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1.
Waste Manag ; 182: 63-73, 2024 Jun 15.
Article En | MEDLINE | ID: mdl-38640752

The incineration bottom ash (IBA) was impregnated with nickel to catalyze toluene (tar surrogate) steam reforming. A toluene conversion of >80 % was achieved at 800℃ without activity decay in a 100-h test for 15 %Ni/IBA. An activation stage was observed for Ni/IBA catalysts in the initial 50 âˆ¼ 400 min under different reaction conditions. A series of experiments and characterizations were performed to explore the possible mechanisms for the activation. It was found that the iron species in IBA gradually migrated to the catalyst surface and formed a Ni-FeOx complex owing to the metal-support interaction. The synergy of Ni-FeOx played an important role in improving the activity of Ni/IBA due to the enhanced lattice oxygen activity. Additionally, Ni/IBA catalysts showed a much lower coke deposition rate than Ni/Al2O3 (1.12 vs. 3.45 mg-C/gcat∙h) because of the variable states of FeOx and the abundant basic sites caused by the alkali and alkaline earth metals contained in IBA.


Ferric Compounds , Incineration , Nickel , Nickel/chemistry , Catalysis , Ferric Compounds/chemistry , Incineration/methods , Toluene/chemistry , Coal Ash/chemistry
2.
Environ Sci Technol ; 58(17): 7662-7671, 2024 Apr 30.
Article En | MEDLINE | ID: mdl-38578018

Photothermal catalysis is extremely promising for the removal of various indoor pollutants owing to its photothermal synergistic effect, while the low light utilization efficiency and unclear catalytic synergistic mechanism hinder its practical applications. Here, nitrogen atoms are introduced, and Pt nanoparticles are loaded on TiO2 to construct Pt/N-TiO2-H2, which exhibits 3.5-fold higher toluene conversion rate than the pure TiO2. Compared to both photocatalytic and thermocatalytic processes, Pt/N-TiO2-H2 exhibited remarkable performance and stability in the photothermocatalytic oxidation of toluene, achieving 98.4% conversion and 98.3% CO2 yield under a light intensity of 260 mW cm-2. Furthermore, Pt/N-TiO2-H2 demonstrated potential practical applicability in the photothermocatalytic elimination of various indoor volatile organic compounds. The synergistic effect occurs as thermocatalysis accelerates the accumulation of carboxylate species and the degradation of aldehyde species, while photocatalysis promotes the generation of aldehyde species and the consumption of carboxylate species. This ultimately enhances the photothermocatalytic process. The photothermal synergistic effect involves the specific conversion of intermediates through the interplay of light and heat, providing novel insights for the design of photothermocatalytic materials and the understanding of photothermal mechanisms.


Oxidation-Reduction , Toluene , Catalysis , Toluene/chemistry , Hot Temperature , Light , Titanium/chemistry , Platinum/chemistry , Volatile Organic Compounds/chemistry
3.
Environ Sci Technol ; 58(11): 5153-5161, 2024 Mar 19.
Article En | MEDLINE | ID: mdl-38456428

Photothermal catalysis exhibits promising prospects to overcome the shortcomings of high-energy consumption of traditional thermal catalysis and the low efficiency of photocatalysis. However, there is still a challenge to develop catalysts with outstanding light absorption capability and photothermal conversion efficiency for the degradation of atmospheric pollutants. Herein, we introduced the Co3O4 layer and Pt nanoclusters into the three-dimensional (3D) porous membrane through the atomic layer deposition (ALD) technique, leading to a Pt/Co3O4/AAO monolithic catalyst. The 3D ordered nanochannel structure can significantly enhance the solar absorption capacity through the light-trapping effect. Therefore, the embedded Pt/Co3O4 catalyst can be rapidly heated and the O2 adsorbed on the Pt clusters can be activated to generate sufficient O2- species, exhibiting outstanding activity for the diverse VOCs (toluene, acetone, and formaldehyde) degradation. Optical characterization and simulation calculation confirmed that Pt/Co3O4/AAO exhibited state-of-the-art light absorption and a notable localized surface plasmon resonance (LSPR) effect. In situ diffuse reflectance infrared Fourier transform spectrometry (in situ DRIFTS) studies demonstrated that light irradiation can accelerate the conversion of intermediates during toluene and acetone oxidation, thereby inhibiting byproduct accumulation. Our finding extends the application of AAO's optical properties in photothermal catalytic degradation of air pollutants.


