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1.
Molecules ; 29(15)2024 Jul 26.
Artículo en Inglés | MEDLINE | ID: mdl-39124912

RESUMEN

It is important to develop effective strategies for enhancing the removal capacity of aromatic volatile organic compounds (VOCs) by modifying conventional porous adsorbents. In this study, a novel HZSM-5 zeolite-supported sulfonic acid (ZSM-OSO3H) was prepared through ClSO3H modification in dichloromethane and employed for the elimination of gaseous o-xylene. The ClSO3H modification enables the bonding of -OSO3H groups onto the HZSM-5 support, achieving a loading of 8.25 mmol·g-1 and leading to a degradation in both crystallinity and textural structure. Within an active temperature range of 110-145 °C, ZSM-OSO3H can efficiently remove o-xylene through a novel reactive adsorption mechanism, exhibiting a removal rate exceeding 98% and reaching a maximum breakthrough adsorption capacity of 264.7 mg. The adsorbed o-xylene derivative is identified as 3,4-dimethylbenzenesulfonic acid. ZSM-OSO3H demonstrates superior adsorption performance for o-xylene along with excellent recyclability. These findings suggest that ClSO3H sulfonation offers a promising approach for modifying various types of zeolites to enhance both the elimination and resource conversion of aromatic VOCs.

2.
Chem Biodivers ; 21(6): e202400150, 2024 Jun.
Artículo en Inglés | MEDLINE | ID: mdl-38548660

RESUMEN

Experiments were conducted in this study on the co-hydropyrolysis of three components of biomass (cellulose, hemicellulose, and lignin) and HDPE by using SR-Pd/Trap-HZ-5 as catalyst. To control the variable, we use the same experiment conditions in co-hydropyrolysis: Si/Al ratio of 50, Pd load 1 %, catalyst to reactant ratio of 1 : 10, 1 MPa, 400 °C, reaction time 1 h. Use XRD, TEM, BET, and NH3-TPD to confirm catalyst successful synthesis; use pine sawdust (PW) co-hydropyrolysis with HDPE to analyse catalytic activity; and use GC/MS to characterize the chemical composition of the bio-oil from the co-hydropyrolysis of biomass components and HDPE. The results show that cellulose has a significant synergistic effect with aromatic hydrocarbon production, whose selectivity was 93.3 %; hemicellulose has a synergistic effect; aromatic selectivity can reach 75.1 %; and a negative synergistic effect between lignin and HDPE was shown as the selectivity of aromatic hydrocarbons decreased from 62.1 % to 15.6 %.


Asunto(s)
Biomasa , Celulosa , Hidrocarburos Aromáticos , Polisacáridos , Pirólisis , Zeolitas , Catálisis , Hidrocarburos Aromáticos/química , Polisacáridos/química , Celulosa/química , Zeolitas/química , Lignina/química
3.
Int J Mol Sci ; 25(4)2024 Feb 17.
Artículo en Inglés | MEDLINE | ID: mdl-38397065

RESUMEN

During the methanol-to-aromatics (MTA) process, a large amount of water is generated, while the influence and mechanism of water on the activity and selectivity of the light olefin aromatization reaction are still unclear. Therefore, a study was conducted to systematically investigate the effects of water on the reactivity and the product distribution in ethylene aromatization using infrared spectroscopy (IR), intelligent gravitation analyzer (IGA), and X-ray absorption fine structure (XAFS) characterizations. The results demonstrated that the presence of water reduced ethylene conversion and aromatic selectivity while increasing hydrogen selectivity at the same contact time. This indicated that water had an effect on the reaction pathway by promoting the dehydrogenation reaction and suppressing the hydrogen transfer reaction. A detailed analysis using linear combination fitting (LCF) of Zn K-edge X-ray absorption near-edge spectroscopy (XANES) on Zn/HZSM-5 catalysts showed significant variations in the state of existence and the distribution of Zn species on the deactivated catalysts, depending on different reaction atmospheres and water contents. The presence of water strongly hindered the conversion of ZnOH+ species, which served as the active centers for the dehydrogenation reaction, to ZnO on the catalyst. As a result, the dehydrogenation activity remained high in the presence of water. This study using IR and IGA techniques revealed that water on the Zn/HZSM-5 catalyst inhibited the adsorption of ethylene on the zeolite, resulting in a noticeable decrease in ethylene conversion and a decrease in aromatic selectivity. These findings contribute to a deeper understanding of the aromatization reaction process and provide data support for the design of efficient aromatization catalysts.


