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1.
Environ Sci Pollut Res Int ; 31(30): 42640-42671, 2024 Jun.
Article in English | MEDLINE | ID: mdl-38902444

ABSTRACT

The current work investigated emerging fields for generating and consuming hydrogen and synthetic Fischer-Tropsch (FT) fuels, especially from detrimental greenhouse gases, CO2 and CH4. Technologies for syngas generation ranging from partial oxidation, auto-thermal, dry, photothermal and wet or steam reforming of methane were adequately reviewed alongside biomass valorisation for hydrogen generation, water electrolysis and climate challenges due to methane flaring, production, storage, transportation, challenges and opportunities in CO2 and CH4 utilisation. Under the same conditions, dry reforming produces more coke than steam reforming. However, combining the two techniques produces syngas with a high H2/CO ratio, which is suitable for producing long-chain hydrocarbons. Although the steam methane reforming (SMR) process has been industrialised, it is well known to consume significant energy. However, coke production via catalytic methane decomposition, the prime hindrance to large-scale implementation of these techniques for hydrogen production, could be addressed by coupling CO with CO2 conversion to alter the H2/CO ratio of syngas, increasing the reaction temperatures in dry reforming, or increasing the steam content fed in steam reforming. Optimised hydrogen production and generation of green fuels from CO2 and CH4 can be achieved by implementing these strategies.


Subject(s)
Carbon Dioxide , Hydrogen , Methane , Biofuels
2.
Article in English | MEDLINE | ID: mdl-38468003

ABSTRACT

The presence of stable and hazardous organic dyes in industrial effluents poses significant risks to both public health and the environment. Activated carbons and biochars are widely used adsorbents for removal of these pollutants, but they often have several disadvantages such as poor recoverability and inseparability from water in the post-adsorption process. Incorporating a magnetic component into activated carbons can address these drawbacks. This study aims to optimizing the production of NiFe2O4-loaded activated carbon (NiFe2O4@AC) derived from a Bidens pilosa biomass source through a hydrothermal method for the adsorption of Rhodamine B (RhB), methyl orange (MO), and methyl red (MR) dyes. Response surface methodology (RSM) and Box-Behnken design (BBD) were applied to analyze the key synthesis factors such as NiFe2O4 loading percentage (10-50%), hydrothermal temperature (120-180 °C), and reaction time (6-18 h). The optimized condition was found at a NiFe2O4 loading of 19.93%, a temperature of 135.55 °C, and a reaction time of 16.54 h. The optimum NiFe2O4@AC demonstrated excellent sorption efficiencies of higher than 92.98-97.10% against all three dyes. This adsorbent was characterized, exhibiting a well-developed porous structure with a high surface area of 973.5 m2 g-1. Kinetic and isotherm were studied with the best fit of pseudo-second-order, and Freundlich or Temkin. Qmax values were determined to be 204.07, 266.16, and 177.70 mg g-1 for RhB, MO, and MR, respectively. By selecting HCl as an elution, NiFe2O4@AC could be efficiently reused for at least 4 cycles. Thus, the Bidens pilosa-derived NiFe2O4@AC can be a promising material for effective and recyclable removal of dye pollutants from wastewater.

3.
RSC Adv ; 14(7): 4509-4517, 2024 Jan 31.
Article in English | MEDLINE | ID: mdl-38312717

ABSTRACT

Tautomerism alters the structure and properties of materials, which can be exploited to control their chemical and biological activities. The role of pH-induced tautomerism of polyvinylpyrrolidone (PVP) was determined by measuring the size, stability, and antioxidant and antibacterial properties of microwave synthesized-silver nanoparticles (AgNPs). TEM and XRD analyses confirmed the formation of face-centered cubic silver nanoparticles. PVP stabilized the AgNPs by interaction with the carbonyl or hydroxyl groups depending on the tautomerization under different pH conditions. At pH 4, PVP was stable in the keto tautomer, stabilizing Ag through electron donation of oxygen atoms in the carbonyl group, producing smaller AgNPs with a higher zeta potential. At pH 7 and 9, the enol tautomer PVP stabilized the AgNPs via oxygen atoms in the hydroxyl group, forming large nanoparticles. The keto form of PVP improved the stability and antioxidant and antibacterial properties of AgNPs compared with the enol form. This study also excluded the antioxidant contribution of PVP via hydrogen donation to free radicals. A facile method for controlling the size of AgNPs by adapting the pH-induced tautomerism of PVP that affects their stability and antioxidant and antibacterial activities is thus reported.