Acetone , Cobalt , Oxides , Toluene , Oxidation-Reduction , Catalysis , Toluene/analysis , Toluene/chemistry
4.
J UOEH ; 46(1): 9-16, 2024.
Article En | MEDLINE | ID: mdl-38479880

This study investigated the permeation resistance of chemical protective gloves made of laminate film comprising nylon, ethylene-vinyl alcohol copolymer (EVOH), and other materials against different chemical substances to examine their usability in different work processes. The permeation resistance of the chemical protective glove was tested using the Japanese Industrial Standards (JIS) test method against twelve substances: acetone, acetonitrile, dichloromethane, ethyl acetate, n-hexane, methanol, tetrahydrofuran, toluene, 2-propanol, 1-butanol, 1,4-diethylene dioxide, and ethanol. After 480 min, no substance, except for methanol and ethanol, permeated at a standard permeation rate of 0.1 µg/cm2/min. Methanol and ethanol showed permeation at 1 min and 30 min elapsed, respectively. Hence, the gloves tested in this study exhibited permeation resistance to various chemical substances, and can thus be used in many work processes. Some film materials have short permeation time against certain chemical substances, but the chemical protective gloves tested in this study can be used at work sites, such as manufacturing sites, that require permeation resistance to different chemical substances.


Gloves, Protective , Occupational Exposure , Methanol , Ethanol/chemistry , Acetone/chemistry , Toluene/chemistry
5.
Chemosphere ; 352: 141346, 2024 Mar.
Article En | MEDLINE | ID: mdl-38311035

Doping proves to be an efficacious method of establishing intermetallic interactions for enhancing toluene oxidation performance of bimetallic oxides. However, conventional bimetallic oxide catalysts are yet to overcome their inadequacy in establishing intermetallic interactions. In this work, the dispersion of Mn-Co bimetallic sites was improved by hydrolytic co-precipitation, strengthening the intermetallic interactions which improved the structural and physicochemical properties of the catalysts, thus significantly enhancing its catalytic behavior. MnCo-H catalysts fabricated by the hydrolytic co-precipitation method showed promising catalytic performance (T50 = 223 °C, T90 = 229 °C), robust stability (at least 100 h) and impressive water resistance (under 10 vol.% of water) for toluene elimination. Hydrolytic co-precipitation has been found to improve dispersion of MnCo elements and to enhance interaction between Co and Mn ions (Mn4+ + Co2+ = Mn3+ + Co3+), resulting in a lower reduction temperature (215 °C) and a weaker Mn-O bond strength, creating more lattice defects and oxygen vacancies, which are responsible for superior catalytic properties of MnCo-H samples. Furthermore, in situ DRIFTs showed that gaseous toluene molecules adsorbed on the surface of MnCo-H were continuously oxidized to benzyl alcohol → benzaldehyde → benzoate, followed by a ring-opening reaction with surface-activated oxygen to convert to maleic anhydride as the final intermediate, which further generates water and carbon dioxide. It was also revealed that the ring-opening reaction for the conversion of benzoic acid to maleic anhydride is the rate-controlling step. This study reveals that optimizing active sites and improving reactive oxygen species by altering the dispersion of bimetals to enhance bimetallic interactions is an effective strategy for the improvement of catalytic behavior, while the hydrolytic co-precipitation method fits well with this corollary.