Asunto(s)
Etilenos , Agua , Hidrógeno , Inmunoglobulina A , Zinc
4.
Environ Sci Pollut Res Int ; 31(7): 11276-11284, 2024 Feb.
Artículo en Inglés | MEDLINE | ID: mdl-38217812

RESUMEN

In this study, we synthesized a Ce-modified Mn/HZSM-5 adsorbent via the ultrasound-assisted impregnation for Hg0 capture. Given the addition of 15% CeO2, ~ 100% Hg0 efficiency was reached at 200 °C, suggesting its promotional effect on Hg0 removal. The doped Ce introduced additional chemisorbed oxygen species onto the adsorbent surfaces, which facilitated the oxidation of Hg0 to HgO. Even though adding CeO2 led to a weakened adsorbent acidity, yet it appeared that this negative affect could be completely overcome by the enhanced oxidative ability, which finally endowed Ce-modified Mn/HZSM-5 with a satisfactory Hg0 removal performance within the whole investigated temperature range. During the Hg0 capture process, chemisorption was predominant with Mn4+operating as the main active site for oxidizing Hg0 to Hg2+. Finally, the 15Ce-Mn/HZSM-5 adsorbent exhibited good recyclability and stability. However, its tolerance to H2O and SO2 appeared relatively weak, suggesting that some modification should be conducted to improve its practicality.


Asunto(s)
Mercurio , Óxidos , Óxidos/química , Mercurio/química , Catálisis , Oxidación-Reducción , Oxígeno/química
5.
Environ Pollut ; 343: 123198, 2024 Feb 15.
Artículo en Inglés | MEDLINE | ID: mdl-38128713

RESUMEN

Wax is a detrimental byproduct of plastic waste pyrolysis causing challenges upon its release into the environment owing to persistence and potential toxicity. In this study, the valorization of wax materials through conversion into BTEX (i.e., benzene, toluene, ethylbenzene, and xylene) was achieved via catalytic pyrolysis using zeolite-based catalysts. The potential of two types of waxes, spent wax (SW), derived from the pyrolysis of plastic waste, and commercial paraffin wax (PW), for BTEX generation, was investigated. Using HZSM-5, higher yields of oil (54.9 wt%) and BTEX (18.2 wt%) were produced from the pyrolysis of SW compared to PW (32.3 and 14.1 wt%, respectively). This is due to the improved accessibility of lighter hydrocarbons in SW to Brønsted and Lewis acid sites in HZSM-5 micropores, promoting cracking, isomerization, cyclization, Diels-Alder, and dehydrogenation reactions. Further, the use of HZSM-5 resulted in significantly larger yields of oil and BTEX from SW pyrolysis compared to Hbeta and HY. This phenomenon is ascribed to the well-balanced distribution of Brønsted and Lewis acid sites and the identical geometric structure of HZSM-5 micropores and BTEX molecules. The addition of Ga to HZSM-5 further led to 2.24% and 28.30% enhancements in oil and BTEX yields, respectively, by adjusting the acidity of the catalyst through the introduction of new Lewis acid sites. The regeneration of the Ga/HZSM-5 catalyst by removing deposited coke on the spent catalyst under air partially recovered catalytic activity. This study not only offers an efficient transformation of undesirable wax into valuable fuels but also provides an environmentally promising solution, mitigating pollution, contributing to carbon capture, and promoting a healthier and more sustainable environment. It also suggests future research directions, including catalyst optimization and deactivation management, feedstock variability exploration, and techno-economic analyses for sustainable wax conversion into BTEX via catalytic pyrolysis.


