Insights into novel phosphorus-doped biochar for tetracycline removal: Non-radical oxidation and adsorption

IF 7.4 2区 工程技术 Q1 ENGINEERING, CHEMICAL Journal of Environmental Chemical Engineering Pub Date : 2024-09-23 DOI:10.1016/j.jece.2024.114224
Xi Fu , Xiaojun Niu , Dongqing Zhang , Ling Li , Xingyao Ye , Shan Liao , Maoyu Li , Chuting Lao , Deye Chen , Yu Lin , Zhiquan Yang
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Abstract

Heteroatom doping has been widely recognized as an emerging and promising strategy for material enhancement and the degradation of organic pollutants. However, most heteroatom doping biochars are used to activate, for example, PMS to generate reactive oxygen species (ROS) to degrade organic pollutants instead of investigating their own ability to produce ROS. Herein, phosphorus-doping biochars (PBC) were synthesized at various temperatures for adsorption and degradation of tetracycline (TC). Compared to the pristine biochar (BC-800), PBC-800 exhibited significant enhancements in the specific surface areas (1307.30 m2·g−1), porosity (0.94 cm3·g−1) and higher removal efficiency (1.25 times higher than BC-800). The abundance of functional groups in the PBC-800 such as electron-rich ketone functional groups (CO), phosphorus-oxygen moieties (P-O), and defective sites within the carbon matrix, have been identified to play crucial roles in TC degradation. The free radical quenching and analysis of electron paramagnetic resonance (EPR) indicated that the presence of persistent free radicals (PFRs) on PBC also influenced the TC removal, and the possible non-radical pathways were proposed. The density functional theory (DFT) calculations proved that PBC-800 exhibited the highest adsorption energy as well as the lowest energy gap between triplet O2 and 1O2, suggesting that the existence of P was conducive to the production of 1O2. This study laid the groundwork for the development of biochars and provided a novel insight into the design of green biomass for effective removal of antibiotics in the future.
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新型掺磷生物炭去除四环素的见解:非自由基氧化和吸附
人们普遍认为,掺杂杂原子是一种新兴的、有前途的材料增强和有机污染物降解策略。然而,大多数掺杂杂原子的生物炭都是用来激活 PMS 等产生活性氧(ROS)以降解有机污染物,而不是研究其自身产生 ROS 的能力。本文在不同温度下合成了掺磷生物炭(PBC),用于吸附和降解四环素(TC)。与原始生物炭(BC-800)相比,PBC-800 在比表面积(1307.30 m2-g-1)、孔隙率(0.94 cm3-g-1)和去除效率(比 BC-800 高 1.25 倍)方面都有显著提高。PBC-800 中丰富的官能团,如电子丰富的酮官能团 (CO)、磷氧分子 (P-O) 和碳基质中的缺陷位点,已被确认在 TC 降解中发挥了关键作用。自由基淬灭和电子顺磁共振(EPR)分析表明,PBC 上持久自由基(PFR)的存在也会影响 TC 的去除,并提出了可能的非自由基途径。密度泛函理论(DFT)计算证明,PBC-800 表现出最高的吸附能以及三重 O2 和 1O2 之间最低的能隙,这表明 P 的存在有利于 1O2 的产生。这项研究为生物炭的开发奠定了基础,并为今后设计有效去除抗生素的绿色生物质提供了新的见解。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
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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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