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1.
ACS Omega ; 9(6): 6749-6760, 2024 Feb 13.
Artículo en Inglés | MEDLINE | ID: mdl-38371817

RESUMEN

Ethylene, a plant hormone, is a gas that plays a crucial role in fruit ripening and senescence. In this work, a novel ethylene scavenger was prepared from amorphous silica-alumina derived from sugar cane bagasse ash (SC-ASA) and used to prolong the shelf life of mango fruits during storage. KMnO4 at 2, 4, or 6 wt %/w was loaded on SC-ASA using an impregnation method. The results showed that 4% w/w KMnO4 loaded on SC-ASA (4KM/SC-ASA) was superior for ethylene removal at an initial ethylene concentration of 400 µL L-1 for 120 min under ambient conditions (25-27 °C and 70-75% relative humidity), resulting in 100% ethylene removal. The kinetic study of ethylene removal showed that the adsorption data were best fitted with a pseudo-first-order kinetic model. The effects of 4KM/SC-ASA as sachets on the quality changes of the mango fruits were investigated, with the results showing that mango fruits packed in cardboard boxes with 4KM/SC-ASA had significantly delayed ripening, low levels of ethylene production, respiration, and weight loss, high fruit firmness, low total soluble solids, and high acidity compared to those of the control treatment. These findings should contribute to developing an ethylene scavenger to extend the shelf life of fruits, reduce the waste of the sugar and ethanol industries, and make it a valuable material.

2.
Chemosphere ; 351: 141140, 2024 Mar.
Artículo en Inglés | MEDLINE | ID: mdl-38190943

RESUMEN

Oxides of silicon (Si), manganese (Mn), and zinc (Zn) have been used as soil amendments to reduce As mobility and uptake in paddy soil systems. However, these amendments are hypothesized to be affected differently depending on the soil pH and their effect on As speciation in rice paddy systems is not fully understood. Herein, we used a microcosm experiment to investigate the effects of natural Si-rich fly ash and synthetic Mn and Zn oxides on the temporal development of porewater chemistry, including aqueous As speciation (As(III), As(V), MMA, DMA, and DMMTA) and solid-phase As solubility, in a naturally calcareous soil with or without soil acidification (with sulfuric acid) during 28 days of flooding and subsequent 14 days of drainage. We found that soil acidification to pH 4.5 considerably increased the solubility of Si, Fe, Mn, and Zn compared to the non-acidified soil. Additions of Mn and Zn oxides decreased the concentrations of dissolved arsenite and arsenate in the non-acidified soil whereas additions of Zn oxide and combined Si-Zn oxides increased them in the acidified soil. The Si-rich fly ash did not increase dissolved Si and As in the acidified and non-acidified soils. Dimethylated monothioarsenate (DMMTA) was mainly observed in the acidified soil during the later stage of soil flooding. The initial 28 days of soil flooding decreased the levels of soluble and exchangeable As and increased As associated with Mn oxides, whereas the subsequent 14 days of soil drainage reversed the trend. This study highlighted that soil acidification considerably controlled the solubilization of Ca and Fe, thus influencing the soil pH-Eh buffering capacity, the solubility of Si, Mn, and Zn oxides, and the mobility of different As species in carbonate-rich and acidic soils under redox fluctuations.


Asunto(s)
Arsénico , Oryza , Contaminantes del Suelo , Óxido de Zinc , Arsénico/análisis , Manganeso/farmacología , Suelo , Silicio/farmacología , Ceniza del Carbón/farmacología , Óxido de Zinc/farmacología , Óxidos/farmacología , Compuestos Orgánicos/farmacología , Zinc/farmacología , Contaminantes del Suelo/análisis
3.
Ind Eng Chem Res ; 62(40): 16254-16267, 2023 Oct 11.
Artículo en Inglés | MEDLINE | ID: mdl-37841414

RESUMEN

The greenhouse gas reduction as well as the utilization of more renewable and clean energy via a dry reforming reaction is of interest. The impact of a CeMgZnAl oxide quad-blend-supported Ni catalyst on performance and anticoking during dry reforming reactions at 700 °C was studied. A high Ce-Mg/Zn ratio, as seen in the CeMg0.5ZnAl-supported nickel catalyst, enhances lattice oxygen, and the presence of strong basic sites, along with the creation of the carbonate intermediate species, is accompanied by the production of gaseous CO through a gasification reaction between the carbon species and Ni-COads-lin site. The phenomena caused the outstanding performance of the Ni/CeMg0.5ZnAl catalyst-CH4 (84%),CO2 (83%) conversions, and the H2/CO (0.80) ratio; moreover, its activity was also stable throughout 30 h.

4.
Sci Rep ; 13(1): 15311, 2023 09 15.
Artículo en Inglés | MEDLINE | ID: mdl-37714873

RESUMEN

Cigarette smoke contains many chemicals, including nicotine, which is harmful and can cause health problems such as carcinogenesis disease, cardiovascular, respiratory, renal, and reproductive systems. Removal of nicotine from mainstream smoke can be done through adsorption with filters or solid adsorbents. In this study, we explored the use of activated carbons for the removal of nicotine from cigarette mainstream smoke. Activated carbons were prepared from dried hemp (Cannabis sativa) stem at an activation temperature of 350-550 °C using phosphoric acid as an activating agent. The results showed that the activated carbons with variable surface functional groups and porosity exhibited high efficiency for nicotine adsorption, removing 68-88% of nicotine from cigarette mainstream smoke. Through X-ray photoelectron spectroscopy and temperature-programmed desorption analyses, we identified that oxygen-containing functional groups, particularly carboxylic groups, exhibited a superior ability to adsorb nicotine. The computational analysis with DFT simulations further supported the importance of oxygen-containing surface functional groups in facilitating nicotine adsorption, with the carboxylic group providing the lowest adsorption energy among other functional groups.