Asunto(s)
Ácidos de Lewis , Pirólisis , Hidrocarburos , Tolueno , Catálisis , Ambiente , Calor
6.
J Environ Manage ; 345: 118661, 2023 Nov 01.
Artículo en Inglés | MEDLINE | ID: mdl-37515885

RESUMEN

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.


Asunto(s)
Compuestos Orgánicos Volátiles , Biomasa , Gases/química , Catálisis , Carbono , Tolueno/química
7.
Molecules ; 28(10)2023 May 22.
Artículo en Inglés | MEDLINE | ID: mdl-37241985

RESUMEN

A niobium-doped HZSM-5 (H[Nb]ZSM-5) was prepared by a hydrothermal synthesis method. The morphology, phase structure, composition, pore structure, and acid content of the catalyst were characterized using a series of analysis techniques such as scanning electron microscope (SEM), energy-dispersive X-ray (EDX), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), nitrogen adsorption-desorption, and temperature programmed desorption measurements (NH3-TPD). The H[Nb]ZSM-5 catalyst fully remained within the crystal framework and pore structure of HZSM-5. Meanwhile, introduction of niobium (V) endowed the catalyst with both Lewis acid and Bronsted acid sites. Catalytic fast pyrolysis (CFP) of alkali lignin was carried out through a pyrolysis and gas chromatography-mass spectrometry (Py-GC/MS) at 650 °C and atmospheric pressure. The results indicated that H[Nb]ZSM-5 can efficiently and selectively convert lignin into monoaromatic hydrocarbons (MAHs), compared to the control HZSM-5. Catalyzed by H[Nb]ZSM-5, the content of MAHs and aliphatic hydrocarbons reached 43.4% and 20.8%, respectively; while under the catalysis of HZSM-5, these values were 35.5% and 3.2%, respectively. H[Nb]ZSM-5 remarkably lowered the phenol content to approximately 2.8%, which is far lower than the content (24.9%) obtained under HZSM-5 catalysis.

8.
Nanotechnology ; 34(23)2023 Mar 20.
Artículo en Inglés | MEDLINE | ID: mdl-36857761

RESUMEN

An ultra-thin overcoating of zirconium oxide (ZrO2) film on CuO-ZnO-Al2O3(CZA) catalysts by atomic layer deposition (ALD) was proved to enhance the catalytic performance of CZA/HZSM-5 (H form of Zeolite Socony Mobil-5) bifunctional catalysts for hydrogenation of CO2to dimethyl ether (DME). Under optimal reaction conditions (i.e. 240 °C and 2.8 MPa), the yield of product DME increased from 17.22% for the bare CZA/HZSM-5 catalysts, to 18.40% for the CZA catalyst after 5 cycles of ZrO2ALD with HZSM-5 catalyst. All the catalysts modified by ZrO2ALD displayed significantly improved catalytic stability of hydrogenation of CO2to DME reaction, compared to that of CZA/HZSM-5 bifunctional catalysts. The loss of DME yield in 100 h of reaction was greatly mitigated from 6.20% (loss of absolute value) to 3.01% for the CZA catalyst with 20 cycles of ZrO2ALD overcoating. Characterizations including hydrogen temperature programmed reduction, x-ray powder diffraction, and x-ray photoelectron spectroscopy revealed that there was strong interaction between Cu active centers and ZrO2.