4.
RSC Adv ; 14(10): 6815-6822, 2024 Feb 21.
Article in English | MEDLINE | ID: mdl-38405073

ABSTRACT

To consider silver nanoparticles (AgNPs) as a colorimetric sensor for H2O2 we require investigation of the effects of the homogeneity of the nanoparticle size and morphology on the sensor parameters. Uniformly-sized Ag nanoparticles with diameters of ∼18.8 ± 2.8 nm were produced using microwave irradiation (AgNP1) but non-uniform particles with diameters of ∼71.2 ± 19.4 nm (AgNP2) were formed without microwave irradiation. Microwave synthesis produced AgNP1 with superiority in terms of repeatability, selectivity and sensor stability for up to eight months of storage over AgNP2. AgNP1 exhibited higher sensitivity and detection limits in the working range of 0.01-40000 µM as compared to AgNP2. The application of the AgNP sensor to milk samples provided recovery values of 99.09-100.56% for AgNP1 and 98.18-101.90% for AgNP2. Microwave irradiation resulted in strong and uniform PVP-Ag interactions for isotropic growth into small nanoparticles. Size and morphology uniformity determined the characteristics of the AgNP sensor that can be applied for H2O2 detection in a wide range of concentrations and real-time evaluation, with the potential for industrial applications.

5.
RSC Adv ; 13(46): 32648-32659, 2023 Oct 31.
Article in English | MEDLINE | ID: mdl-37936636

ABSTRACT

Saponin is a plant-derived chemical with an amphiphilic glycoconjugate structure extracted from sapindaceae plants like Sapindus rarak. This study investigated saponin extract of Sapindus rarak as a natural template for formation of mesoporous zeolite Y. Surface area and mesoporosity of zeolite Y were improved with optimization of Sapindus rarak extract (SRE) concentration (Y-Ln; n = 2, 5, 10 or 15 mL), reaching 216.26 m2 mesoporous area and 0.214 cm3 g-1 mesoporous volume for Y-L10 samples. A different loading of Ni was impregnated onto Y-L10 zeolite to improve Lewis/Brønsted acidity as catalysts in the deoxygenation of Reutealis trisperma oil (RTO) into hydrocarbon fuels. Impregnating 15% Ni on NaY zeolite enhanced Lewis acidity to 0.4556 mmol g-1, producing 48.8% liquid oil with 85.43% degree of deoxygenation. A high selectivity towards C15 and C17 hydrocarbon was analyzed from liquid yield, indicating the contributing factor from Lewis acidity and mesoporosity to enhance deoxygenation and prevent the hydrocracking reaction.

6.
RSC Adv ; 13(45): 31989-31999, 2023 Oct 26.
Article in English | MEDLINE | ID: mdl-37915446

ABSTRACT

Conversion of red mud (RM) that contains a high level of silica, alumina and iron minerals into heterogenous catalysts, offers a route for the utilization of abundant toxic by-products of bauxite refining. In this study, the conversion of red mud into mesoporous Fe-aluminosilicate produced selective catalysts for the deoxygenation of waste cooking oil to green diesel hydrocarbons. Direct conversion of red mud in the presence cetyltrimethylammonium bromide into Fe-aluminosilicate (RM-CTA) produced a highly mesoporous structure with oligomeric Fe2O3 clusters within the pores. When red mud was treated with citric acid (RM-CA-CTA), a wide distribution of Fe2O3 particles was obtained on the aluminosilicate external surface. TEM analysis showed a well-defined hexagonal mesoporosity of Fe-aluminosilicate obtained from untreated red mud, while the treated red mud produced lower regularity mesopores. RM-CTA exhibits 60% WCO conversion and 83.72% selectivity towards liquid products with 80.44% diesel hydrocarbon (C11-C18) yield. The high selectivity was due to the high acidity of Fe-aluminosilicate to dissociate the C-O bond and the regularity of mesostructure for efficient hydrocarbon diffusion, preventing a cracking reaction.

