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1.
J Hazard Mater ; : 124203, 2020 Oct 08.
Artigo em Inglês | MEDLINE | ID: mdl-33268207

RESUMO

Plasma catalysis technology has been demonstrated to be effective for the decomposition of volatile organic compounds (VOCs). It is highly desired to explore the effect of supports on VOCs oxidation processes during plasma catalysis. In this work, four supports of SiO2, ZSM-5-300, ZSM-5-38 and γ-Al2O3 loading with transition metal oxides were used to decompose toluene at room temperature. It was found that toluene decomposition with 1 wt%Mn/γ-Al2O3 was highest, which was strongly proportional to the ozone decomposition ability of the catalyst. The plasma catalytic decomposition of toluene over 1 wt% MnO2 on different supports were characterized using in situ plasma diffuse reflectance infrared Fourier transform spectrometer. The results showed that 1 wt%Mn/γ-Al2O3 could further catalyze toluene to carbonate and bicarbonate via the breakage of C-C bonds from benzoic acid, while that was difficult for 1 wt% Mn/SiO2, 1 wt%Mn/ZSM-5-300 and 1 wt%Mn/ZSM-5-38. The reaction mechanism of toluene decomposition on different catalysts were proposed.

2.
Chemosphere ; 247: 125863, 2020 May.
Artigo em Inglês | MEDLINE | ID: mdl-31972485

RESUMO

Plasma-catalysis technologies (PCTs) have the potential to control the emissions of volatile organic compounds, although their low-energy efficiency is a bottleneck for their practical applications. A plasma-catalyst reactor filled with a CeO2/γ-Al2O3 catalyst was developed to decompose toluene with a high-energy efficiency enhanced by the elevating reaction temperature. When the reaction temperature was raised from 50 °C to 250 °C, toluene conversion dramatically increased from 45.3% to 95.5% and the energy efficiency increased from 53.5 g/kWh to 113.0 g/kWh. Conversely, the toluene conversion using a thermal catalysis technology (TCT) exhibited a maximum of 16.7%. The activation energy of toluene decomposition using PCTs is 14.0 kJ/mol, which is far lower than those of toluene decomposition using TCTs, which implies that toluene decomposition using PCT differs from that using TCT. The experimental results revealed that the Ce3+/Ce4+ ratio decreased and Oads/Olatt ratio increased after the 40-h evaluation experiment, suggesting that CeO2 promoted the formation of the reactive oxygen species that is beneficial for toluene decomposition.


Assuntos
Poluentes Atmosféricos/análise , Gases em Plasma/química , Tolueno/análise , Compostos Orgânicos Voláteis/análise , Óxido de Alumínio/química , Catálise , Cério/química , Temperatura Alta , Modelos Teóricos , Oxirredução
3.
J Hazard Mater ; 373: 698-704, 2019 Jul 05.
Artigo em Inglês | MEDLINE | ID: mdl-30959283

RESUMO

The plasma-catalytic oxidation of methane (CH4) is a potential reaction for controlling CH4 emissions at low temperatures. However, the mechanism of the CH4 plasma-catalytic oxidation is still unknown, which inhibits the further optimization of the oxidation process. Herein, a CH4 oxidation mechanism over an Au/γ-Al2O3 catalyst was proposed based on our experimental findings. CH4 is first decomposed to CH3 and H by the discharge, and a fraction of the CH3 is adsorbed on γ-Al2O3 surface for deep oxidation. The oxygen atoms produced by the discharge react with H2O to yield surface reactive OH groups that contribute to the CH3 oxidation. Oxygen atoms also promote the release of H2O from the surfaces of the γ-Al2O3 and Au/γ-Al2O3 and especially promote CO2 desorption from the surface of the Au/γ-Al2O3. When γ-Al2O3 was used as the catalyst, the CO2 selectivity was only 15 vol.%, and the CH4 conversion decreased after 7 h of plasma-catalytic oxidation. In contrast, when Au/γ-Al2O3 was used, the CO2 selectivity was 80 vol.%, long-term CH4 conversion was obtained. Experimental results revealed that Au was beneficial for the decomposition of surface carbonate species into gaseous CO2, whereas the carbonate species accumulated on γ-Al2O3 when Au was absent.