9.
Bioresour Technol ; 373: 128702, 2023 Apr.
Artículo en Inglés | MEDLINE | ID: mdl-36740100

RESUMEN

Air gasification of the Wood-Plastic Composite (WPC) was performed over Ni-loaded HZSM-5 catalysts to generate H2-rich gas. Increasing SiO2/Al2O3 ratio (SAR) of HZSM-5 adversely affected catalytic activity, where the highest gas yield (51.38 wt%) and H2 selectivity (27.01 vol%) were acquired using 20 %Ni/HZSM-5(30) than those produced over 20 %Ni/HZSM-5(80) and 20 %Ni/HZSM-5(280). Reducing SAR was also favorably conducive to increasing the acyclic at the expense of cyclic compounds in oil products. These phenomena are attributed to enhanced acid strength and Ni dispersion of 20 %Ni/HZSM-5(30) catalyst. Moreover, catalytic activity in the terms of gas yield and H2 selectivity enhanced with growing Ni loading to 20 %. Also, the addition of promoters (Cu and Ca) to 20 %Ni/HZSM-5(30) boosted the catalytic efficiency for H2-rich gas generation. Raising temperature indicated a positive relevance with the gas yield and H2 selectivity. WPC valorization via gasification technology would be an outstanding outlook in the terms of a waste-to-energy platform.


Asunto(s)
Plásticos , Dióxido de Silicio , Madera , Temperatura , Catálisis
10.
Molecules ; 27(22)2022 Nov 18.
Artículo en Inglés | MEDLINE | ID: mdl-36432121

RESUMEN

Due to their high lipid content, microalgae are one of the most significant sources of green hydrocarbons, which might help lessen the world's need for fossil fuels. Many zeolite-based catalysts are quickly deactivated by coke production and have a short lifetime. In this study, a bimetallic Lanthanum-Cerium (La-Ce)-modified HZSM-5 zeolite catalyst was synthesized through an impregnation method and was tested for the conversion of hydrolyzed oil into oxygen-free hydrocarbon fuels of high energy content. Initially, hydrolyzed oil (HO), the byproduct of the transesterification process, was obtained by the reaction of crude oil derived from Chlorella vulgaris microalgae and a methanol. Various catalysts were produced, screened, and evaluated for their ability to convert algal HO into hydrocarbons and other valuable compounds in a batch reactor. The performance of HZSM-5 was systematically tested in view of La-Ce loaded on conversion, yield, and selectivity. NH3-TPD analysis showed that the total acidity of the La-Ce-modified zeolites was lower than that of the pure HZSM-5 catalyst. TGA testing revealed that including the rare earth elements La and Ce in the HZSM-5 catalyst lowered the catalyst propensity for producing coke deposits. The acid sites necessary for algal HO conversion were improved by putting La and Ce into HZSM-5 zeolite at various loading percentages. The maximum hydrocarbon yield (42.963%), the highest HHV (34.362 MJ/Kg), and the highest DOD% (62.191%) were all achieved by the (7.5%La-2.5%Ce)/HZSM-5 catalyst, which was synthesized in this work. For comparison, the hydrocarbon yield for the parent HZSM-5 was 21.838%, the HHV was (33.230 MJ/Kg), and the DOD% was 44.235%. In conclusion, La and Ce-loading on the parent HZSM-5 may be responsible for the observed alterations in textural properties; nevertheless, there is no clear correlation between the physical features and the hydrocarbon yield (%). The principal effect of La and Ce modifying the parent HZSM-5 zeolite was to modify the acidic sites needed to enhance the conversion (%) of the algal HO during the catalytic deoxygenation process, which in turn raised the hydrocarbon yield (%) and increased the HHV and DOD%.


