渊, 杨庆, 王喜龙, 李威, 李萍萍. 腐殖酸负载对萘和1-萘酚在生物炭上吸附动力学的影响[J]. 环境化学, 2020, (1): 101-109. doi: 10.7524/j.issn.0254-6108.2019081511
引用本文: 张萌, 吕耀斌, 朱一滔, 施羲渊, 杨庆, 王喜龙, 李威, 李萍萍. 腐殖酸负载对萘和1-萘酚在生物炭上吸附动力学的影响[J]. 环境化学, 2020, (1): 101-109. doi: 10.7524/j.issn.0254-6108.2019081511
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ZHANG Meng, LYU Yaobin, ZHU Yitao, SHI Xiyuan, YANG Qing, WANG Xilong, LI Wei, LI Pingping. Impact of humic acid coating on sorption kinetics of naphthalene and 1-naphthol on biochar[J]. Environmental Chemistry, 2020, (1): 101-109. doi: 10.7524/j.issn.0254-6108.2019081511
Citation: ZHANG Meng, LYU Yaobin, ZHU Yitao, SHI Xiyuan, YANG Qing, WANG Xilong, LI Wei, LI Pingping. Impact of humic acid coating on sorption kinetics of naphthalene and 1-naphthol on biochar[J]. Environmental Chemistry, 2020, (1): 101-109. doi: 10.7524/j.issn.0254-6108.2019081511
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腐殖酸负载对萘和1-萘酚在生物炭上吸附动力学的影响

  • 1. 南京林业大学南方现代林业协同创新中心, 生物与环境学院, 南京, 210037;

  • 2. 北京大学城市与环境学院, 地表过程分析与模拟教育部重点实验室, 北京, 100871

    • 通讯作者: 张萌, E-mail: zhangmeng@njfu.edu.cn ; 
  • 基金项目:

    国家自然科学基金（41701555，31700441），南京林业大学大学生创新训练计划项目（2019NFUSPITP0434）和江苏高校优势学科建设工程项目（PAPD）资助.

Impact of humic acid coating on sorption kinetics of naphthalene and 1-naphthol on biochar

  • 1. Co-Innovation Center for Sustainable Forestry in Southern China, College of Biology and the Environment, Nanjing Forestry University, Nanjing, 210037, China;

  • 2. Laboratory for Earth Surface Processes, College of Urban and Environmental Sciences, Peking University, Beijing, 100871, China

    • Corresponding author: ZHANG Meng, zhangmeng@njfu.edu.cn ; 
  • Fund Project: Supported by the National Natural Science Foundation of China(41701555, 31700441),Students Practice Innovation and Training Program of Nanjing Forestry University(2019NFUSPITP0434)and Priority Academic Program Development of Jiangsu Higher Education Institutions(PAPD).