Manganese Compounds , Manganese , Nitrosourea Compounds , Toluene , Manganese/chemistry , Oxidation-Reduction , Toluene/chemistry , Maleic Anhydrides , Oxides/chemistry , Water , Cobalt/chemistry , Oxygen/chemistry , Catalysis
6.
Environ Sci Technol ; 58(9): 4428-4437, 2024 Mar 05.
Article En | MEDLINE | ID: mdl-38400916

The adsorption and activation of pollutant molecules and oxygen play a critical role in the oxidation reaction of volatile organic compounds (VOCs). In this study, superior adsorption and activation ability was achieved by modulating the interaction between Pt nanoparticles (NPs) and UiO-66 (U6) through the spatial position effect. Pt@U6 exhibits excellent activity in toluene, acetone, propane, and aldehyde oxidation reactions. Spectroscopic studies, 16O2/18O2 kinetic isotopic experiments, and density functional theory (DFT) results jointly reveal that the encapsulated Pt NPs of Pt@U6 possess higher electron density and d-band center, which is conducive for the adsorption and dissociation of oxygen. The toluene oxidation reaction and DFT results indicate that Pt@U6 is more favorable to activate the C-H of toluene and the C═C of maleic anhydride, while Pt/U6 with lower electron density and d-band center exhibits a higher oxygen dissociation temperature and higher reactant activation energy barriers. This study provides a deep insight into the architecture-performance relation of Pt-based catalysts for the catalytic oxidation of VOCs.


Metal-Organic Frameworks , Nanoparticles , Phthalic Acids , Volatile Organic Compounds , Volatile Organic Compounds/chemistry , Toluene/chemistry , Oxygen
7.
Chemosphere ; 351: 141197, 2024 Mar.
Article En | MEDLINE | ID: mdl-38244866

One of the main gaseous pollutants released by chemical production industries are benzene, toluene and xylene (BTX). These dangerous gases require immediate technology to combat them, as they put the health of living organisms at risk. The development of heterogeneous photocatalytic oxidation technology offers several viewpoints, particularly in gaseous-phase decontamination without an additional supply of oxidants in air at atmospheric pressure. However, difficulties such as low quantum efficiency, ability to absorb visible light, affinity towards CO2 and H2O synthesis, and low stability continue to limit its practical use. This review presents recent advances in dry-phase heterogeneous photodegradation as an advanced technology for the practical removal of BTX molecules. This review also examines the impact of low-cost light sources, the roles of the active sites of photocatalysts, and the feasible concentration range of BTX molecules. Numerous studies have demonstrated a significant improvement in the efficiency of the photodegradation of volatile organic compounds by enhancing the photocatalytic reactor system and other factors, such as humidity, temperature, and flow rate. The mechanism for BTX photodegradation based on density functional theory (DFT), electron paramagnetic resonance (EPR) and diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) investigations is also discussed. Finally, the present research complications and anticipated future developments in the field of heterogeneous photocatalytic oxidation technology are discussed.


Benzene , Xylenes , Benzene/chemistry , Xylenes/chemistry , Toluene/chemistry , Catalysis , Light , Gases
8.
Chemosphere ; 351: 141261, 2024 Mar.
Article En | MEDLINE | ID: mdl-38244873

Rapid industrial growth and urbanization have resulted in a significant rise in environmental pollution issues, particularly indoor air pollutants. As a result, it is crucial to design and develop technologies and/or catalysts that are not only cost-effective but also promising high performance and practical applicability. However, achieving this goal has been so far remained a challenging task. Herein, a series of transition metal M - TiO2 (M = W, Fe, Mn) nanocrystals was prepared for photocatalytic degradation of volatile organic compounds (VOCs), i.e., toluene. Of the nanocomposites tested, W-TiO2 showed significantly improved photocatalytic activity for VOC degradation under UV irradiation compared to the others. In particular, the optimized W dopant amount of 0.5 wt% resulted in the outstanding degradation performance of toluene (96%) for the obtained W-TiO2(0.5%) nanocomposite. Moreover, W-TiO2(0.5%) nanocomposite exhibited good stability for 32 h working under high toluene concentration (10 ppm) compared to the pristine TiO2. The current work demonstrates the potential usage of M - TiO2 nanocrystals, particularly W-TiO2(0.5%), as a promising photocatalyst for efficient VOCs degradation.