7.
RSC Adv ; 13(21): 14236-14248, 2023 May 09.
Article in English | MEDLINE | ID: mdl-37180015

ABSTRACT

Optimization of hierarchical ZSM-5 structure by variation of the first hydrothermal step at different times provides insight into the evolution of micro/mesopores and its effect as a catalyst for deoxygenation reaction. The degree of tetrapropylammonium hydroxide (TPAOH) incorporation as an MFI structure directing agent and N-cetyl-N,N,N-trimethylammonium bromide (CTAB) as a mesoporogen was monitored to understand the effect towards pore formation. Amorphous aluminosilicate without the framework-bound TPAOH achieved within 1.5 h of hydrothermal treatment provides flexibility to incorporate CTAB for forming well-defined mesoporous structures. Further incorporation of TPAOH within the restrained ZSM-5 framework reduces the flexibility of aluminosilicate gel to interact with CTAB to form mesopores. The optimized hierarchical ZSM-5 was obtained by allowing hydrothermal condensation at 3 h, in which the synergy between the readily formed ZSM-5 crystallites and the amorphous aluminosilicate generates the proximity between micropores and mesopores. A high acidity and micro/mesoporous synergy obtained after 3 h exhibit 71.6% diesel hydrocarbon selectivity because of the improved diffusion of reactant within the hierarchical structures.

8.
Environ Sci Pollut Res Int ; 30(21): 60106-60120, 2023 May.
Article in English | MEDLINE | ID: mdl-37017846

ABSTRACT

Microplastic (MP) is an emerging contaminant of concern due to its ubiquitous quantity in the environment, small size, and potential toxicity due to strong affinity towards other contaminants. In this work, MP particles (5-300 µm) were extracted from a commercial facial cleanser and determined to be irregular polyethylene (PE) microbeads based on characterization with field emission scanning electron microscopy (FESEM) and Raman spectroscopy. The potential of extracted MP acting as toxic pollutants' vector was analyzed via adsorption of methylene blue and methyl orange dye where significant dye uptake was observed. Synthetic wastewater containing the extracted MP was subjected to a continuous-flow column study using palm kernel shell and coconut shell biochar as the filter/adsorbent media. The prepared biochar was characterized via proximate and ultimate analysis, FESEM, contact angle measurement, atomic force microscopy (AFM), and Fourier transform infrared (FTIR) spectroscopy to investigate the role of the biochar properties in MP removal. MP removal performance was determined by measuring the turbidity and weighing the dry mass of particles remaining in the effluent following treatment. Promising results were obtained from the study with highest removal of MP (96.65%) attained through palm kernel shell biochar with particle size of 0.6-1.18 mm and continuous-flow column size of 20 mm.


Subject(s)
Microplastics , Water Pollutants, Chemical , Plastics , Water Pollutants, Chemical/analysis , Wastewater , Charcoal/chemistry , Adsorption , Spectroscopy, Fourier Transform Infrared
9.
Nanoscale Adv ; 4(13): 2836-2843, 2022 Jun 28.
Article in English | MEDLINE | ID: mdl-36131999

ABSTRACT

The effect of the copper (Cu) content on Cu oxide loaded onto a carbon nanotube (CuO/CNT) catalyst on the mechanistic, kinetic, and photonic efficiency of the photodegradation of p-chloroaniline (PCA) under visible (Vis) and ultraviolet (UV) light irradiation has been explored. For low-loading (1-5 wt%) CuO/CNTs, photodegradation performed better under UV (>84%) rather than the Vis system; this may be due to the presence of abundant defect sites on both CuO and CNTs, which allowed the multielectron reduction of oxygen at their impurity levels to generate more hydrogen peroxide and subsequent ·OH radicals. The active species under UV were in the following order: h+ ≫ e- > ·OH, while it was vice versa for the Vis system with a well-balanced 50 wt% CuO/CNT catalyst that exhibited a similar performance. The kinetic study showed the transition of the kinetic order from the zeroth to the first order on increasing the PCA concentration under the Vis system and vice versa for the UV system. The Thiele modulus (ϕ) further confirmed that the effect of internal mass transfer was negligible under UV light. In contrast, the transition from mass transfer to kinetic control limitation was observed under the Vis system. The optimum PCA degradation predicted from the response surface analysis was 97.36% at the reaction pH of 7.3, catalyst dosage of 0.45 g L-1, and initial PCA concentration of 11.02 mg L-1. The condition obtained was fairly close to the forecasted value with an error of 0.26%.