Asunto(s)
Cerio , Chlorella vulgaris , Coque , Microalgas , Zeolitas , Lantano , Hidrocarburos
11.
Molecules ; 27(21)2022 Oct 25.
Artículo en Inglés | MEDLINE | ID: mdl-36364049

RESUMEN

Biodiesel is generally produced from vegetable oils and methanol, which also generates glycerol as byproduct. To improve the overall economic performance of the process, the selective formation of methanol from glycerol is important in biodiesel production. In the present study, a CaO modified HZSM-5 zeolite was prepared by an impregnation method and used for the conversion of glycerol to methanol. We found that the 10%CaO/HZSM-5 with Si/Al ratio of 38 exhibited highest selectivity to methanol of 70%, with a glycerol conversion of 100% under 340 ℃ and atmospheric pressure. The characterization results showed that the introduction of a small amount of CaO into the HZSM-5 did not affect the structure of zeolite. The incorporation of HZSM-5 as an acidic catalyst and CaO as a basic catalyst in a synergistic catalysis system led to higher conversion of glycerol and selectivity of methanol.


Asunto(s)
Zeolitas , Metanol/química , Biocombustibles , Glicerol , Catálisis
12.
Molecules ; 27(21)2022 Oct 25.
Artículo en Inglés | MEDLINE | ID: mdl-36364078

RESUMEN

Despite the extensive research into the catalytic uses of zeolite-based catalysts, these catalysts have a limited useful lifetime because of the deactivating effect of coke production. This study looks at the use of Cerium (Ce) loaded HZSM-5 zeolite catalysts in the hydrocarbon and oxygenated chemical conversion from Chlorella Vulgaris microalgae crude oil. Characterization of structure, morphology, and crystallinity was performed after the catalysts were manufactured using the impregnation technique. Soxhlet extraction was carried out to extract the crude oil of microalgae. Transesterification reaction was used to produce algal hydrolyzed oil (HO), and the resulting HO was put to use in a batch reactor at 300 °C, 1000 rpm, 7 bars of nitrogen pressure, a catalyst to the algal HO ratio of 15% (wt. %), and a retention time of 6 h. To determine which Ce-loaded HZSM-5 catalysts would be most effective in converting algal HO into non-oxygenated molecules (hydrocarbons), we conducted a series of tests. Liquid product characteristics were analyzed for elemental composition, higher heating value (HHV), atomic ratios of O/C and H/C, and degree of deoxygenation (DOD%). Results were categorized into three groups: product yield, chemical composition, and carbon number distribution. When Cerium was added to HZSM-5 zeolite at varying loading percentages, the zeolite's acid sites became more effective in facilitating the algal HO conversion. The results showed that 10%Ce/HZSM-5 had the greatest conversion of the algal HO, the yield of hydrocarbons, HHV, and DOD% (98.2%, 30%, 34.05 MJ/Kg, and 51.44%, respectively) among all the synthesized catalysts in this research. In conclusion, the physical changes seen in the textural characteristics may be attributed to Cerium-loading on the parent HZSM-5; nevertheless, there is no direct association between the physical features and the hydrocarbons yield (%). The primary impact of Cerium alteration of the parent HZSM-5 zeolite was to change the acidic sites required to boost the conversion (%) of the algal HO in the catalytic deoxygenation process, which in turn increased the hydrocarbons yield (%), which in turn increased the HHV and DOD%.


Asunto(s)
Cerio , Chlorella vulgaris , Microalgas , Petróleo , Zeolitas , Biocombustibles , Biomasa , Catálisis , Hidrocarburos , Calor
13.
Molecules ; 27(19)2022 Oct 02.
Artículo en Inglés | MEDLINE | ID: mdl-36235064

