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由糖浆基废物制备含羰基、羟基和氨基的微孔碳质纳米球去除磺胺甲恶唑

Preparation of carbonyl, hydroxyl, and amino-functionalized microporous carbonaceous nanospheres from syrup-based waste to remove sulfamethazine.

机构信息

Department of Chemistry, Chemical engineering and Environmental Science, Fujian Provincial Key Laboratory of Modern Analytical Science and Separation Technology (Minnan Normal University) & Fujian Provincial Key Laboratory of Pollution Monitoring and Control (Minnan Normal University), Minnan Normal University, Zhangzhou, China.

Laboratory of Marine Chemistry and Environmental Monitoring Technology, Third Institute of Oceanography, Ministry of Natural Resources, Xiamen, China.

出版信息

Environ Sci Pollut Res Int. 2022 Apr;29(19):27688-27702. doi: 10.1007/s11356-021-18375-5. Epub 2022 Jan 4.

DOI:10.1007/s11356-021-18375-5
PMID:34984610
Abstract

Sulfadiazine (SDZ) was a persistent sulfonamide antibiotic with a potential risk to human health. The waste dipping syrup was considered useless and environmentally unfriendly solution. In this work, carbonyl-, hydroxyl-, and amino-functionalized microporous carbonaceous nanospheres were synthesized using waste dipping syrup with glucose, fructose, and nitrogen, which was used as precursor for hydrothermal and pyrolysis process. The products were characterized using X-ray diffraction (XRD), scanning electron microscopy (SEM), Fourier-transformed infrared spectroscopy (FTIR), the point of zero charge (PZC), Xray photoelectron spectroscopy (XPS), and Brunauer-Emmett-Teller (BET). The carbonaceous nanospheres with large BET surface area (924.528 m/g), micropores (2.127 nm), and high micro-porosity (89.54 %) allowed the rapid diffusion of SDZ (0.512nm×0.738 nm) into micropores of nanospheres. The majority SDZ (initial concentration = 20 mg/L) was removed (>96.8%) in the presence of 1.0 g/L nanoparticles after 40-min reaction at pH = 6.0. The adsorption capacity of SDZ onto nanospheres was 96.6 mg/g. The adsorption kinetic and equilibrium followed pseudo-first-order model and Langmuir isotherm, respectively. The intra-particle diffusion model indicated a three-step adsorption process. In addition, the regenerated nanospheres could be reused over four recycles. The optimal fabrication was realized at lower hydrothermal and pyrolysis temperature of 180 °C and 400 °C, respectively, which involved no additional chemical activating agent and had a high yield (70.8 %). Collectively, hydroxylation, carboxylation, amination, large specific surface area, and multi-microporosity may be responsible for improved adsorption performance of SDZ onto nanospheres. The findings provided a novel pathway for SDZ-loading wastewater treatment using waste syrup.

摘要

磺胺嘧啶(SDZ)是一种持久性的磺胺类抗生素,对人类健康具有潜在风险。废浸镀液被认为是无用的和对环境不友好的解决方案。在这项工作中,使用废浸镀液中的葡萄糖、果糖和氮源合成了羰基、羟基和氨基功能化的微孔碳质纳米球,这些物质被用作水热和热解过程的前体。使用 X 射线衍射(XRD)、扫描电子显微镜(SEM)、傅里叶变换红外光谱(FTIR)、零电荷点(PZC)、X 射线光电子能谱(XPS)和 Brunauer-Emmett-Teller(BET)对产物进行了表征。具有大 BET 表面积(924.528 m/g)、微孔(2.127 nm)和高微孔率(89.54%)的碳质纳米球允许 SDZ(0.512nm×0.738nm)快速扩散到纳米球的微孔中。在 pH = 6.0 下,反应 40 分钟后,在 1.0 g/L 纳米颗粒的存在下,大多数 SDZ(初始浓度= 20 mg/L)被去除(>96.8%)。纳米球对 SDZ 的吸附容量为 96.6 mg/g。吸附动力学和平衡分别遵循拟一级模型和朗缪尔等温线。内颗粒扩散模型表明存在三步吸附过程。此外,再生纳米球可在四个循环以上重复使用。最佳制备工艺是在较低的水热和热解温度 180°C 和 400°C 下实现的,该工艺不涉及额外的化学活化剂,产率高(70.8%)。总的来说,羟基化、羧基化、氨基化、大比表面积和多微孔可能是导致 SDZ 吸附性能提高的原因。研究结果为利用废浸镀液处理 SDZ 负载废水提供了一条新途径。

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