4.
J Hazard Mater ; 347: 150-159, 2018 Apr 05.
Artigo em Inglês | MEDLINE | ID: mdl-29306216

RESUMO

A dielectric barrier discharge (DBD) catalyst hybrid reactor with CeO2/γ-Al2O3 catalyst balls was investigated for benzene decomposition at atmospheric pressure and 30 °C. At an energy density of 37-40 J/L, benzene decomposition was as high as 92.5% when using the hybrid reactor with 5.0wt%CeO2/γ-Al2O3; while it was 10%-20% when using a normal DBD reactor without a catalyst. Benzene decomposition using the hybrid reactor was almost the same as that using an O3 catalyst reactor with the same CeO2/γ-Al2O3 catalyst, indicating that O3 plays a key role in the benzene decomposition. Fourier transform infrared spectroscopy analysis showed that O3 adsorption on CeO2/γ-Al2O3 promotes the production of adsorbed O2- and O22‒, which contribute benzene decomposition over heterogeneous catalysts. Nano particles as by-products (phenol and 1,4-benzoquinone) from benzene decomposition can be significantly reduced using the CeO2/γ-Al2O3 catalyst. H2O inhibits benzene decomposition; however, it improves CO2 selectivity. The deactivated CeO2/γ-Al2O3 catalyst can be regenerated by performing discharges at 100 °C and 192-204 J/L. The decomposition mechanism of benzene over CeO2/γ-Al2O3 catalyst was proposed.

5.
Environ Sci Pollut Res Int ; 24(19): 16195-16205, 2017 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-28540542

RESUMO

To reveal the seasonal variations and sources of PM2.5-bound polycyclic aromatic hydrocarbons (PAHs) during haze and non-haze episodes, daily PM2.5 samples were collected from March 2015 to February 2016 in a mixed multi-function area in Hangzhou, China. Ambient concentrations of 16 priority-controlled PAHs were determined. The sums of PM2.5-bound PAH concentrations during the haze episodes were 4.52 ± 3.32 and 13.6 ± 6.29 ng m-3 in warm and cold seasons, respectively, which were 1.99 and 1.49 times those during the non-haze episodes. Four PAH sources were identified using the positive matrix factorization model and conditional probability function, which were vehicular emissions (45%), heavy oil combustion (23%), coal and natural gas combustion (22%), and biomass combustion (10%). The four source concentrations of PAHs consistently showed higher levels in the cold season, compared with those in the warm season. Vehicular emissions were the most considerable sources that result in the increase of PM2.5-bound PAH levels during the haze episodes, and heavy oil combustion played an important role in the aggravation of haze pollution. The analysis of air mass back trajectories indicated that air mass transport had an influence on the PM2.5-bound PAH pollution, especially on the increased contributions from coal combustion and vehicular emissions in the cold season.


Assuntos
Poluentes Atmosféricos/análise , Hidrocarbonetos Policíclicos Aromáticos/análise , China , Monitoramento Ambiental , Material Particulado , Estações do Ano , Emissões de Veículos
6.
Environ Sci Pollut Res Int ; 24(1): 135-145, 2017 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-27475434

RESUMO

To investigate the characteristics of polycyclic aromatic hydrocarbons (PAHs) during haze episodes in warm seasons, daily PM2.5 and gaseous samples were collected from March to September 2015 in Hangzhou, China. Daily samples were further divided into four groups by the definition of haze according to visibility and relative humidity (RH), including non-haze (visibility, >10 km), light haze (visibility, 8-10 km, RH <90 %), medium haze (visibility, 5-8 km, RH <90 %), and heavy haze (visibility, <5 km, RH <90 %). Significantly higher concentrations of PM2.5-bound PAHs were found in haze days, but the mean PM2.5-bound PAH concentrations obviously decreased with the aggravation of haze pollution from light to heavy. The gas/particle partitioning coefficients of PAHs decreased from light-haze to heavy-haze episodes, which indicated that PM2.5-bound PAHs were restricted to adhere to the particulate phase with the aggravation of haze pollution. Absorption was considered the main mechanism of gas/particle partitioning of PAHs from gaseous to particulate phase. Analysis of air mass transport indicated that the PM2.5-bound PAH pollution in haze days was largely from regional sources but also significantly affected by long-range air mass transport. The inhalation cancer risk associated with PAHs exceeded the acceptable risk level markedly in both haze and non-haze days.


Assuntos
Poluentes Atmosféricos/análise , Hidrocarbonetos Policíclicos Aromáticos/análise , China , Monitoramento Ambiental , Temperatura Alta , Material Particulado/análise , Estações do Ano
7.
J Hazard Mater ; 161(1): 42-8, 2009 Jan 15.
Artigo em Inglês | MEDLINE | ID: mdl-18440132

RESUMO

A series of Si-doped TiO2 (Si/TiO2) photocatalysts supported on woven glass fabric were prepared by hydrothermal method for photocatalytic reduction of NO with NH3. The photocatalytic activity tests were carried out in a continuous Pyrex reactor with the flow rate of 2000mL/min under UV irradiation (luminous flux: 1.1x10(4)lm, irradiated catalyst area: 160cm2). The photocatalysts were characterized by X-ray diffraction (XRD), BET, X-ray photoelectron spectroscopy (XPS), Fourier transform infrared (FT-IR) spectrophotometer, transmission electron microscopy (TEM), photoluminescence (PL) and temperature-programmed desorption (TPD). The experiment results showed that NO conversion on Si/TiO2 at 323K could exceed 60%, which was about 50% higher than that on Degussa P25 and pure TiO2. With the doping of Si, photocatalysts with smaller crystal size, larger surface area and larger pore volume were obtained. It was also found that Ti-O-Si bands were formed on the surface of Si/TiO2 and that the surface hydroxyl concentration was greatly increased. As a result, total acidity and NH3 chemisorption amount were enhanced for Si/TiO2 leading to its photocatalytic activity improvement.


