Centro de Recursos Naturais e Ambiente (CERENA), Chemical Engineering Department, Instituto Superior Técnico, University of Lisbon, Av. Rovisco Pais, 1049-001 Lisbon, Portugal.
Centro de Desenvolvimento de Produto e Transferência de Tecnologia (CDP2T), Escola Superior de Tecnologia de Setúbal, Instituto Politécnico de Setúbal, 2910-761 Setúbal, Portugal.
Int J Mol Sci. 2024 May 29;25(11):5958. doi: 10.3390/ijms25115958.
Advanced oxidation processes, including photocatalysis, have been proven effective at organic dye degradation. Tailored porous materials with regulated pore size, shape, and morphology offer a sustainable solution to the water pollution problem by acting as support materials to grafted photocatalytic nanoparticles (NPs). This research investigated the influence of pore and particle sizes of photocatalytic MICROSCAFS on the degradation of methyl orange (MO) in aqueous solution (10 mg/L). Photocatalytic MICROSCAFS are made of binder-less supported P25 TiO NPs within MICROSCAFS, which are silica-titania microspheres with a controlled size and interconnected macroporosity, synthesized by an adapted sol-gel method that involves a polymerization-induced phase separation process. Photocatalytic experiments were performed both in batch and flow reactors, with this latter one targeting a proof of concept for continuous transformation processes and real-life conditions. Photocatalytic degradation of 87% in 2 h (batch) was achieved, using a calibrated solar light simulator (1 sun) and a photocatalyst/pollutant mass ratio of 23. This study introduces a novel flow kinetic model which provides the modeling and simulation of the photocatalytic MICROSCAFS performance. A scavenger study was performed, enabling an in-depth mechanistic understanding. Finally, the transformation products resulting from the MO photocatalytic degradation were elucidated by high-resolution mass spectrometry experiments and subjected to an in silico toxicity assessment.
高级氧化工艺,包括光催化,已被证明在有机染料降解方面非常有效。定制的多孔材料具有可调节的孔径、形状和形态,可作为接枝光催化纳米颗粒 (NPs) 的支撑材料,为水污染问题提供可持续的解决方案。本研究考察了光催化 MICROSCAFS 的孔和颗粒尺寸对水溶液中甲基橙 (MO) 降解的影响(10mg/L)。光催化 MICROSCAFS 由 MICROSCAFS 内无粘结剂支撑的 P25 TiO2 NPs 组成,这些 NPs 是二氧化硅-二氧化钛微球,具有受控的尺寸和互连通孔性,通过一种经过改进的溶胶-凝胶法合成,该方法涉及聚合诱导相分离过程。在批处理和流动反应器中进行了光催化实验,后者旨在证明连续转化过程和实际条件的概念验证。使用校准的太阳模拟器(1 个太阳)和光催化剂/污染物质量比为 23,在 2 小时内实现了 87%的光催化降解。本研究引入了一种新的流动动力学模型,该模型提供了光催化 MICROSCAFS 性能的建模和模拟。进行了清除剂研究,实现了深入的机理理解。最后,通过高分辨率质谱实验阐明了 MO 光催化降解产生的转化产物,并对其进行了计算机毒性评估。