铁掺杂石墨化多孔磁性生物炭耦合过硫酸盐氧化体系去除水体中雌激素的过程和机理研究

The water bodies near the concentrated animal feeding operations (CAFOs) areas are seriously polluted by the estrogens in livestock and poultry excrement, which may bring harm to the ecological environment and human health. Iron-doped, porous and graphitized biochar has great potential in activating persulfate to treat organic pollutants, while the relevant studies are lacked. There is no report on the application of this system in the treatment of estrogen in water bodies, and the relevant processes and mechanisms are not clear. Therefore, this project intends to adopt the "one-step" method to optimize the preparation of iron-doped graphitic porous magnetic biochar (Fe/GPMB) and establish a coupling system with persulfate for the removal of estrogen in water. The batch experiment, the heterogeneous magnetic catalyst/persulfate reaction system (HMC/PS) experiment and the persulfate-enhanced permeable reactive barriers system (PE-PRB) experiment will be carried out to investigate the estrogen removal efficiency and the major impact factors of this coupling system, to explore the role of each component in coupling system for estrogen removal, and to elucidate the estrogen degradation pathways. In addition, the in-situ EPR continuous detection method and electrochemical analysis method will be applied to reveal the mechanism of activating persulfate and estrogen removal by Fe/GPMB. Therefore, it is expected that the results of the project will provide important theoretical basis and technical support for the development of a green, cheap and efficient method for the treatment of estrogen in water.

集约化养殖区畜禽粪便中的雌激素对附近水体污染严重，危害生态环境和人类健康。铁掺杂、多孔化和石墨化处理后的生物炭在活化过硫酸盐修复有机物污染水体方面具有较好应用潜力，但尚无将该体系应用于水体中雌激素处理的报道，且相关过程和机理尚不清楚。因此，本项目拟采用“一步法”优化制备出铁掺杂石墨化多孔磁性生物炭（Fe/GPMB），并与过硫酸盐形成耦合体系，用于水体中雌激素的去除。拟通过静态条件下的批量实验，以及动态条件下的非均相磁性催化剂/过硫酸盐反应系统（HMC/PS）和过硫酸盐强化可渗透反应墙（PE-PRB）实验，考察耦合体系去除雌激素的效能和关键影响因子，研究耦合体系中各组分在雌激素去除中的作用，探究雌激素降解路径；并通过原位EPR连续检测和电化学分析法综合揭示Fe/GPMB活化过硫酸盐和雌激素去除的机理。本研究有望为发展一种绿色、廉价、高效的水体中雌激素去除方法提供重要理论依据与技术支持。

集约化养殖区畜禽污水中以雌激素为代表的有机污染物对附近水体污染严重，危害生态环境和人类健康。基于过硫酸盐活化的高级氧化法在有机污染水体处理中具有广阔的应用前景。本项目主要通过调控改性方法、热解条件等实现生物炭基材料的铁掺杂、多孔化和石墨化，同时改善炭材料的导电性、孔特性和稳定性，增加电子转移速率和吸附能力，从而有效发挥生物炭的基质作用、吸附作用和活化过硫酸盐作用。项目中研究了铁掺杂石墨化多孔磁性生物炭/过硫酸盐体系去除雌激素的过程和优化去除条件，评估了石墨化生物炭基材料催化活化过硫酸盐体系中材料的稳定性、重复利用性和抗环境因素干扰能力，探究理化因子和水环境条件对耦合体系去除污染物效能的影响及作用机制。项目明确了不同石墨化生物炭基材料/过硫酸盐体系产生的活性物质、雌激素降解路径和中间产物；同时结合电化学等表征手段综合分析铁掺杂石墨化多孔磁性生物炭耦合过硫酸盐体系中活性位点和活性物质的产生，以及自由基、非自由基中电子转移机制。项目综合揭示铁掺杂石墨化多孔磁性生物炭活化过硫酸盐对水体中雌激素去除的机理，以及该耦合体系在实际水体雌激素污染修复中的应用潜力。本研究为发展一种绿色、廉价、高效生物炭基材料及其耦合过硫酸盐体系对水体中雌激素去除提供重要理论依据与技术支持。