Efficient tetracycline degradation via flow-through peroxymonosulfate activation by dual heteroatom-doped wood-derived catalytic membrane

IF 7.4 2区 工程技术 Q1 ENGINEERING, CHEMICAL
Li Zhao , Zifeng Qiu , Hong Ma , Ruiying Zhu , Xiaofang Pan , Xiaochun Wu , Xiaobo Gong
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Abstract

The widespread use of antibiotics in the medical industry and in animal husbandry has led to significant environmental pollution. Effective purification of high concentrations of tetracycline (TC) in practical pharmaceutical wastewater remains a substantial challenge. The integration of advanced oxidation with membrane separation technology shows great application potential. In this study, a P and N co-doped balsa wood membrane (PNWM) were fabricated using heteroatomic doped biochar material, aiming to synergize filtration and catalytic oxidation. The catalytic activity of the PNWM/peroxymonosulfate (PMS) system was systematically evaluated. Targeting TC as the pollutant, the PNWM/PMS system achieved a degradation efficiency exceeding 97 % within 30 min and a total organic carbon (TOC) removal efficiency of 63.9 %, surpassing the performance of unmodified wood-based membrane. These excellent results were attributed to the doping of N and P atoms, which increased surface defects and specific area, thereby enhancing the adsorption and degradation of TC by PNWM. The graphite N facilitated electron transfer, while pyridine N served as active sites for PMS activation. Additionally, the low electronegativity of the P formed electronic regions of varying intensities on the PNWM surface, contributing to PMS activation. The membrane process also enhanced mass transfer during the degradation process. Both radical (·OH, SO4·ˉ, O2·ˉ) and non-radical (1O2, electron transfer) pathways cooperated in TC degradation in PNWM/PMS system. Consequently, heteroatom-doped biochar film materials prepared through simple methods provide a promising approach for the effective treatment of refractory organic pollutants in wastewater.

双杂原子掺杂木质催化膜通过流动过硫酸盐活化高效降解四环素
抗生素在医疗行业和畜牧业中的广泛使用导致了严重的环境污染。有效净化实际制药废水中的高浓度四环素(TC)仍然是一项巨大的挑战。高级氧化与膜分离技术的结合显示出巨大的应用潜力。本研究利用异原子掺杂的生物炭材料制作了一种 P 和 N 共掺杂的轻木膜(PNWM),旨在实现过滤和催化氧化的协同作用。系统评估了 PNWM/过氧单硫酸盐(PMS)的催化活性。以三氯甲烷为污染物,PNWM/PMS 系统在 30 分钟内的降解效率超过 97%,总有机碳(TOC)去除率达到 63.9%,超过了未改性木基膜的性能。这些优异的结果归功于 N 原子和 P 原子的掺杂,它们增加了表面缺陷和比面积,从而提高了 PNWM 对 TC 的吸附和降解能力。石墨 N 促进了电子转移,而吡啶 N 则成为 PMS 活化的活性位点。此外,P 的低电负性在 PNWM 表面形成了不同强度的电子区域,有助于 PMS 的活化。膜过程还增强了降解过程中的质量转移。在 PNWM/PMS 系统中,自由基(-OH、SO4-ˉ、O2-ˉ)和非自由基(1O2、电子传递)途径在 TC 降解过程中都起到了作用。因此,通过简单方法制备的掺杂杂原子的生物炭薄膜材料为有效处理废水中的难降解有机污染物提供了一种可行的方法。
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来源期刊
Journal of Environmental Chemical Engineering
Journal of Environmental Chemical Engineering Environmental Science-Pollution
CiteScore
11.40
自引率
6.50%
发文量
2017
审稿时长
27 days
期刊介绍: The Journal of Environmental Chemical Engineering (JECE) serves as a platform for the dissemination of original and innovative research focusing on the advancement of environmentally-friendly, sustainable technologies. JECE emphasizes the transition towards a carbon-neutral circular economy and a self-sufficient bio-based economy. Topics covered include soil, water, wastewater, and air decontamination; pollution monitoring, prevention, and control; advanced analytics, sensors, impact and risk assessment methodologies in environmental chemical engineering; resource recovery (water, nutrients, materials, energy); industrial ecology; valorization of waste streams; waste management (including e-waste); climate-water-energy-food nexus; novel materials for environmental, chemical, and energy applications; sustainability and environmental safety; water digitalization, water data science, and machine learning; process integration and intensification; recent developments in green chemistry for synthesis, catalysis, and energy; and original research on contaminants of emerging concern, persistent chemicals, and priority substances, including microplastics, nanoplastics, nanomaterials, micropollutants, antimicrobial resistance genes, and emerging pathogens (viruses, bacteria, parasites) of environmental significance.
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