  • 摘要: 进入环境的生物炭对有机污染物的吸附过程受到普遍共存的溶解性有机质的影响.本研究将两种腐殖酸组分负载在以玉米秸秆为原料、不同炭化温度下（200、400、600℃）制得的生物炭上，考察极性和非极性有机污染物萘和1-萘酚在原始和腐殖酸负载生物炭上的吸附动力学，分别应用拟一级、拟二级和双室一级3种动力学模型对实验数据进行拟合.结果表明，拟二级和双室一级动力学模型均能较好地描述动力学吸附过程.腐殖酸负载对生物炭上萘和1-萘酚的吸附动力学有显著影响，使得平衡吸附量（Qe）下降，而表观吸附速率提高.致密的芳香碳组分和纳米级孔隙主要对萘和1-萘酚在生物炭上的慢吸附单元起作用，腐殖酸负载降低了生物炭的芳香化程度和孔隙度，慢吸附对总吸附的贡献（fslow）降低.生物炭内部有机碳的致密性降低，使得萘和1-萘酚分子容易扩散进入生物炭颗粒内部，加之表面积和孔隙度减少，缩短吸附平衡时间，两种化合物的慢吸附速率常数（kslow）均提高.负载腐殖酸后，两种化合物的快吸附速率常数（kfast）的变化却不同.腐殖酸负载向生物炭表面引入含氧极性官能团，阻碍萘分子向表面疏水吸附位点扩散，使得萘的kfast下降；而由于1-萘酚是极性有机物，除了疏水作用，其结构中的—OH能通过氢键与生物炭表面相互作用，其kfast反而升高.
    Abstract: The sorption process of organic pollutants on biochars in the environment is affected by the ubiquitously existed dissolved organic matter. In this study, two humic acid (HA) fractions were coated on maize-derived biochars which were generated at different charring temperatures (200, 400, 600℃) to get HA-biochar complexes. The sorption kinetics of a polar organic pollutant (1-naphthol) and a nonpolar one (naphthalene) on the original and HA-coated biochars were investigated. The results showed that the kinetic data were better fitted with the pseudo second-order model, followed by the two-compartment one in comparison with the pseudo first-order model. Humic acid coating had significant impact on the sorption kinetics of the two tested compounds on biochars. Coating with HA decreased the equilibrium sorption capacity (Qe), but increased the apparent sorption rate. The HA coating decreased the amount of aromatic carbon components and porous structures in biochars, which were responsible for the slow sorption of naphthalene and 1-naphthol on biochars, resulting in the reduction of slow sorption contributions to total sorption (fslow). The decreased condensation of organic carbon in the biochars induced by HA allowed the naphthalene and 1-naphthol molecules to diffuse more easily into biochars. In addition, the decrease of surface area and porosity shortened the sorption equilibrium time, and thus the rate constants for slowly sorbing component (kslow) of both compounds increased. However, the change in fast sorption rate constants of these two compounds was different after HA coating. The introduction of O-containing polar functionalities to the biochars caused by HA coating would block the diffusion of naphthalene molecules towards the hydrophobic sorption sites on the surface of biochars, lowering its fast-sorbing rate constant (kfast). But as 1-naphthol was a polar compound with -OH substitution in its structure, which was able to interact with biochar surfaces via hydrogen bonds, thus leading to a higher kfast value.
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  • 收稿日期:  2019-08-15
  • 刊出日期:  2020-01-01

腐殖酸负载对萘和1-萘酚在生物炭上吸附动力学的影响

    通讯作者: 张萌, E-mail: zhangmeng@njfu.edu.cn ; 
  • 1. 南京林业大学南方现代林业协同创新中心, 生物与环境学院, 南京, 210037;
  • 2. 北京大学城市与环境学院, 地表过程分析与模拟教育部重点实验室, 北京, 100871
  • 收稿日期:  2019-08-15
  • 网络出版日期:  2020-01-01
基金项目:

国家自然科学基金（41701555，31700441），南京林业大学大学生创新训练计划项目（2019NFUSPITP0434）和江苏高校优势学科建设工程项目（PAPD）资助.

摘要: 进入环境的生物炭对有机污染物的吸附过程受到普遍共存的溶解性有机质的影响.本研究将两种腐殖酸组分负载在以玉米秸秆为原料、不同炭化温度下（200、400、600℃）制得的生物炭上，考察极性和非极性有机污染物萘和1-萘酚在原始和腐殖酸负载生物炭上的吸附动力学，分别应用拟一级、拟二级和双室一级3种动力学模型对实验数据进行拟合.结果表明，拟二级和双室一级动力学模型均能较好地描述动力学吸附过程.腐殖酸负载对生物炭上萘和1-萘酚的吸附动力学有显著影响，使得平衡吸附量（Qe）下降，而表观吸附速率提高.致密的芳香碳组分和纳米级孔隙主要对萘和1-萘酚在生物炭上的慢吸附单元起作用，腐殖酸负载降低了生物炭的芳香化程度和孔隙度，慢吸附对总吸附的贡献（fslow）降低.生物炭内部有机碳的致密性降低，使得萘和1-萘酚分子容易扩散进入生物炭颗粒内部，加之表面积和孔隙度减少，缩短吸附平衡时间，两种化合物的慢吸附速率常数（kslow）均提高.负载腐殖酸后，两种化合物的快吸附速率常数（kfast）的变化却不同.腐殖酸负载向生物炭表面引入含氧极性官能团，阻碍萘分子向表面疏水吸附位点扩散，使得萘的kfast下降；而由于1-萘酚是极性有机物，除了疏水作用，其结构中的—OH能通过氢键与生物炭表面相互作用，其kfast反而升高.

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