10.
RSC Adv ; 12(3): 1604-1627, 2022 Jan 05.
Article in English | MEDLINE | ID: mdl-35425206

ABSTRACT

Sustainable renewable energy production is being intensely disputed worldwide because fossil fuel resources are declining gradually. One solution is biodiesel production via the transesterification process, which is environmentally feasible due to its low-emission diesel substitute. Significant issues arising with biodiesel production are the cost of the processes, which has stuck its sustainability and the applicability of different resources. In this article, the common biodiesel feedstock such as edible and non-edible vegetable oils, waste oil and animal fats and their advantages and disadvantages were reviewed according to the Web of Science (WOS) database over the timeframe of 1970-2020. The biodiesel feedstock has water or free fatty acid, but it will produce soap by reacting free fatty acids with an alkali catalyst when they present in high portion. This reaction is unfavourable and decreases the biodiesel product yield. This issue can be solved by designing multiple transesterification stages or by employing acidic catalysts to prevent saponification. The second solution is cheaper than the first one and even more applicable because of the abundant source of catalytic materials from a waste product such as rice husk ash, chicken eggshells, fly ash, red mud, steel slag, and coconut shell and lime mud. The overview of the advantages and disadvantages of different homogeneous and heterogeneous catalysts is summarized, and the catalyst promoters and prospects of biodiesel production are also suggested. This research provides beneficial ideas for catalyst synthesis from waste for the transesterification process economically, environmentally and industrially.

11.
ACS Omega ; 7(4): 3324-3340, 2022 Feb 01.
Article in English | MEDLINE | ID: mdl-35128243

ABSTRACT

Solvent-based recycling of plastic can offer the main improvement when it is employed for pyrolysis-catalytic steam reforming. In this research, plastic waste dissolved in phenol was used as a feed for catalytic cracking and steam reforming reactions for valuable liquid fuels and hydrogen production, which is gaining the attention of researchers globally. Microplastic wastes (MPWs) are tiny plastic particles that arise due to product creation and breakdown of larger plastics. They can be found mainly in several habitats, including seas and freshwater ecosystems. MPWs harm aquatic species, turtles, and birds and were chosen to recover in this study that can be reacted on the catalyst surface. Biphasic anatase-rutile TiO2 with spherical-shaped support for Ni and Pd metals with nanosized particles was synthesized via the hydrothermal treatment method, and its chemical and physical properties were characterized accordingly. According to temperature-programmed desorption of carbon dioxide (CO2-TPD) and temperature-programmed reduction of hydrogen (H2-TPR) results, the incorporation of Pd into Ni/TNPs enhanced the basicity of the support surface and the redox properties of catalysts, which were strongly linked to the improved hydrogen yield (71%) and phenol conversion (79%) at 600 °C. The Ni-Pd/TNPs nanocatalyst, with remarkable stability for 72 h of time on stream, is a promising catalyst for the MPW-phenol cracking and steam reforming reactions toward H2 production for clean energy generation and other environmental applications. Besides, this study has also highlighted the opportunities of overcoming the risk of microplastic waste and converting it into valuable fuels such as decamethyltetrasiloxane, phenanthrene, methyl palmitate, benzenepropanoic acid, benzoic acid, azulene, xanthene, anisole, biphenyl, phthalic acid, diisooctyl phthalate, etc.

