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在自然 pH 条件下,通过光芬顿降解对乙酰氨基酚时考虑到明确的辐射吸收效应的反应动力学公式。

Reaction kinetics formulation with explicit radiation absorption effects of the photo-Fenton degradation of paracetamol under natural pH conditions.

机构信息

Instituto de Desarrollo Tecnológico para la Industria Química (INTEC), Consejo Nacional de Investigaciones Científicas y Técnicas (CONICET) and Universidad Nacional del Litoral (UNL), Ruta Nacional N° 168, 3000, Santa Fe, Argentina.

出版信息

Environ Sci Pollut Res Int. 2021 May;28(19):23946-23957. doi: 10.1007/s11356-020-11993-5. Epub 2021 Jan 4.

Abstract

The degradation of paracetamol (PCT) in an aqueous medium using the Fenton and photo-Fenton reactions was investigated. The aim of this research was the development of a kinetic model based on a reaction mechanism, which includes two main intermediates of PCT degradation and the local volumetric rate of photon absorption (LVRPA). Ferrioxalate was used as a catalyst and the working pH was adjusted to 5.5 (natural pH). Experimental work was planned through a D-optimal experimental design and performed in a flat plate reactor irradiated by a solar simulator. Hydrogen peroxide (HP) concentration, reaction temperature, and radiation level were the operating parameters. The photo-Fenton reaction allowed to reach a minimum relative PCT concentration of 2.01% compared to 5.04% achieved with Fenton reaction. Moreover, the photo-Fenton system required a 50% shorter reaction time and lower HP concentration than in dark conditions (90 min and 189 mg L vs. 180 min and 334 mg L, respectively). The experimental results were used to estimate the kinetic parameters of the proposed kinetic model employing a nonlinear, multi-parameter regression method. The values obtained from the normalized root-mean-square error (14.52, 1.96, 4.36, 13.16, and 8.72 % for PCT, benzoquinone, hydroquinone, HP, and oxalate, respectively) showed a good agreement between the predicted and experimental data.

摘要

采用芬顿和光芬顿反应研究了在水介质中对扑热息痛(PCT)的降解。本研究的目的是开发一种基于反应机制的动力学模型,该模型包括 PCT 降解的两个主要中间体和局部光子吸收体积速率(LVRPA)。使用草酸盐作为催化剂,工作 pH 值调整为 5.5(自然 pH 值)。通过 D-最优实验设计规划实验工作,并在太阳能模拟器照射的平板反应器中进行。过氧化氢(HP)浓度、反应温度和辐射水平是操作参数。与芬顿反应相比,光芬顿反应可使相对 PCT 浓度达到最低,为 2.01%,而光芬顿反应仅为 5.04%。此外,光芬顿体系所需的 HP 浓度和反应时间比暗条件下分别短 50%和低 334 mg/L(90 min 和 189 mg/L)。实验结果用于通过非线性、多参数回归方法估计所提出的动力学模型的动力学参数。归一化均方根误差(14.52%、1.96%、4.36%、13.16%和 8.72%,分别为 PCT、苯醌、对苯二酚、HP 和草酸盐)的值表明预测数据与实验数据之间具有良好的一致性。

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