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通过利用从黑砂中获得的草酸亚铁进行高级氧化过程实现可见光驱动的苯酚降解:动力学研究

Visible Light-Driven Phenol Degradation via Advanced Oxidation Processes with Ferrous Oxalate Obtained from Black Sands: A Kinetics Study.

作者信息

Galeas Salomé, Guerrero Víctor H, Pontón Patricia I, Goetz Vincent

机构信息

Doctoral School Energy and Environment, University of Perpignan Via Domitia (UPVD), 52 Avenue Paul Alduy, 66100 Perpignan, France.

PROMES-CNRS UPR 8521, PROcesses Materials and Solar Energy, Rambla de la Thermodynamique, 66100 Perpignan, France.

出版信息

Molecules. 2025 May 6;30(9):2059. doi: 10.3390/molecules30092059.

DOI:10.3390/molecules30092059
PMID:40363864
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC12073611/
Abstract

Ferrous oxalate dihydrate (α-FOD) was synthesized from Ecuadorian black sands for phenol removal from aqueous solutions. Visible light-driven photodegradation kinetics were studied by varying the initial pollutant concentration, solution pH, and α-FOD dosage and by adding peroxydisulfate (PDS), including quenching tests. A representative model of phenol photodegradation was obtained by the Langmuir-Hinshelwood mechanism over a large range of concentrations (apparent kinetic constant, k = 0.524 h). Almost complete removal was reached within 1 h under dark + 9 h under visible irradiation. The degradation rate was slightly affected by pH in the range of 3 to 9, with a significant improvement at pH 11 (k = 1.41-fold higher). The optimal α-FOD dosage was ~0.5 g/L. Two regimes were observed when using PDS: first, a heterogeneous Fenton-like process during the first few minutes after PDS addition; second, pure photocatalysis to completely remove the phenol. When comparing the two systems, without and with PDS, the half-life time for pure photocatalysis was 2.5 h (after the lamp was switched on). When adding PDS (1.0 mM), the half-life time was reduced to a few minutes (5 min after PDS addition, phenol removal was 66%). The photocatalyst presented remarkable degradation efficiency up to five repeated cycles.

摘要

以厄瓜多尔黑砂为原料合成了二水合草酸亚铁(α-FOD),用于从水溶液中去除苯酚。通过改变初始污染物浓度、溶液pH值、α-FOD用量以及添加过二硫酸盐(PDS)并进行猝灭试验,研究了可见光驱动的光降解动力学。通过Langmuir-Hinshelwood机理在较大浓度范围内获得了苯酚光降解的代表性模型(表观动力学常数,k = 0.524 h)。在黑暗中1小时加上可见光照射9小时内几乎可实现完全去除。在3至9的pH范围内,降解速率受pH值的影响较小,在pH 11时显著提高(k高1.41倍)。最佳α-FOD用量约为0.5 g/L。使用PDS时观察到两种情况:第一,添加PDS后的最初几分钟内是类非均相芬顿过程;第二,是完全去除苯酚的纯光催化过程。比较有无PDS的两种体系时,纯光催化的半衰期为2.5小时(灯开启后)。添加PDS(1.0 mM)时,半衰期缩短至几分钟(添加PDS后5分钟,苯酚去除率为66%)。该光催化剂在五个重复循环中均表现出显著的降解效率。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/bc85/12073611/c7ec1c4bb063/molecules-30-02059-g008.jpg
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https://cdn.ncbi.nlm.nih.gov/pmc/blobs/bc85/12073611/f5d9717f6038/molecules-30-02059-g007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/bc85/12073611/c7ec1c4bb063/molecules-30-02059-g008.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/bc85/12073611/84903fad6d4a/molecules-30-02059-g001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/bc85/12073611/8883a6949849/molecules-30-02059-g002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/bc85/12073611/fe6ea0d1c884/molecules-30-02059-g003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/bc85/12073611/3490e34d96f3/molecules-30-02059-g004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/bc85/12073611/117673820ae9/molecules-30-02059-g005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/bc85/12073611/0b446a72394b/molecules-30-02059-g006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/bc85/12073611/f5d9717f6038/molecules-30-02059-g007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/bc85/12073611/c7ec1c4bb063/molecules-30-02059-g008.jpg

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