Shandong Key Laboratory of Water Pollution Control and Resource Reuse, School of Environmental Science & Engineering, Shandong University, Qingdao 266237, PR China.
Centre for Technology in Water and Wastewater, School of Civil and Environmental Engineering, University of Technology Sydney, Ultimo, NSW 2007, Australia.
Sci Total Environ. 2020 Sep 1;733:139267. doi: 10.1016/j.scitotenv.2020.139267. Epub 2020 May 8.
An innovative ammoniation-hydrothermal method of biochar production was developed for the adsorption of phenanthrene (PHE) from aqueous solutions in this paper. Phragmites australis (PA) was used to produce biochar in a hydrothermal kettle at 280 °C in muffle furnace using urea as an ammoniation reagent. Characterizations were executed by scanning electron microscope (SEM), N adsorption/desorption isotherms, X-ray diffraction (XRD), elemental analysis, X-ray photoelectron spectroscopy (XPS) and Fourier transform infrared spectroscopy (FT-IR) to explore its morphological, physical, and chemical properties. Batch experiments of PHE adsorption were carried out to study the adsorption isotherms and kinetics. Quantum chemistry computational simulations were employed based on density functional theory (DFT) to establish and optimize adsorption configurations and analyze the biochar's structural effects on adsorption performance. Results showed that the ammoniation-hydrothermal method produced biochar with a higher surface area and a maximum equilibrium adsorption capacity of 1.97 mg/g. The adsorption fitted well with Freundlich isotherm model (R > 0.96) and Pseudo-second-order kinetic model (R > 0.82). Adsorption energy calculation revealed that the N functionalities, especially pyridine N in the N-doped biochar structure, exhibited stronger binding ability with PHE, which contributed most to the favorable adsorption ability of the ammoniation-hydrothermal biochar.
本文开发了一种创新性的生物炭氨化-水热生产方法，用于从水溶液中吸附水中的菲（PHE）。本研究采用尿素作为氨化试剂，在马弗炉中 280°C 的水热釜内用芦苇（PA）制备生物炭。通过扫描电子显微镜（SEM）、N 吸附/解吸等温线、X 射线衍射（XRD）、元素分析、X 射线光电子能谱（XPS）和傅里叶变换红外光谱（FT-IR）对其形态、物理和化学性质进行了表征。进行了 PHE 吸附的批量实验，以研究吸附等温线和动力学。基于密度泛函理论（DFT）的量子化学计算模拟用于建立和优化吸附构型，并分析生物炭的结构对吸附性能的影响。结果表明，氨化-水热法制备的生物炭具有更高的比表面积，最大平衡吸附容量为 1.97mg/g。吸附拟合良好的 Freundlich 等温模型（R>0.96）和拟二级动力学模型（R>0.82）。吸附能计算表明，N 官能团，特别是 N 掺杂生物炭结构中的吡啶 N，与 PHE 具有更强的结合能力，这对氨化-水热生物炭的有利吸附能力贡献最大。