12.
Int J Biol Macromol ; 204: 593-605, 2022 Apr 15.
Article in English | MEDLINE | ID: mdl-35157900

ABSTRACT

Conversion of lignocellulosic biowastes from agricultural industry into nanocrystalline cellulose provides pathway to reduce environmental pollution while enhancing the economic value of biowastes. Nanocellulose (NCC) with uniform morphology was isolated from pepper (Piper nigrum L.) stalk waste (PW) using acid hydrolysis method. The role of inorganic acids (sulfuric acid, hydrochloric acid, phosphoric acid), organic acids (oxalic acid, citric acid, acetic acid) and variation of sonication times were investigated on the physicochemical characteristics, self-assembled structure, crystallinity, particle size, zeta potential and thermal stability of the isolated nanocellulose. Hydrolysis using inorganic acids transformed cellulose from PW into a spherical shaped NCC at ~33-67 nm of average diameter. Meanwhile hydrolysis in organic acids produced rod-shaped NCC at 210-321 nm in length. This study highlighted the role of acidity strength for organic acid and inorganic acid in controlling the level of hydrogen bond dissociation and the dissolution of amorphous fragments, which consequently directing the morphology and the physicochemical properties of NCCs.


Subject(s)
Industrial Waste , Piper nigrum , Cellulose/chemistry , Hydrolysis , Particle Size
13.
Environ Chem Lett ; 20(2): 1421-1451, 2022.
Article in English | MEDLINE | ID: mdl-35018167

ABSTRACT

Water contamination is an environmental burden for the next generations, calling for advanced methods such as adsorption to remove pollutants. For instance, unwanted biowaste and invasive plants can be converted into biosorbents for environmental remediation. This would partly solve the negative effects of invasive plants, estimated at 120 billion dollars in the USA. Here we review the distribution, impact, and use of invasive plants for water treatment, with emphasis on the preparation of biosorbents and removal of pollutants such as cadmium, lead, copper, zinc, nickel, mercury, chromate, synthetic dyes, and fossil fuels. Those biosorbents can remove 90-99% heavy metals from aqueous solutions. High adsorption capacities of 476.190 mg/g for synthetic dyes and 211 g/g for diesel oils have been observed. We also discuss the regeneration of these biosorbents.

14.
Environ Chem Lett ; 20(2): 1309-1331, 2022.
Article in English | MEDLINE | ID: mdl-35035338

ABSTRACT

Pollution and diseases such as the coronavirus pandemic (COVID-19) are major issues that may be solved partly by nanotechnology. Here we review the synthesis of ZrO2 nanoparticles and their nanocomposites using compounds from bacteria, fungi, microalgae, and plants. For instance, bacteria, microalgae, and fungi secret bioactive metabolites such as fucoidans, digestive enzymes, and proteins, while plant tissues are rich in reducing sugars, polyphenols, flavonoids, saponins, and amino acids. These compounds allow reducing, capping, chelating, and stabilizing during the transformation of Zr4+ into ZrO2 nanoparticles. Green ZrO2 nanoparticles display unique properties such as a nanoscale size of 5-50 nm, diverse morphologies, e.g. nanospheres, nanorods and nanochains, and wide bandgap energy of 3.7-5.5 eV. Their high stability and biocompatibility are suitable biomedical and environmental applications, such as pathogen and cancer inactivation, and pollutant removal. Emerging applications of green ZrO2-based nanocomposites include water treatment, catalytic reduction, nanoelectronic devices, and anti-biofilms.

15.
Chemosphere ; 288(Pt 2): 132535, 2022 Feb.
Article in English | MEDLINE | ID: mdl-34648794

ABSTRACT

The growing prevalence of new toxins in the environment continues to cause widespread concerns. Pharmaceuticals, organic pollutants, heavy metal ions, endocrine-disrupting substances, microorganisms, and others are examples of persistent organic chemicals whose effects are unknown because they have recently entered the environment and are displaying up in wastewater treatment facilities. Pharmaceutical pollutants in discharged wastewater have become a danger to animals, marine species, humans, and the environment. Although their presence in drinking water has generated significant concerns, little is known about their destiny and environmental effects. As a result, there is a rising need for selective, sensitive, quick, easy-to-handle, and low-cost early monitoring detection systems. This study aims to deliver an overview of a low-cost carbon-based composite to detect and remove pharmaceutical components from wastewater using the literature reviews and bibliometric analysis technique from 1970 to 2021 based on the web of science (WoS) database. Various pollutants in water and soil were reviewed, and different methods were introduced to detect pharmaceutical pollutants. The advantages and drawbacks of varying carbon-based materials for sensing and removing pharmaceutical wastes were also introduced. Finally, the available techniques for wastewater treatment, challenges and future perspectives on the recent progress were highlighted. The suggestions in this article will facilitate the development of novel on-site methods for removing emerging pollutants from pharmaceutical effluents and commercial enterprises.