Air Pollutants , Nanocomposites , Titanium/chemistry , Ultraviolet Rays , Toluene/chemistry , Nanocomposites/chemistry , Catalysis , Air Pollutants/chemistry
9.
Waste Manag ; 175: 191-203, 2024 Mar 01.
Article En | MEDLINE | ID: mdl-38215582

Converting waste resources into porous carbon for pollutants capture is an effective strategy to achieve the environmental goal of "treating waste with waste". Cork is an ideal precursor of porous carbons due to its ordered honeycomb-like cell structure and layered composition distribution. Herein, N-doped porous carbons (PCs) were prepared via two steps of urea-assisted hydrothermal carbonization and chemical activation to mitigate volatile organic compounds (VOCs) pollution. Results indicated that the obtained PC4-800 exhibited remarkable features for adsorption including high total pore volume (0.97 cm3/g) and specific surface area (1864.89 m2/g), as well as abundant N-containing functional groups. The excellent pore structure was primarily owing to the corrosion of the carbon matrix by the gas produced from the reaction of K2CO3 and N-containing functional groups. The adsorption results showed that the PC4-800 have an outstanding toluene adsorption capacity (867.03 mg/g) that outperforming majority of adsorbents previously reported. There are substantial pores in N-doped PCs with a pore width of 1.71-2.28 nm, which is 3 to 4 times the molecular dynamic diameter of toluene, and plays a crucial role in the absorption process. Moreover, the promotional influence of N-functional groups on the toluene adsorption process was verified through DFT calculation by Gaussian imitating, where N-6 generated π-electron enrichment sites on the surface of N-doped PCs, facilitating π-π dispersion with the benzene ring in toluene. This study provides a new strategy to convert waste cork into high-performance adsorbents for VOCs removal.


Volatile Organic Compounds , Porosity , Carbon , Adsorption , Toluene/chemistry
10.
Environ Sci Pollut Res Int ; 31(1): 982-994, 2024 Jan.
Article En | MEDLINE | ID: mdl-38030837

The reasonable geometry design of non-thermal plasma (NTP) reactor is significant for its performance. However, optimizing the reactor structure has received insufficient attention in the studies on removing volatile organic compounds by NTP. Several dielectric barrier discharge (DBD) reactors with various barrier thicknesses and discharge gaps were designed, and their discharge characteristics and toluene degradation performance were explored comprehensively. The number and intensity of current pulses, discharge power, emission spectrum intensity and gas temperature of the DBD reactors increased as barrier thickness decreased. The toluene removal efficiency and mineralization rate increased from 23.2-87.1% and 5.3-27.9% to 81.7-100% and 15.9-51.3%, respectively, when the barrier thickness reduced from 3 to 1 mm. With the increase of discharge gap, the breakdown voltage, discharge power, gas temperature and residence time increased, while the discharge intensity decreased. The reactor with the smallest discharge gap (3.5 mm) exhibited the highest toluene removal efficiency (78.4-100%), mineralization rate (15.6-40.9%) and energy yield (8.4-18.7 g/kWh). Finally, the toluene degradation pathways were proposed based on the detected organic intermediates. The findings can provide critical guidance for designing and optimizing of DBD reactor structures.


