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1.
Sci Rep ; 12(1): 15271, 2022 Sep 10.
Artigo em Inglês | MEDLINE | ID: mdl-36088488

RESUMO

Mesoporous silica NSG had been synthesized while employing gelatin as a natural template to successfully increase the particle size and expand the pore diameter of NSG. All silica samples exhibited a similar XRD pattern with a broad peak centred at 2θ = 22.9°, as the characteristic of amorphous silica. FTIR results showed that the reduction of Si-O-Si symmetric stretching vibrations at 1075 cm-1 was due to the use of a high percentage of gelatin. Moreover, TEM analysis displayed the mesoporous channels in the form of a honeycomb structure with a diameter of ± 6 nm. Gelatin enhanced the surface area of silica from 467 to 510 m2/g, the pore volume from 0.64 to 0.72 cc/g and expanded the pore diameter from 3.5 nm to 6.0 nm. The expansion of the ordered mesopores with the increase of P123: gelatin ratios was elucidated by the pore size distribution. The adsorption capacity of methylene blue (MB) was improved on mesoporous silica with an expanded pore dimension to give 168 mg/g adsorption capacity within 70 min.


Assuntos
Azul de Metileno , Dióxido de Silício , Adsorção , Gelatina , Porosidade , Dióxido de Silício/química
2.
Materials (Basel) ; 15(16)2022 Aug 09.
Artigo em Inglês | MEDLINE | ID: mdl-36013608

RESUMO

TiO2/SBA-15 photocatalysts were successfully prepared by impregnating low loading titania to SBA-15 via slow calcination. The photocatalyst is efficient for fast methylene blue removal via adsorption and photodegradation methods. The impregnation of low TiO2 loading via slow calcination enhanced TiO2 dispersion that preserved the SBA-15 porosity and uniform morphology. High interfacial interaction of TiO2/SBA-15 improves TiO2 photoresponse by narrowing the bandgap, resulting in a stronger redox ability. The methylene blue removal on 10%TiO2/SBA-15 followed the pseudo-second-order kinetic model that reached 67% removal efficiency in 90 min. The synergy between adsorption and photodegradation is responsible for the fast methylene blue removal. These results indicate the importance of maintaining the adsorption capacity in SBA-15 after impregnation with TiO2 for efficient adsorption-photodegradation processes, which can be achieved by controlling the deposition of TiO2 on SBA-15. A low titania loading further reduced the cost of photocatalysts, thus becoming a potential material for environmental pollution treatment.

3.
Materials (Basel) ; 15(8)2022 Apr 08.
Artigo em Inglês | MEDLINE | ID: mdl-35454437

RESUMO

Mesoporous sodalite nanoparticles were directly synthesized from Indonesian kaolin with the addition of CTABr as a mesopore template. The studies highlighted the importance of aging time (3-12 h) and temperature (50-80 °C) on increasing surface area and mesoporosity of sodalite. Indonesian kaolin was used without pre-treatment and transformed to sodalite following the initial molar composition of 10 Na2O: 2 SiO2: Al2O3: 128 H2O. Characterization data revealed the formation of high surface area sodalite with mesoporosity at increasing aging temperatures and times. The presence of CTABr as templates produced sodalites nanoparticles with smaller aggregates than the non-template sodalite. The sodalite sample obtained at 80 °C of crystallization temperature for 9 h (S80H9) displayed the highest mesopore volume (0.07612 cm3/g) and the highest adsorption capacity of Pb2+ (212.24 mg/g). Pb2+ was suggested to adsorb via ion exchange with the Na+ counter cation and physical adsorption.

4.
Int J Biol Macromol ; 204: 593-605, 2022 Apr 15.
Artigo em Inglês | MEDLINE | ID: mdl-35157900

RESUMO

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.


Assuntos
Resíduos Industriais , Piper nigrum , Celulose/química , Hidrólise , Tamanho da Partícula
5.
Materials (Basel) ; 14(22)2021 Nov 10.
Artigo em Inglês | MEDLINE | ID: mdl-34832181

RESUMO

Hematite (α-Fe2O3) with uniform hexagonal flake morphology has been successfully synthesized using a combination of gelatin as natural template with F127 via hydrothermal method. The resulting hematite was investigated as adsorbent and photocatalyst for removal of ibuprofen as pharmaceutical waste. Hexagonal flake-like hematite was obtained following calcination at 500 °C with the average size was measured at 1-3 µm. Increasing the calcination temperature to 700 °C transformed the uniform hexagonal structure into cubic shape morphology. Hematite also showed high thermal stability with increasing the calcination temperatures; however, the surface area was reduced from 47 m2/g to 9 m2/g. FTIR analysis further confirmed the formation Fe-O-Fe bonds, and the main constituent elements of Fe and O were observed in EDX analysis for all samples. α-Fe2O3 samples have an average adsorption capacity of 55-25.5 mg/g at 12-22% of removal efficiency when used as adsorbent for ibuprofen. The adsorption capacity was reduced as the calcination temperatures increased due to the reduction of available surface area of the hexagonal flakes after transforming into cubes. Photocatalytic degradation of ibuprofen using hematite flakes achieved 50% removal efficiency; meanwhile, combination of adsorption and photocatalytic degradation further removed 80% of ibuprofen in water/hexane mixtures.