Subject(s)
Pharmaceutical Preparations , Wastewater , Carbon , Humans
16.
Sci Total Environ ; 810: 152115, 2022 Mar 01.
Article in English | MEDLINE | ID: mdl-34896138

ABSTRACT

The presence of microplastics (MP) and nanoplastics (NP) in the environment poses significant hazards towards microorganisms, humans, animals and plants. This paper is focused on recent literature studies and patents discussing the removal process of these plastic pollutants. Microplastics and nanoplastics can be quantified by counting, weighing, absorbance and turbidity and can be further analyzed using scanning electron microscopy (SEM), dynamic light scattering (DLS), Fourier transform infrared spectroscopy (FTIR), Raman spectroscopy, surface-enhanced Raman spectroscopy and Raman tweezers. Mitigation methods reported are categorized depending on the removal characteristics: (i) Filtration and separation method: Filtration and separation, electrospun nanofiber membrane, constructed wetlands; (ii) Capture and surface attachment method: coagulation, flocculation and sedimentation (CFS), electrocoagulation, adsorption, magnetization, micromachines, superhydrophobic materials and microorganism aggregation; and (iii) Degradation method: photocatalytic degradation, microorganism degradation and thermal degradation; where removal efficiency between 58 and 100% were reported. As these methods are significantly distinctive, the parameters which affect the MP/NP removal performance e.g., pH, type of plastics, presence of interfering chemicals or ions, surface charges etc. are also discussed. 42 granted international patents related to microplastics and nanoplastics removal are also reviewed where the majority of these patents are focused on separation or filtration devices. These devices are efficient for microplastics up to 20 µm but may be ineffective for nanoplastics or fibrous plastics. Several patents were found to focus on methods similar to literature studies e.g., magnetization, CFS, biofilm and microorganism aggregation; with the addition of another method: thermal degradation.


Subject(s)
Microplastics , Water Pollutants, Chemical , Flocculation , Humans , Plastics , Wastewater , Water Pollutants, Chemical/analysis
17.
Environ Sci Pollut Res Int ; 28(28): 37354-37370, 2021 Jul.
Article in English | MEDLINE | ID: mdl-33712959

ABSTRACT

Red mud as industrial waste from bauxite was utilized as a precursor for the synthesis of mesoporous ZSM-5. A high concentration of iron oxide in red mud was successfully removed using alkali fusion treatment. Mesoporous ZSM-5 was synthesized using cetyltrimethylammonium bromide (CTABr) as a template via dual-hydrothermal method, and the effect of crystallization time was investigated towards the formation of mesopores. Characterization using X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FTIR), N2 adsorption-desorption, scanning electron microscopy (SEM), and transmission electron microscopy (TEM) indicated the formation of cubic crystallite ZSM-5 with high surface area and mesopore volume within 6 h of crystallization. Increasing the crystallization time revealed the evolution of highly crystalline ZSM-5; however, the surface area and mesoporosity were significantly reduced. The effect of mesoporosity was investigated on the adsorption of methylene blue (MB). Kinetic and thermodynamic analysis of MB adsorption on mesoporous ZSM-5 was carried out at a variation of adsorption parameters such as the concentration of MB solution, the temperatures of solution, and the amount of adsorbent. Finally, methanol, 1-butanol, acetone, hydrochloric acid (HCl), and acetonitrile were used as desorbing agents to investigate the reusability and stability of mesoporous ZSM-5 as an adsorbent for MB removal.