Toluene , Volatile Organic Compounds , Toluene/chemistry , Volatile Organic Compounds/chemistry
11.
Environ Sci Technol ; 58(2): 1410-1419, 2024 Jan 16.
Article En | MEDLINE | ID: mdl-38158605

Catalytic oxidation has been considered an effective technique for volatile organic compound degradation. Development of metal foam-based monolithic catalysts coupling electromagnetic induction heating (EMIH) with efficiency and low energy is critical yet challenging in industrial applications. Herein, a Mn18.2-NF monolithic catalyst prepared by electrodeposition exhibited superior toluene catalytic activity under EMIH conditions, and the temperature of 90% toluene conversion decreased by 89 °C compared to that in resistance furnace heating. Relevant characterizations proved that the skin effect induced by EMIH encouraged activation of gaseous oxygen, leading to superior low-temperature redox properties of Mn18.2-NF under the EMIH condition. In situ Fourier transform infrared spectroscopy results showed that skin effect-induced activation of oxidizing species further accelerated the conversion of intermediates. As a result, the Mn18.2-NF monolithic catalyst under EMIH demonstrated remarkable performance for the toluene oxidation, surpassing the conventional nonprecious metal catalyst and other reported monolithic catalysts.


Oxides , Toluene , Toluene/chemistry , Oxides/chemistry , Oxidation-Reduction , Temperature , Catalysis
12.
Environ Sci Technol ; 57(48): 20053-20063, 2023 Dec 05.
Article En | MEDLINE | ID: mdl-37936384

Modulating oxygen vacancies of catalysts through crystal facet engineering is an innovative strategy for boosting the activity for ozonation of catalytic volatile organic compounds (VOCs). In this work, three kinds of facet-engineered monoclinic NiO catalysts were successfully prepared and utilized for catalytic toluene ozonation (CTO). Density functional theory calculations revealed that Ni vacancies were more likely to form preferentially than O vacancies on the (110), (100), and (111) facets of monoclinic NiO due to the stronger Ni-vacancy formation ability, further affecting O-vacancy formation. Extensive characterizations demonstrated that Ni vacancies significantly promoted the formation of O vacancies and thus reactive oxygen species in the (111) facet of monoclinic NiO, among the three facets. The performance evaluation showed that the monoclinic NiO catalyst with a dominant (111) facet exhibits excellent performance for CTO, achieving a toluene conversion of ∼100% at 30 °C after reaction for 120 min under 30 ppm toluene, 210 ppm ozone, 45% relative humidity, and a space velocity of 120 000 h-1. This outperformed the previously reported noble/non-noble metal oxide catalysts used for CTO at room temperature. This study provided novel insight into the development of highly efficient facet-engineered catalysts for the elimination of catalytic VOCs.


Ozone , Volatile Organic Compounds , Toluene/chemistry , Oxides , Oxygen , Catalysis
13.
Environ Sci Pollut Res Int ; 30(47): 104194-104208, 2023 Oct.
Article En | MEDLINE | ID: mdl-37697201

Waste Zanthoxylum bungeanum branches were used to prepare activated carbon adsorbents with high mesopore ratio by H3PO4 staged activation method with adding KNO3 additive. The prepared activated carbon adsorbents were characterized by SEM, BET, FT-IR, and XRD. The adsorption properties of the prepared activated carbon adsorbents were evaluated by the toluene adsorption/desorption in air. The quasi-first-order, quasi-second-order, and Bangham models were used to fit the obtained toluene adsorption results. The oxidative etching of KNO3 additive improved the pore-forming ability of the H3PO4 activator to enhance the activation pore-forming effects of the selected biomass raw material. The secondary pore-forming effects of K atoms promoted the effective expansion of the pore diameter in the activated carbon preparation process to prepare activated carbon adsorbents with high mesopore proportion. The specific surface area and mesopore proportion of the activated carbon adsorbents prepared by adding KNO3 additive exceeded 1100 m2/g and 71.00%, respectively, and the toluene adsorption capacity exceeded 370.00 mg/g. The rich mesopore structures can effectively reduce the toluene mass transfer resistance, which can promote the corresponding activated carbon adsorbent to be regenerated by low-temperature (40 °C) thermal desorption. The toluene adsorption on the prepared activated carbon adsorbents includes surface adsorption and diffusion in pore structures, and the toluene adsorption mechanism is more consistent with the Bangham kinetic model.