6.
Faraday Discuss ; 230(0): 52-67, 2021 Jul 16.
Artigo em Inglês | MEDLINE | ID: mdl-33870391

RESUMO

The combination of a methanol synthesis catalyst and a solid acid catalyst opens the possibility to obtain olefins or paraffins directly from CO2 and H2 in one step. In this work several PdZn/TiO2-ZSM-5 hybrid catalysts were employed under CO2 hydrogenation conditions (240-360 °C, 20 bar, CO2/N2/H2 = 1 : 1 : 3) for the synthesis of CH3OH, consecutive dehydration to dimethyl ether and further oxygenate conversion to hydrocarbons. No significant changes after 36 h reaction on the methanol synthesis catalyst (PdZn/TiO2) were observed by XRD, XAS or XPS. No olefins were observed, indicating that light olefins undergo further hydrogenation under the reaction conditions, yielding the corresponding alkanes. Increasing the aluminium sites in the zeolites (Si : Al ratio 80 : 1, 50 : 1 and 23 : 1) led to a higher concentration of mild Brønsted acid sites, promoting hydrocarbon chain growth.

7.
Environ Sci Pollut Res Int ; 28(28): 37354-37370, 2021 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-33712959

RESUMO

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.


Assuntos
Azul de Metileno , Poluentes Químicos da Água , Adsorção , Cinética , Microscopia Eletrônica de Transmissão , Espectroscopia de Infravermelho com Transformada de Fourier , Difração de Raios X
8.
RSC Adv ; 11(27): 16376-16387, 2021 Apr 30.
Artigo em Inglês | MEDLINE | ID: mdl-35479131

RESUMO

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.

9.
RSC Adv ; 11(36): 21885-21896, 2021 Jun 21.
Artigo em Inglês | MEDLINE | ID: mdl-35480811

RESUMO

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.

10.
RSC Adv ; 11(50): 31807-31816, 2021 Sep 21.
Artigo em Inglês | MEDLINE | ID: mdl-35496871

RESUMO

Low temperature CO2 methanation is a favorable pathway to achieve high selectivity to methane while increasing the stability of the catalysts. A Ba promoted Ni/Sm2O3 catalyst was investigated for CO2 methanation at atmospheric pressure with the temperature ranging from 200-450 °C. 5Ni-5Ba/Sm2O3 showed significant enhancement of CO2 conversion particularly at temperatures ≤ 300 °C compared to Ni/Sm2O3. Incorporation of Ba into 5Ni/Sm2O3 improved the basicity of the catalysts and transformed the morphology of Sm2O3 from random structure into uniform groundnut shape nanoparticles. The uniformity of Sm2O3 created interparticle porosity that may be responsible for efficient heat transfer during a long catalytic reaction. Ba is also postulated to catalyze oxygen vacancy formation on Sm2O3 under a reducing environment presumably via isomorphic substitution. The disappearance of a high temperature (∼600 °C) reduction peak in H2-TPR analysis revealed the reducibility of NiO following impregnation with Ba. However, further increasing the Ba loading to 15% formed BaNiO3-BaNiO2.36 phases which consequently reduced the activity of the Ni-Ba/Sm2O3 catalyst at low temperature. Ni was suggested to segregate from BaNiO3-BaNiO2.36 at high temperature thus exhibiting comparable activity with Ni/Sm2O3 at 450 °C.

11.
Sci Total Environ ; 711: 135066, 2020 Apr 01.
Artigo em Inglês | MEDLINE | ID: mdl-32000337

RESUMO

Size tunable mesoporous carbon microspheres, MCMs were obtained using Pluronic F127 and gelatin in co-templating method via hydrothermal and pyrolysis treatments. The presence of gelatin increased the mechanical strength of Pluronic F127 which can sustain the uniform microspherical structure of carbon following pyrolysis at 950 °C. The diameter of MCMs were controlled by variation of weight ratios between Pluronic F127 to gelatin from 1:0.01 to 1:1. MCMs exhibited inter-particulate mesoporous structure with high thermal stability (<500 °C). The MCMs were used as adsorbent for removal of ibuprofen and the kinetic studies using linear regression analysis revealed the adsorption fits pseudo second-order kinetic. The rate of adsorption and the amount of adsorbed ibuprofen were correlated well with the surface area and the crystallite size of MCMs. The efficiencies of ibuprofen adsorption on MCMs were also investigated when ibuprofen was dissolved at different concentration of water and hexane mixtures, the effect temperature variation and the amount MCMs to the volume of ibuprofen solution.