Subject(s)
Methylene Blue , Water Pollutants, Chemical , Adsorption , Kinetics , Microscopy, Electron, Transmission , Spectroscopy, Fourier Transform Infrared , X-Ray Diffraction
18.
RSC Adv ; 11(36): 21885-21896, 2021 Jun 21.
Article in English | MEDLINE | ID: mdl-35480811

ABSTRACT

The activity of mesoporous Al-MCM-41 for deoxygenation of Reutealis trisperma oil (RTO) was enhanced via modification with NiO nanoparticles. Deoxygenation at atmospheric pressure and under H2 free conditions required acid catalysts to ensure the removal of the oxygenated fragments in triglycerides to form liquid hydrocarbons. NiO at different weight loadings was impregnated onto Al-MCM-41 and the changes of Lewis/Brønsted acidity and mesoporosity of the catalysts were investigated. The activity of Al-MCM-41 was enhanced when impregnated with NiO due to the increase of Lewis acidity originating from NiO nanoparticles and the mesoporosity of Al-MCM-41. Increasing the NiO loading enhanced the Lewis acidity but not Brønsted acidity, leading to a higher conversion towards liquid hydrocarbon yield. Impregnation with 10% of NiO on Al-MCM-41 increased the conversion of RTO to hydrocarbons via the deoxygenation pathway and reduced the products from cracking reaction, consequently enhancing the green diesel (C11-C18) hydrocarbon products.

19.
RSC Adv ; 11(27): 16376-16387, 2021 Apr 30.
Article in English | MEDLINE | ID: mdl-35479131

ABSTRACT

Catalytic CO2 hydrogenation to CH4 offers a viable route for CO2 conversion into carbon feedstock. The research aimed to enhance CO2 conversion at low temperature and to increase the stability of Ni catalysts using zeolite as a support. NaZSM-5 (MFI), NaA (LTA), NaY (FAU), and NaBEA (BEA) synthesized from kaolin were impregnated with 15% Ni nanoparticles in order to elucidate the effect of surface area, porosity and basicity of the zeolite in increasing Ni activity at mild temperature of ∼200 °C. A highly dispersed Ni catalyst was produced on high surface area NaY meanwhile the mesoporosity of ZSM-5 has no significant effect in improving Ni dispersion. However, the important role of zeolite mesoporosity was observed on the stability of the catalyst. Premature deactivation of Ni/NaA within 10 h was due to the relatively small micropore size that restricted the CO2 diffusion, meanwhile Ni/NaZSM-5 with a large mesopore size exhibited catalytic stability for 40 h of reaction. Zeolite NaY enhanced Ni activity at 200 °C to give 21% conversion with 100% CH4 selectivity. In situ FTIR analysis showed the formation of hydrogen carbonate species and formate intermediates at low temperatures on Ni/NaY, which implied the efficiency of electron transfer from the basic sites of NaY during CO2 reduction. The combination of Ni/NaY interfacial interaction and NaY surface basicity promoted CO2 methanation reaction at low temperature.

20.
Inorg Chem ; 59(3): 1723-1735, 2020 Feb 03.
Article in English | MEDLINE | ID: mdl-31961141

ABSTRACT

Phosphate and nitrate were loaded on silica BEA (P/HSi@BEA and N/HSi@BEA), which is fibrously protonated by the impregnation method for n-hexane and cyclohexane isomerization. The characterization analysis specified the removal of tetrahedral aluminum atoms in the framework, which was triggered by the existence of phosphate and nitrate groups in the catalyst. The exchanged role of Si(OH)Al to P-OH as active acidic sites in the P/HSi@BEA catalyst reduced its acidic strength, which was confirmed by the FTIR results. Lewis acidic sites of P/HSi@BEA performance are a significant part in the generation of high protonic acid sites, as proven by the in situ ESR study. However, FTIR evacuation and 27Al NMR revealed that the reduction in the amount of extraframework Al (EFAl) is due to its interaction with the nitrate group on the outside of the catalyst surface. The N/HSi@BEA catalyst exhibited high acidic strength because of the existence of more Si(OH)Al, which was initiated during the nitrate-incorporation process. Of significance is that the catalytic performance of n-hexane isomerization in the presence of hydrogen reached 50.3% product isomer yield at 250 °C, which might be ascribed to the presence of P-OH active sites that are responsible for accepting electrons, forming active protonic acid sites. NO3-EFAl interaction induced the formation of Brønsted acid sites, and higher mesopore volume favors the production of cyclohexane isomers up to 48.4% at 250 °C. This fundamental study exhibits that significant interactions given by such phosphate and nitrate groups with the unique silica fibrous BEA support could enhance isomerization, which contributes to the high quality of fuel.

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