Toluene , Zanthoxylum , Toluene/chemistry , Adsorption , Charcoal/chemistry , Spectroscopy, Fourier Transform Infrared
14.
Environ Sci Pollut Res Int ; 30(44): 99830-99841, 2023 Sep.
Article En | MEDLINE | ID: mdl-37615912

The controllable preparation of efficient non-crystalline solid solution catalysts is a great challenge in the catalytic oxidation of volatile organic compounds. In this work, series non-crystalline solid solution structured Ce-Mn co-oxide nanofibers were creatively prepared by adjusting Ce/Mn molar ratios using electrospinning. 0.20CeMnOx (the ratio of Ce to Mn was 0.2) displayed an outstanding low-temperature toluene oxidation activity (T90 = 233 °C). The formation of the amorphous solid solution and the unique nanofiber structure both contributed to a large specific surface area (S = 173 m2 g-1) and high adsorbed oxygen content (Oads/O = 41.3%), which enhanced the number of active oxygen vacancies. The synergies between non-crystalline structure and active oxygen species markedly improved oxygen migration rate as well as redox ability of the catalysts. Additionally, in situ diffuse reflectance infrared Fourier transform spectra showed that the absorbed toluene could be completely oxidized to CO2 and H2O with benzyl alcohol, benzaldehyde, benzoic acid, and maleic anhydride as intermediates. In summary, this study provided an alternative route for the synthesis of non-crystalline metal co-oxide nanofibers.


Nanofibers , Oxides , Oxides/chemistry , Temperature , Oxygen/chemistry , Toluene/chemistry , Catalysis
15.
Chemosphere ; 340: 139761, 2023 Nov.
Article En | MEDLINE | ID: mdl-37558001

BTEX (benzene, toluene, ethylbenzene, xylene) are common pollutants often found in former gasworks sites together with some other contaminants like indene, indane and naphthalene (Ie, Ia, N). This study aimed to evaluate the inhibitory or stimulative substrate interactions between BTEX, and Ie, Ia, N during aerobic biodegradation. For this, batch bottles, containing originally anaerobic subsurface sediments, groundwater and indigenous microorganisms from a contaminated former gasworks site, were spiked with various substrate combinations (BTEX, BTEXIe, BTEXIa, BTEXN, BTEXIeIa, BTEXIeN, BTEXIaN, BTEXIeIaN). Subsequently concentrations were monitored over time. For the BTEXIeIaN mixture, initial concentrations were between 1 and 5 mg L-1, and all compounds were completely degraded by the microbial consortia within 39 days of incubation. The experimental data were fitted to a first order kinetic degradation model for interpretation of inhibition/stimulation between the compounds. Results showed that indene, indane, and naphthalene inhibited the degradation of benzene, toluene, ethylbenzene, o-xylene, with benzene being the most affected. M/p-xylene is the only compound whose biodegradation is stimulated by the presence of indene and indane (individually or mixed) but inhibited by the presence of naphthalene. 16S rRNA amplicon sequencing revealed differentiation in the microbial communities within the batches with different substrate mixtures, especially within the two microbial groups Micrococcaceae and Commamonaceae. Indene had more effect on the BTEX microbial community than indane or naphthalene and the presence of indene increased the relative abundance of Micrococcaceae family. In conclusion, co-presence of various pollutants leads to differentiation in degradation processes as well as in microbial community development. This sheds some light on the underlying reasons for that organic compounds present in mixtures in the subsurface of former gasworks sites are either recalcitrant or subjective towards biodegradation, and this understanding helps to further improve the bioremediation of such sites.