Assuntos
Microesferas , Carbono , Gelatina , Ibuprofeno , Cinética , Poloxâmero
12.
Phys Chem Chem Phys ; 21(29): 16154-16160, 2019 Jul 24.
Artigo em Inglês | MEDLINE | ID: mdl-31294427

RESUMO

The interaction between Pd and TiO2 for promoting photocatalytic activity was investigated by tailoring the size of Pd nanoparticles and monitoring the photocatalytic activity of methanol photo-reforming reaction for hydrogen gas production. We show that at 0.6 wt% Pd loading, the catalyst with highly dispersed nanoparticles obtained at 1 °C temperature exhibits superior photocatalytic activity for hydrogen gas production. At different weights of Pd loading, tailoring two sets of catalysts with different structural properties provides correlation between the changes in the Pd local structures and the rate of hydrogen production. The impact of controlling the structural properties of metal nanoparticles on influencing H2 production outweighs the effect of metal loading variation. The differences of Pd/TiO2 activity at the different metal loadings were correlated with the changes in the Pd local structure consequently affecting the electronic transfer and photocatalytic efficiency.

13.
Top Catal ; 61(3): 144-153, 2018.
Artigo em Inglês | MEDLINE | ID: mdl-30930591

RESUMO

Catalytic upgrading of CO2 to value-added chemicals is an important challenge within the chemical sciences. Of particular interest are catalysts which are both active and selective for the hydrogenation of CO2 to methanol. PdZn alloy nanoparticles supported on TiO2 via a solvent-free chemical vapour impregnation method are shown to be effective for this reaction. This synthesis technique is shown to minimise surface contaminants, which are detrimental to catalyst activity. The effect of reductive heat treatments on both structural properties of PdZn/TiO2 catalysts and rates of catalytic CO2 hydrogenation are investigated. PdZn nanoparticles formed upon reduction showed high stability towards particle sintering at high reduction temperature with average diameter of 3-6 nm to give 1710 mmol kg-1 h of methanol. Reductive treatment at high temperature results in the formation of ZnTiO3 as well as PdZn, and gives the highest methanol yield.

14.
Sci Total Environ ; 563-564: 921-32, 2016 Sep 01.
Artigo em Inglês | MEDLINE | ID: mdl-26524993

RESUMO

Novel nanomaterials based on doped TiO2 nanoparticles with different morphological, textural and band-gap properties have been synthesized using scalable methods. The influence of synthetic parameters such as titanium source (titanium(IV) isopropoxide and titanium(IV) butoxide), doping quantity (0%, 2% or 5% Zn), acidic solution for the hydrolysis reaction (ascorbic acid, nitric acid) and calcination temperatures (500°C and 600°C) was simultaneously investigated. The obtained nanomaterials were characterized by different methods and photocatalytic tests of methylene blue (MB) degradation under UV-light were conducted to determine their activity. The results revealed that the synthesized nanomaterials are porous aggregates with very high crystallinity and are mainly composed of the anatase phase; although their physical properties vary depending on the different synthetic parameters employed. These changes are able to modify the apparent rate constant of the degradation of MB up to one order of magnitude, indicating, substantial changes in their photoactivity. Hybrid materials TiO2-Pd nanoparticles have also been prepared, characterized and tested for hydrogen production using photocatalytic methanol reforming where supported palladium nanoparticles acted as co-catalyst. Furthermore, the hybrid materials TiO2-Pd nanoparticles were studied in photocatalytic tests of methylene blue degradation under visible LED-light. The results obtained in the production of hydrogen from the photocatalytic reforming of methanol by hybrid materials suggest that the reported hybrid systems could be suitable photocatalysts for future sustainable hydrogen production upon tuning of the morphological, textural and band gap energy properties to allow processes to be carried out under visible light.


Assuntos
Hidrogênio/química , Nanopartículas Metálicas/química , Metanol/química , Titânio/química , Eliminação de Resíduos Líquidos/métodos , Poluentes Químicos da Água/química , Química Verde , Azul de Metileno/química , Fotólise , Raios Ultravioleta
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