RESUMEN

Microalgae is one of the most important sources of green hydrocarbons because it contains a high percentage of lipids and is likely to reduce reliance on fossil fuels. Several zeolite-based catalysts have a short lifetime due to coke-formation deactivation. In this study, a lanthanum-modified HZSM-5 zeolite catalyst for the conversion of crude oil into non-oxygenated compounds (hydrocarbons) and oxygenated compounds has been investigated. The crude oil of Chlorella Vulgaris microalgae was extracted using Soxhlet and converted into hydrolyzed oil (HO) through a transesterification reaction. The experiments were conducted in a batch reactor (300 °C, 1000 rpm, 7 bar of N2, the catalyst to the algal HO ratio of 15% (wt.%) and 6 h). The results were organized into three groups: product yield, chemical composition, and carbon number distribution. The liquid products were investigated, including their elemental composition, higher heating value (HHV), atomic ratios of O/C and H/C, and degree of deoxygenation (DOD%). The loading of lanthanum into HZSM-5 zeolite with different loading percentages enhanced the acid sites needed for the algal HO conversion. Among all the synthesized catalysts, 10%La/HZSM-5 produced the highest conversion of the algal HO, the highest yield of hydrocarbons, the highest HHV, and the highest DOD%; those were 100%, 36.88%, 34.16 MJ/kg, and 56.11%, respectively. The enhanced catalytic conversion was due to the presence of lanthanum, which alters the active sites for the desired reactions of catalytic deoxygenation. The main effect of the modification of the parent HZSM-5 zeolite with lanthanum led to adjusting the acidic sites needed to increase the conversion (%) of the algal HO in the catalytic deoxygenation process and thus increase the hydrocarbon yield (%), which in turn led to an increase in the HHV and DOD%. The proposed La-based zeolite composite is promising for different energy applications due to its unique benefits compared to other expensive and less-stable catalysts.


Asunto(s)
Chlorella vulgaris , Coque , Microalgas , Petróleo , Zeolitas , Biocombustibles , Biomasa , Carbono , Catálisis , Hidrocarburos , Lantano , Lípidos
14.
J Environ Manage ; 324: 116392, 2022 Dec 15.
Artículo en Inglés | MEDLINE | ID: mdl-36208512

RESUMEN

The main objective of the current work is to investigate the effect of nickel-waste chicken eggshell modified Hydrogen exchanged Zeolite Socony Mobil-5 (Ni-WCE/HZSM-5) on pyrolysis of high-density polyethylene (HDPE). Ni-WCE/HZSM-5 was synthesized via the impregnation incipient wetness (IWI) method with Ni and WCE mass loading of 4 and 12 wt% respectively. HZSM-5, CaO, WCE, WCE/HZSM-5, and Ni/HZSM-5 were prepared for comparison purposes with Ni-WCE/HZSM-5. All the synthesized catalysts were characterized for phase analysis, metal loading, surface morphology, and textural properties. The impregnation of nickel and WCE had significantly affected the original framework of HZSM-5, where the crystallinity percentage and average crystal size of HZSM-5 dropped to 44.97% and increased to 47.90 nm respectively. The surface morphology of HZSM-5 has drastically changed from a cubic-like shape into a spider web-like surface after the impregnation of WCE. The BET surface area of HZSM-5 has been lowered due to the impregnation of nickel and WCE, but the total pore volume has increased greatly from 0.2291 cm3/g to 0.2621 cm3/g. The catalyst performance was investigated in the pyrolysis of HDPE via a fixed bed reactor and the pyrolysis oil was further analysed to evaluate the distribution of C6 to C9> hydrocarbons. Among the tested catalytic samples, the highest pyrolysis oil yield was achieved by WCE (80%) followed by CaO (78%), WCE/HZSM-5 (63%), HZSM-5 (61%), Ni/HZSM-5 (44%) and Ni-WCE/HZSM-5 (50%). For hydrocarbon distribution in pyrolysis oil, the Ni/HZSM-5 produced the highest of total C6 and C7 hydrocarbons at 12% and 27% respectively followed by WCE/HZSM-5 (4% and 20%), non-catalytic (5% and 13%), Ni-WCE/HZSM-5 (0% and 15%), WCE (0% and 10%), HZSM-5 (0% and 6%) and CaO (0% and 0%).