Environmental Pollutants , Indenes , Microbiota , Benzene/chemistry , Biodegradation, Environmental , Kinetics , RNA, Ribosomal, 16S/genetics , Benzene Derivatives/chemistry , Xylenes/metabolism , Toluene/chemistry , Naphthalenes
16.
Environ Sci Pollut Res Int ; 30(45): 100907-100919, 2023 Sep.
Article En | MEDLINE | ID: mdl-37644267

ZSM-5 zeolite has been considered a promising adsorbent for capturing VOCs. However, its hydrophilicity and narrow micropore structure limit their practical application especially under humid atmospheres. In this study, the pure silica mesoporous molecular sieve MCM-41 was assembled on ZSM-5 zeolite with different SiO2/Al2O3 ratios (SARs) via a surfactant-mediated recrystallization method. Then, its adsorption-desorption behaviors were investigated using n-hexane, toluene, and ethyl acetate as VOC model molecules. The results showed that the hydrophobicity of ZSM-5/MCM-41 composites and their VOC diffusion behaviors were significantly improved. Furthermore, the SARs of the ZSM-5 precursors had a remarkable influence on the adsorption performance of ZSM-5/MCM-41 composites. ZSM-5/MCM-41(130) was the optimum option, and its dynamic adsorption capacity for ethyl acetate (111.30 mg·g-1) was higher than that of the corresponding ZSM-5 zeolites even under statured humidity. Meanwhile, the ratios of dynamic adsorption capacities at humid and dry atmospheres (qs,wet/qs,dry) of ZSM-5/MCM-41(130) for n-hexane, toluene, and ethyl acetate were 84.89%, 61.46%, and 73.81% respectively. The results will provide guidelines for the preparation of hydrophobic adsorbents.


Volatile Organic Compounds , Zeolites , Silicon Dioxide/chemistry , Volatile Organic Compounds/chemistry , Adsorption , Zeolites/chemistry , Toluene/chemistry
17.
J Environ Manage ; 345: 118661, 2023 Nov 01.
Article En | MEDLINE | ID: mdl-37515885

Volatile organic compounds (VOCs) evolved from biomass gasification plays a positive role in the formation of PM2.5 and odor pollution. In order to improve the removal rate of various VOCs produced by biomass gasification, a nickel-based supported HZSM-5 cataly st (Ni/HZSM-5 and Ni-Ca-Co/HZSM-5) was prepared by different auxiliary methods, Ni loadings, and pyrolysis temperatures. The catalytic cracking performance of Ni/HZSM-5 catalysts for different VOCs model compounds such as toluene, phenol, furan, acetic acid and cyclohexane were studied in a fixed-bed reactor. The catalysts were further characterized and analyzed by XRD, SEM, XPS and BET. The results showed that the Ni/HZSM--C-Co5 catalyst prepared by ultrasonic-assisted excess impregnation method with Ni loading of 8 wt%, Ca loading of 4 wt%, Co loading of 0.1 wt% had strong catalytic activity for VOCs degradation. With the increase of the cracking temperature, the conversion rate and gas yield of from model compound cracking improved significantly. At 800 °C, the conversion of each model compound was more than 90%, accompanied by the generation of cracking gases such as H2 and CH4. The selectivity of H2 and CH4 from toluene cracking reached 93%, and cyclohexane reached 98%. The models with higher oxygen content and lower bond energy were more likely to undergo reforming reaction to form small molecular gas. Model compounds with large molecular weight and high carbon content provided more carbon sources. Under the conversion degree towards the gas direction was high. This study provides a new idea on the removal of VOCs for the efficient utilization of biomass resources.


Volatile Organic Compounds , Biomass , Gases/chemistry , Catalysis , Carbon , Toluene/chemistry
18.
Environ Sci Pollut Res Int ; 30(40): 92238-92254, 2023 Aug.
Article En | MEDLINE | ID: mdl-37488383

