School of Water Conservancy and Architectural Engineering, Shihezi University, Shihezi 832003, PR China; State Key Laboratory of Coal Mine Disaster Dynamics and Control, Chongqing University, Chongqing 400044, PR China.
State Key Laboratory of Coal Mine Disaster Dynamics and Control, Chongqing University, Chongqing 400044, PR China; Key Laboratory of Yangtze River Water Environment, Ministry of Education, Tongji University, Shanghai 200092, PR China.
J Hazard Mater. 2021 Aug 15;416:125796. doi: 10.1016/j.jhazmat.2021.125796. Epub 2021 Apr 1.
The N, S co-doped biochar (N, S-BC) with multistage pore structure was successfully synthesized from nanocellulose and thiourea by one-step pyrolysis, which could effectively activate peroxymonosulfate (PMS) to degrade sulfamethoxazole (SMX) in water. Moreover, the removal efficiency of SMX by this oxidation system was 2.3-3.1 times than that of other systems activated by common metal oxides (such as FeO、FeO, and MnO). More importantly, the mechanism of the N, S-BC/PMS process was deduced by reactive oxygen species (ROS) quenching experiment and electron paramagnetic resonance (EPR) test, which exhibited that surface-bound free radicals and singlet oxygen (O) played an essential role in the SMX degradation. Surprisingly, the sulfate radical (SO) and hydroxyl radical (OH) produced in this system existed in a bound state on the surface of the carbon catalyst to react with SMX, rather than dispersed in the aqueous solution. This particular form of free radicals could resist the influence of background substances and pH changes in water, and maintain excellent SMX degradation efficiency under different water matrices and pH. This study provides a new insight into the application of carbon catalyst in actual water pollution control.
N、S 共掺杂生物炭(N、S-BC)具有多级孔结构,是通过一步热解纳米纤维素和硫脲成功合成的,可有效激活过一硫酸盐(PMS)来降解水中的磺胺甲恶唑(SMX)。此外,该氧化体系对 SMX 的去除效率比其他由常见金属氧化物(如 FeO、FeO 和 MnO)激活的体系高 2.3-3.1 倍。更重要的是,通过活性氧物种(ROS)猝灭实验和电子顺磁共振(EPR)测试推导出了 N、S-BC/PMS 工艺的机理,表明表面结合的自由基和单线态氧(O)在 SMX 降解中起着重要作用。令人惊讶的是,该体系中生成的硫酸根自由基(SO)和羟基自由基(OH)以结合态存在于碳催化剂表面与 SMX 反应,而不是分散在水溶液中。这种特殊形式的自由基可以抵抗水中背景物质和 pH 值变化的影响,在不同的水基质和 pH 值下保持优异的 SMX 降解效率。本研究为碳催化剂在实际水污染控制中的应用提供了新的思路。