Asunto(s)
Pirólisis , Zeolitas , Animales , Polietileno , Níquel/química , Pollos , Cáscara de Huevo , Calor , Catálisis , Zeolitas/química , Hidrocarburos , Biocombustibles
15.
Bioresour Technol ; 360: 127594, 2022 Sep.
Artículo en Inglés | MEDLINE | ID: mdl-35809872

RESUMEN

The weight loss characteristics, product distribution and bio-oil composition of co-pyrolysis of rice straw (RS) and Chlorella vulgaris (CV) were investigated by microwave oven. Then, the catalytic effect of activated carbon (AC) and HZSM-5 on these characteristics were studied. Results showed that AC strongly improved co-pyrolysis weight loss characteristics and obtained maximum average weight loss rate (Ra) at 30% addition with 0.01639 wt.%/s. While HZSM-5 promoted the characteristics as addition was lower than 10%. In the case of compound additives, 20% A7H3 obtained the maximum Ra (0.01413 wt.%/s). Furthermore, both single AC and HZSM-5 showed negative effect on bio-oil production, while 20% A7H3 (AC/HZSM-5 = 7:3) achieved the maximum production (24%). For bio-oil composition, 30% A10H0 showed strong selectivity for phenol and N-heterocycle and 10% A0H10 showed strong aromatization capacity, and the addition of 20% A7H3 increased the hydrocarbons content from 20.79% to 31.63% compared with the blank group.


Asunto(s)
Chlorella vulgaris , Oryza , Biocombustibles , Biomasa , Catálisis , Carbón Orgánico , Calor , Microondas , Pirólisis , Pérdida de Peso
16.
Environ Res ; 214(Pt 2): 113911, 2022 11.
Artículo en Inglés | MEDLINE | ID: mdl-35863449

RESUMEN

This research studied the catalytic pyrolysis of oil sludge (OS) over metal-loaded HZSM-5 catalysts, an eco-friendly and cost-effective technology to produce value-added aromatics such as benzene, toluene, ethylbenzene, and xylene (BTEXs). In particular, it evaluated the respective effects of the experimental parameters: the type and amount of the metal loaded, the reaction temperature, and the OS/catalyst ratio, on the BTEXs yield sequentially to achieve optimum conditions. This evaluation showed that the highest yields of the BTEXs (6.61 wt%) and other aromatics were achieved when Ni was incorporated into the HZSM-5 (Ni/HZSM-5) followed by the corresponding yields of Ga/HZSM-5 and Fe/HZSM-5, due to a better distribution of Ni on the support surface and an enhanced acidity strength of this catalyst. Further, increase in Ni loading (up to 10 wt% Ni/HZSM-5) increased the BTEXs yield to 13.48 wt%. However, the excessive Ni loading (15 wt% Ni/HZSM-5) resulted in a reduced BTEXs yield due to the blockage of the zeolite channels. Next, an increase in the reaction temperature from 500 °C to 600 °C increased the yield of the BTEXs and other aromatics. However, a further increase in the reaction temperature to 650 °C decreased slightly their yield because of the stimulating secondary reactions at high temperatures. The increase of catalyst amount (OS/catalyst of 1/3) also maximized the BTEXs yield (30.50 wt%).


Asunto(s)
Pirólisis , Zeolitas , Biocombustibles/análisis , Catálisis , Calor , Metales , Aguas del Alcantarillado
17.
Sci Total Environ ; 827: 154186, 2022 Jun 25.
Artículo en Inglés | MEDLINE | ID: mdl-35231512