A series of xCe-MnO2 (x = 0-1) catalysts were synthesized using ammonium oxalate as a precipitator via the redox precipitation method and hydrothermal synthesis method. The results indicate that 0.25Ce-MnO2 exhibited the highest catalytic activity for toluene oxidation, with the T99 of 240 °C. Characterization results from XRD, Raman, SEM, TEM, EDS-mapping, BET, and other techniques reveal that the 0.25Ce-MnO2 catalyst exhibited a three-dimensional multistage ultrathin nanosheet structure by adjusting the introduction amount of Ce, with abundant active sites, and effectively formed Ce-Mn homogeneous dispersion. The larger pore size and volume of 0.25Ce-MnO2 catalyst lead to it excellent toluene transfer ability. Furthermore, compared with MnO2, the crystal pattern of 0.25Ce-MnO2 shifted to the tetragonal cryptomelane type α-MnO2 phase and exposed more crystal planes which are beneficial to catalyze toluene. H2-TPR, O2-TPD, and XPS characterization further confirmed the strong interaction between Ce and Mn oxides, which exhibited better low-temperature reducibility and oxygen migration, along with abundant Ce3+ and Mn3+ species, where lattice oxygen played a major role. Moreover, in situ DRIFTS revealed that the 0.25Ce-MnO2 catalyst showed higher adsorption and desorption capacity for toluene than the MnO2 catalyst, and benzoate species were the key intermediates for catalytic oxidation. Additionally, benzoate and surface phenolic species were the key intermediates for catalytic oxidation of MnO2. Because 0.25Ce-MnO2 possesses better ability of converting toluene to benzoate species, it exhibits better activity.


Oxides , Toluene , Oxides/chemistry , Toluene/chemistry , Temperature , Manganese Compounds/chemistry , Oxidation-Reduction , Catalysis , Oxygen/chemistry
19.
Chemosphere ; 338: 139467, 2023 Oct.
Article En | MEDLINE | ID: mdl-37437617

Subsurface co-contamination by multiple pollutants can be challenging for the design of bioremediation strategies since it may require promoting different and often antagonistic degradation pathways. Here, we investigated the simultaneous degradation of toluene and chloroform (CF) in a continuous-flow anaerobic bioelectrochemical reactor. As a result, 47 µmol L-1 d-1 of toluene and 60 µmol L-1 d-1 of CF were concurrently removed, when the anode was polarized at +0.4 V vs. Standard Hydrogen Electrode (SHE). Analysis of the microbial community structure and key functional genes allowed to identify the involved degradation pathways. Interestingly, when acetate was supplied along with toluene, to simulate the impact of a readily biodegradable substrate on process performance, toluene degradation was adversely affected, likely due to competitive inhibition effects. Overall, this study proved the efficacy of the developed bioelectrochemical system in simultaneously treating multiple groundwater contaminants, paving the way for the application in real-world scenarios.


Groundwater , Microbiota , Water Pollutants, Chemical , Biodegradation, Environmental , Toluene/chemistry , Chloroform , Anaerobiosis , Groundwater/chemistry , Water Pollutants, Chemical/chemistry
20.
Molecules ; 28(11)2023 May 25.
Article En | MEDLINE | ID: mdl-37298823

With the development of the chemical industry, benzene, toluene, ethylbenzene, and xylene (BTEX) have gradually become the major indoor air pollutants. Various gas treatment techniques are widely used to prevent the physical and mental health hazards of BTEX in semi-enclosed spaces. Chlorine dioxide (ClO2) is an alternative to chlorine as a secondary disinfectant with a strong oxidation ability, a wide range of action, and no carcinogenic effects. In addition, ClO2 has a unique permeability which allows it to eliminate volatile contaminants from the source. However, little attention has been paid to the removal of BTEX by ClO2, due to the difficulty of removing BTEX in semi-enclosed areas and the lack of testing methods for the reaction intermediates. Therefore, this study explored the performance of ClO2 advanced oxidation technology on both liquid and gaseous benzene, toluene, o-xylene, and m-xylene. The results showed that ClO2 was efficient in the removal of BTEX. The byproducts were detected by gas chromatography-mass spectrometry (GC-MS) and the reaction mechanism was speculated using the ab initio molecular orbital calculations method. The results demonstrated that ClO2 could remove the BTEX from the water and the air without causing secondary pollution.


Air Pollution, Indoor , Benzene , Benzene/chemistry , Toluene/chemistry , Xylenes/chemistry , Air Pollution, Indoor/analysis , Benzene Derivatives/chemistry , Gases/analysis , Environmental Monitoring/methods
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