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1.
J Environ Sci (China) ; 134: 55-64, 2023 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-37673533

RESUMO

Vacuum ultraviolet (VUV) photolysis is a facile method for volatile organic compounds (VOCs) elimination, but is greatly limited by the relatively low removal efficiency and the possible secondary pollution. To overcome above drawbacks, we developed an efficient method for VOCs elimination via VUV photolysis coupled with wet scrubbing process. In this coupled process, volatile toluene, a representative of VOCs, was oxidized by the gas-phase VUV photolysis, and then scrubbed into water for further oxidation by the liquid-phase VUV photolysis. More than 96% of toluene was efficiently removed by this coupled process, which was 2 times higher than that in the gas-phase VUV photolysis. This improvement was attributed to the synergistic effect between gas-phase and liquid-phase VUV photolysis. O3 and HO• are the predomination reactive species for the toluene degradation in this coupled process, and the generation of O3 in gas-phase VUV photolysis can efficiently enhance the HO• production in liquid-phase VUV photolysis. The result from in-situ proton transfer reaction ionization with mass analyzer (PTR-MS) further suggested that most intermediates were trapped by the wet scrubbing process and efficiently oxidized by the liquid-phase VUV photolysis, showing a high performance for controlling the secondary pollution. Furthermore, the result of stability test and the reuse of solution demonstrated that this coupled process has a highly stable and sustainable performance for toluene degradation. This study presents an environmentally benign and highly efficient VUV photolysis for gaseous VOCs removal in the wet scrubbing process.


Assuntos
Compostos Orgânicos Voláteis , Fotólise , Vácuo , Oxirredução , Gases , Tolueno
2.
Chemosphere ; 309(Pt 2): 136656, 2022 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-36191768

RESUMO

The elimination of volatile organic compounds (VOCs) via vacuum ultraviolet (VUV) photolysis is greatly limited by low removal efficiency and gaseous byproducts generation, while photocatalytic oxidation of VOCs suffers from catalytic deactivation. Herein, a coupled process of gaseous VUV photolysis with aqueous photocatalytic oxidation with P25 as the catalyst was firstly proposed for efficient aromatic VOCs removal (VUV/P25). The removal efficiency of toluene reached 86.2% in VUV/P25 process, but was only 33.6% and 58.1% in alone gaseous VUV photolysis and aqueous ultraviolet photocatalytic oxidation (UV/P25) process, respectively. Correspondingly, the outlet CO2 concentration in VUV/P25 process reached 132 ppmv. Toluene was firstly destructed by high-energy photons generated from gaseous VUV photolysis, resulting in its incomplete oxidation to form soluble intermediates including acids, aldehydes, esters. These soluble intermediates would be further degraded and mineralized into CO2 in subsequent aqueous UV/P25 process. Notably, the concentrations of intermediates in VUV/P25 were much lower than those in VUV photolysis, indicating the synergy effect of VUV photolysis and UV/P25 process. The stability tests proved that VUV/P25 process maintained an excellent toluene degradation performance and P25 did not suffer from catalytic deactivation. In addition to toluene, the VUV/P25 system also achieved the efficient and sustainable degradation of styrene and chlorobenzene, suggesting its good application prospect in industrial VOCs treatment. This study proposes an efficient and promising strategy for deep oxidation of multiple aromatic VOCs in industries.


Assuntos
Compostos Orgânicos Voláteis , Fotólise , Vácuo , Dióxido de Carbono , Raios Ultravioleta , Tolueno/análise , Oxirredução , Gases , Água , Clorobenzenos , Aldeídos , Estirenos
3.
Chemosphere ; 263: 128089, 2021 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-33297087

RESUMO

We investigated the adsorption mechanisms for removing fluoride based on experimental and modeling studies. Lanthanum-aluminum perovskite was designed for treating wastewater contaminated by fluoride. A fluorine-species model was developed to calculate the concentrations of different species of fluorine: F-, HF, HF2-. Multiple kinetic models were examined and the pseudo-second order model was found the best to fit the experimental data, implying fast-chemisorption. The thermodynamic data were fitted by the Langmuir model and Freundlich model at different temperatures, indicating heterogeneous adsorption at low temperature and homogeneous adsorption at high temperature. The La2Al4O9 material had less influence from negative ions when adsorbing fluoride. The adsorption mechanisms were further studied using experiments and Density Functional Theory calculations. The adsorption experiments could be attributed to the lattice plane (1 2 1) and La, O, Al sites. More Al sites were required than La sites for the increase of fluoride concentration. By contrast, more La sites than Al sites were needed for increased pH.


Assuntos
Poluentes Químicos da Água , Purificação da Água , Adsorção , Alumínio , Compostos de Cálcio , Fluoretos , Concentração de Íons de Hidrogênio , Cinética , Lantânio , Óxidos , Termodinâmica , Titânio
4.
Chemosphere ; 244: 125567, 2020 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-31837565

RESUMO

Toluene is a representative and toxic contaminant in industry or indoor airs. In this work, a novel and facile method was developed to prepare mesoporous TiO2 for the photo-catalytic oxidation of toluene in a wet-scrubbing reactor. Interestingly, by changing the preparation parameters, including dosage of template material, hydrolysis rate, hydrothermal temperature and calcination temperature, the crystalline phase of catalyst could be partially adjusted among brookite, anatase and rutile. With 30 ppm toluene input, an enhanced toluene removal of 62% and CO2 production of 95 ppm were achieved, while no soluble or particulate byproduct was released. In contrast to traditional photo-catalysis, the UV adsorbing ability of catalyst, the cluster of mesoporous TiO2 and the corresponding structure in micrometer-scale were key to the UV utilization and toluene removal in wet-scrubbing reactor.


Assuntos
Modelos Químicos , Titânio/química , Tolueno/química , Adsorção , Catálise , Oxirredução , Raios Ultravioleta
5.
Chemosphere ; 227: 401-408, 2019 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-31003124

RESUMO

The traditional treatment processes for volatile organic compounds (VOCs) removal generally suffered several disadvantages, such as secondary air-pollutants. To overcome these issues, wet scrubber coupled with heterogeneous UV/Fenton was developed for gaseous VOCs (i.e. toluene) removal. ZSM-5 supported iron oxide (Fe/ZSM-5) was prepared as a multifunctional catalyst for activation of H2O2 and enhancement of gas-liquid mass transfer. Toluene was removed efficiently by this coupled process with the removal efficiency of 85% during 120 min. Many intermediates were detected in the solution by GC-MS while no intermediates were observed in the outlet gas, suggesting that wet scrubber coupled with heterogeneous UV/Fenton could significantly reduce secondary air pollutants. The possible mechanism of toluene oxidation was proposed including the physical adsorption by Fe/ZSM-5 and OH oxidation. This study provides an environmentally benign and highly efficient chemical scrubbing process for gaseous VOCs removal.


Assuntos
Filtros de Ar , Poluentes Atmosféricos/química , Compostos Orgânicos Voláteis/química , Adsorção , Poluentes Atmosféricos/análise , Catálise , Gases , Peróxido de Hidrogênio/química , Ferro/química , Oxirredução , Tolueno/química , Raios Ultravioleta
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