State Key Laboratory of Urban Water Resources and Environment, School of Environment, Harbin Institute of Technology, Harbin 150090, China.
State Key Laboratory of Urban Water Resources and Environment, School of Environment, Harbin Institute of Technology, Harbin 150090, China.
J Hazard Mater. 2022 Jun 15;432:128757. doi: 10.1016/j.jhazmat.2022.128757. Epub 2022 Mar 23.
Novel nitrogen (N)-doped cellulose biochar (NC1000-10) with large adsorption capacity (103.59 mg g) for atrazine (ATZ) was synthesized through the one-pot method. It has the best adsorption efficiency than N-doped biochars prepared from hemicellulose and lignin. The adsorption behaviors of ATZ by N-doped biochars with different N doping ratios (NC1000-5, NC1000-10, NC1000-20 and NC1000-30) were significantly different, which was attributed to the difference of sp conjugate C (I/I = 0.99-1.18) and doped heteroatom N (pyridinic N, pyrrolic N and graphitic N). Adsorption performance of ATZ on NC1000-10 conformed to the pseudo-second-order kinetic and Langmuir adsorption isotherm model. Thermodynamic calculations showed that adsorption performance was favorable. Besides, wide pH adaptability (pH = 2-10), good resistance to ionic strength and excellent recycling efficiency make it have extensive practical application potential. Further material characterizations and the density functional theory (DFT) calculations indicated that good adsorption performance of NC1000-10 for ATZ mainly depended on chemisorption, and π-π electron donor-acceptor (EDA) interaction contributed the most due to high graphitization degree. Specifically, pyridinic N and graphitic N further promoted adsorption performance by hydrophobic effect and π-π EDA interaction between ATZ and NC1000-10, respectively. Pyrrolic N and other surface functional groups (-COOH, -OH) facilitated the hydrogen bond effect.
通过一步法合成了具有大吸附量（103.59mg/g）的新型氮（N）掺杂纤维素生物炭（NC1000-10），用于吸附莠去津（ATZ）。它的吸附效率优于由半纤维素和木质素制备的 N 掺杂生物炭。不同 N 掺杂比（NC1000-5、NC1000-10、NC1000-20 和 NC1000-30）的 N 掺杂生物炭对 ATZ 的吸附行为存在显著差异，这归因于 sp 共轭 C（I/I = 0.99-1.18）和掺杂杂原子 N（吡啶 N、吡咯 N 和石墨 N）的差异。ATZ 在 NC1000-10 上的吸附性能符合准二级动力学和 Langmuir 吸附等温线模型。热力学计算表明吸附性能是有利的。此外，宽 pH 适应性（pH = 2-10）、良好的耐离子强度和优异的回收效率使其具有广泛的实际应用潜力。进一步的材料特性和密度泛函理论（DFT）计算表明，NC1000-10 对 ATZ 具有良好的吸附性能主要取决于化学吸附，而由于高石墨化程度，π-π 电子给体-受体（EDA）相互作用的贡献最大。具体而言，吡啶 N 和石墨 N 通过疏水效应和 ATZ 与 NC1000-10 之间的π-π EDA 相互作用进一步促进了吸附性能，吡咯 N 和其他表面官能团（-COOH、-OH）则促进了氢键作用。