Assuntos
Óxido Nítrico/análise , Óxido Nítrico/química , Compostos de Amônio Quaternário/química , Silício/química , Temperatura , Titânio/química , Água/química , Catálise , Difusão , Microscopia Eletrônica de Transmissão , Oxirredução , Fotoquímica , Espectrofotometria , Difração de Raios X
8.
J Hazard Mater ; 162(2-3): 1249-54, 2009 Mar 15.
Artigo em Inglês | MEDLINE | ID: mdl-18650000

RESUMO

Catalysts based on MnO(x)/TiO(2) were prepared by sol-gel, impregnation, and coprecipitation methods for low-temperature selective catalytic reduction (SCR) of NO with NH(3). Among the catalysts, the sample prepared by sol-gel method had the best performance on both activity and SO(2) resistance. From the results of thermo gravimetric analysis (TGA), X-ray diffraction (XRD), transmission electron microscopy (TEM) and X-ray photoelectron spectrum (XPS), it was known that manganese oxides and titania existed in different phase in the samples prepared by three methods. Strong interaction, large surface area, high concentration of hydroxyl groups, high concentration of amorphous Mn on the surface might be the main reasons for the excellent performance of the catalysts.


Assuntos
Temperatura Baixa , Compostos de Manganês/química , Óxido Nítrico/química , Óxidos/química , Titânio/química , Catálise , Microscopia Eletrônica de Transmissão , Oxirredução , Difração de Raios X
9.
Environ Sci Technol ; 41(16): 5812-7, 2007 Aug 15.
Artigo em Inglês | MEDLINE | ID: mdl-17874791

RESUMO

Manganese oxides and iron-manganese oxides supported on TiO2 were prepared by the sol-gel method and used for low-temperature selective catalytic reduction (SCR) of NO with NH3. Base on the previous study, Mn(0.4)/ TiO2 and Fe(0.1)-Mn(0.4)/TiO2 were then selected to carry out the in situ diffuse reflectance infrared transform spectroscopy (DRIFT) investigation for revealing the reaction mechanism. The DRIFT spectroscopy for the adsorption of NH3 indicated the presence of coordinated NH3 and NH4+ on both of the two catalysts. When NO was introduced, the coordinated NH3 on the catalyst surface was consumed rapidly, indicating these species could react with NO effectively. When NH3 was introduced into the sample preadsorbed with NO + O2, SCR reaction would not proceed on Mn(0.4)/TiO2. However, for Fe(0.1)-Mn(0.4)/ TiO2 the bands due to coordinated NH3 on Fe2O3 were formed. Simultaneously, the bidentate nitrates were transformed to monodentate nitrates and NH4+ was detected. And NO2 from the oxidation of NO on catalyst could react with NH4+ leading to the reduction of NO. Therefore, it was suggested that the SCR reaction on Fe(0.1)-Mn(0.4)/TiO2 could also take place in a different way from the reactions on Mn(0.4)/TiO2 proposed by other researchers. Furthermore, the SCR reaction steps for these two kinds of catalysts were proposed.


Assuntos
Amônia/química , Manganês/química , Óxido Nítrico/química , Espectrofotometria Infravermelho/métodos , Temperatura , Titânio/química , Adsorção , Catálise , Oxirredução
10.
J Hazard Mater ; 145(3): 488-94, 2007 Jul 16.
Artigo em Inglês | MEDLINE | ID: mdl-17188430

RESUMO

A catalyst based on MnO(x)/TiO(2) was prepared by sol-gel method for low-temperature selective catalytic reduction (SCR) of NO with NH(3). Focusing on the effects of the operating parameters, the SCR reaction was investigated at temperatures from 353 to 523K under steady and transient states. Under the optimal conditions, the efficiency of NO removal could exceed 90% at temperature of 423K. Furthermore, within the range investigated, the reaction order of NO, NH(3), O(2) was determined to be 1, 0, and 0.5, respectively. Apparent activation energy was also calculated to be 38kJ/mol, lower than that for most of the catalysts reported by previous investigations.


Assuntos
Amônia/química , Óxido de Magnésio/química , Óxido Nítrico/química , Titânio/química , Catálise , Géis , Oxirredução , Soluções , Temperatura
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