RESUMEN

Energy shortage and environmental pollution have attracted long-term attention. In this study, CaO were prepared from waste eggshell (EGC), preserved egg shell (PEC), clam shell (CLC) and crab shell (CRC), which were then compared with commercial CaO (CMC) to catalyze microwave-assisted pyrolysis of waste cooking oil (WCO) for enrichment of aromatics in bio-oil. The characterization results indicated that EGC and CLC contained 95.54% and 95.61% CaO respectively, which were higher than that of CMC (95.11%), and the pore properties of EGC were the best. In addition, the effects of CaO type and catalytic mode on pyrolysis were studied. In CaO catalytic pyrolysis, CMC and CLC in-situ catalysis produced more aromatics than ex-situ catalysis, and PEC and CRC were more conducive to aromatics formation in ex-situ condition. EGC was conducive to produce benzene, toluene and xylene (BTX) both in in-situ (19.04%) and ex-situ (20.76%) catalytic pyrolysis. In CaO/HZSM-5 catalysis, the optimal dual catalytic mode for generating monocyclic aromatic hydrocarbons (MAHs) was Mode A (CaO separated from HZSM-5 for ex-situ catalysis), and EGC/HZSM-5 performed well in benzene, toluene and xylene (BTX) production.


Asunto(s)
Microondas , Pirólisis , Animales , Benceno , Biocombustibles , Biomasa , Catálisis , Culinaria , Calor , Aceites de Plantas , Polifenoles , Tolueno , Xilenos
18.
Angew Chem Int Ed Engl ; 61(13): e202114953, 2022 Mar 21.
Artículo en Inglés | MEDLINE | ID: mdl-35104006

RESUMEN

The transformation of methane into high value-added chemicals such as aromatics provides a more desired approach towards sustainable chemistry but remains a critical challenge due to the low selectivity of aromatics and poor stability. Herein, we first report a coupling reaction of CH3 Cl and CO (CCTA) based on methane conversion, which achieves extremely high aromatics selectivity (82.2 %) with the selectivity of BTX up to ca. 60 % over HZSM-5. The promoting effects have been demonstrated on other zeolites especially 10-membered rings (10 MR) zeolites. Multiple characterizations show that 2,3-dimethyl-2-cyclopentene-1-one (DMCPO) is generated from acetyl groups and olefins. Furthermore, isotopic labeling analysis confirms that CO is inserted into the DMCPO and aromatics rings. A new aromatization mechanism is proposed, including the formation of the above intermediates, which conspicuously weakens the hydrogen transfer reaction, leading to a considerable increase of aromatics selectivity and a dramatic drop in alkanes.

19.
Bioresour Technol ; 349: 126787, 2022 Apr.
Artículo en Inglés | MEDLINE | ID: mdl-35134525

RESUMEN

Fresh HZSM-5 catalyst modification experiment was carried out on the direct non-thermal plasma (DNTP) reactor. The aim of this work was to study the effects of modified voltages on the physicochemical properties of HZSM-5 and its enhancement in biomass catalytic pyrolysis. The results showed that DNTP modification was performed at different voltages of 20 kV, 22 kV, 24 kV, compared with fresh HZSM-5, the effect of 22 kV voltage was preferably. H-22 had the largest specific surface area and mesoporous volume, and the total acid content added 17.02%. The biomass catalytic pyrolysis test was used to test the HZSM-5 catalytic activity after modification. The results showed that the catalyst obtained by the catalyst under 22 kV modified voltage had the highest monocyclic aromatic hydrocarbon selectivity of 40.55%.


Asunto(s)
Biocombustibles , Gases em Plasma , Biomasa , Catálisis , Calor , Pirólisis
20.
Molecules ; 27(2)2022 Jan 08.
Artículo en Inglés | MEDLINE | ID: mdl-35056711

RESUMEN

Decomposition of N2O on modified zeolites, crystalline titanosilicalites, and related amorphous systems is studied by the catalytic and spectroscopic methods. Zinc-containing HZSM-5 zeolites and titanosilicalites with moderate Ti/Si ratios are shown to exhibit a better catalytic performance in N2O decomposition as compared with conventionally used Cu/HZSM-5 zeolites and amorphous Cu-containing catalysts. Dehydroxylation of the HZSM-5 zeolite by calcination at 1120 K results in an enhancement of the N2O conversion. The mechanism of the reaction and the role of coordinatively unsaturated cations and Lewis acid sites in N2O decomposition are discussed on the basis of the spectroscopic data.

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