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竹基氮掺杂磁性多孔水凝胶协同 KFeO 和 CaCO 活化去除苯酚:影响因素与机制。

Bamboo-derived nitrogen-doping magnetic porous hydrochar coactivated by KFeO and CaCO for phenol removal: Governing factors and mechanisms.

机构信息

National Joint Engineering Research Center for Highly-Efficient Utilization Technology of Forest Biomass Resources, College of Materials & Chemical Engineering, Southwest Forestry University, Kunming, 650224, PR China.

Xiamen Key Laboratory for High-valued Conversion Technology of Agricultural Biomass (Xiamen University), Fujian Provincial Engineering and Research Center of Clean and High-valued Technologies for Biomass, College of Energy, Xiamen University, Xiamen, 361102, PR China.

出版信息

Environ Pollut. 2023 Aug 15;331(Pt 1):121871. doi: 10.1016/j.envpol.2023.121871. Epub 2023 May 22.

Abstract

In this study, a novel nitrogen-doped magnetic Fe-Ca codoped biochar for phenol removal was successfully fabricated via a hydrothermal and coactivation pyrolysis method. A series of adsorption process parameters (KFeO to CaCO ratio, initial phenol concentration, pH value, adsorption time, adsorbent dosage and ion strength) and adsorption models (kinetic models, isotherms and thermodynamic models) were determined using batch experiments and various analysis techniques (XRD, BET, SEM-EDX, Raman spectroscopy, VSM, FTIR and XPS) to investigate the adsorption mechanism and metal-nitrogen-carbon interaction. The biochar with a ratio of Biochar: KFeO: CaCO = 3:1:1 exhibited superior properties for adsorption of phenol and had a maximum adsorption capacity of 211.73 mg/g at 298 K, C = 200 mg/L, pH = 6.0 and t = 480 min. These excellent adsorption properties were due to superior physicomechanical properties (a large specific surface area (610.53 m/g) and pore volume (0.3950 cm/g), a well-developed pore structure (hierarchical), a high graphitization degree (I/I = 2.02), the presence of O/N-rich functional groups and Fe-Ox,Ca-Ox, N-doping, as well as synergistic activation by KFeO and CaCO). The Freundlich and pseudo-second-order models effectively fit the adsorption data, indicating multilayer physicochemical adsorption. Pore filling and π-π interactions were the predominant mechanisms for phenol removal, and H-bonding interactions, Lewis-acid-base interactions, and metal complexation played an important role in enhancing phenol removal. A simple, feasible approach with application potential to organic contaminant/pollutant removal was developed in this study.

摘要

在这项研究中,通过水热和共活化热解方法成功制备了一种用于去除苯酚的新型氮掺杂磁性 Fe-Ca 共掺杂生物炭。通过批量实验和各种分析技术(XRD、BET、SEM-EDX、拉曼光谱、VSM、FTIR 和 XPS)确定了一系列吸附过程参数(KFeO 与 CaCO 的比例、初始苯酚浓度、pH 值、吸附时间、吸附剂用量和离子强度)和吸附模型(动力学模型、等温线和热力学模型),以研究吸附机制和金属-氮-碳相互作用。在 298 K、C = 200 mg/L、pH = 6.0 和 t = 480 min 时,Biochar:KFeO:CaCO = 3:1:1 的比例下的生物炭对苯酚的吸附性能优越,最大吸附容量为 211.73 mg/g。这些优异的吸附性能归因于优越的物理机械性能(大的比表面积(610.53 m2/g)和孔体积(0.3950 cm3/g)、发达的孔结构(分级)、高石墨化程度(I/I = 2.02)、存在富 O/N 的官能团和 Fe-Ox、Ca-Ox、N 掺杂以及 KFeO 和 CaCO 的协同活化)。Freundlich 和准二级模型有效地拟合了吸附数据,表明是多层物理化学吸附。孔填充和π-π相互作用是去除苯酚的主要机制,氢键相互作用、路易斯酸碱相互作用和金属络合在增强苯酚去除方面起着重要作用。本研究开发了一种具有应用潜力的去除有机污染物/污染物的简单、可行的方法。

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