Asunto(s)
Fumar Cigarrillos , Nicotina , Humanos , Adsorción , Carcinogénesis , Carbón Orgánico , Oxígeno
5.
Environ Res ; 237(Pt 1): 116957, 2023 Nov 15.
Artículo en Inglés | MEDLINE | ID: mdl-37634694

RESUMEN

This study investigates the use of a hexagonal-porous aluminosilicate (HAS) adsorbent derived from bagasse bottom ash (BBA), an agricultural solid waste, for the adsorption of ammonia nitrogen (NH3-N)-a key water pollutant from agricultural and farming activities. Sodium silicate derived from BBA via the alkaline fusion method was employed, resulting in energy savings due to a synthesis temperature 1.53 times lower than that of commercial sodium silicate synthesis. The sol-gel method was utilized to successfully synthesize HAS featuring a high surface area and porosity using the sodium silicate prepared from BBA. However, an increase in aluminum content resulted in a decrease in surface area and hexagonal porosity. In performance tests, the HAS(5) adsorbent exhibited the most efficient NH3-N removal, outperforming other adsorbents by 4.54-25.19 times across all initial concentrations. This enhanced efficiency can be attributed to its numerous acidic surface sites, enabling the bonding of NH3-N molecules through monolayer adsorption on the HAS surface.

6.
Environ Res ; 236(Pt 1): 116742, 2023 11 01.
Artículo en Inglés | MEDLINE | ID: mdl-37507043

RESUMEN

This study investigates the impact of microporous (SP-C) and micro-mesoporous carbon (DP-C) supports on the dispersion and phase transformation of iron oxides and their arsenic (V) removal efficiency. The research demonstrates that carbon-supported iron oxide sorbents exhibit superior As(V) uptake capacity compared to unsupported Fe2O3, attributed to reduced iron oxide crystallite sizes and As(V) adsorption on carbon supports. Maximum As(V) uptake capacities of 23.8 mg/g and 18.9 mg/g were achieved for Fe/SP-C and Fe/DP-C at 30 wt% and 50 wt% iron loading, respectively. The study reveals a nonlinear relationship between As(V) sorption capacity and iron oxide crystallite size after excluding As(V) adsorption capacity on carbon supports, suggesting the iron oxide phase (Fe3O4) plays a role in determining adsorption capacity. Iron oxide-loaded DP-C sorbents exhibit faster adsorption rates at low As(V) concentrations (5 mg/L) than SP-C sorbents due to their bimodal pore structure. Adsorption behavior varies at higher As(V) concentrations (45 mg/L), with Fe/DP-C reaching maximum capacity more slowly due to limited available adsorptive sites. All adsorbents maintained near-complete As(V) removal efficiency over five cycles. The findings provide insights for designing more efficient adsorbents for As(V) removal from contaminated water sources.


Asunto(s)
Arsénico , Contaminantes Químicos del Agua , Purificación del Agua , Carbono , Contaminantes Químicos del Agua/análisis , Cinética , Arsénico/análisis , Hierro/química , Adsorción , Agua
7.
ACS Omega ; 8(22): 19320-19328, 2023 Jun 06.
Artículo en Inglés | MEDLINE | ID: mdl-37305267

RESUMEN

Sugarcane bagasse fly ash is industrial waste produced by incinerating biomass to generate power and steam. The fly ash contains SiO2 and Al2O3, which can be used to prepare aluminosilicate. This latter material exhibits high potential as an adsorbent in various applications, including the livestock industry where issues related to contamination of aflatoxins in animal feeds need to be addressed; addition of adsorbents can help decrease the concentration of aflatoxins during feed digestion. In this study, the effect of the structure of silica prepared from sugarcane bagasse fly ash on physicochemical properties and aflatoxin B1 (AFB1) adsorption capability compared with that of bentonite was investigated. BPS-5, Xerogel-5, MCM-41, and SBA-15 mesoporous silica supports were synthesized using sodium silicate hydrate (Na2SiO3) from sugarcane bagasse fly ash as a silica source. BPS-5, Xerogel-5, MCM-41, and SBA-15 exhibited amorphous structures, while sodium silicate possessed a crystalline structure. BPS-5 possessed larger pore size, pore volume, and pore size distribution with a bimodal mesoporous structure, while Xerogel-5 exhibited lower pore size and pore size distribution with a unimodal mesoporous structure. BPS-5 with a negatively charged surface exhibited the highest AFB1 adsorption capability compared with other porous silica. However, the AFB1 adsorption capability of bentonite was superior to those of all porous silica. Sufficient pore diameter with high total pore volume as well as high intensity of acid sites and negative charge on the surface of the adsorbent is required to increase AFB1 adsorption in the in vitro gastrointestinal tract of animals.

8.
ACS Omega ; 8(19): 17134-17142, 2023 May 16.
Artículo en Inglés | MEDLINE | ID: mdl-37214707

RESUMEN

Regenerated cellulose (RC) produced from waste pineapple leaves was used to develop a colorimetric sensor as a Cu-PAN sheet (RCS). Microcrystalline cellulose derived from dried pineapple leaves was combined with Cu-PAN, dissolved in NaOH and urea, and made into an RC sheet using Na2SO4 as a coagulant. The RCS was used as an H2S indicator at various H2S concentrations (0-50 ppm) and temperatures (5-25 °C). The RCS color changed from purple to New York pink when exposed to H2S. A colorimeter method was used to develop prediction curves with values of R2 > 0.95 for H2S concentrations at 5-25 °C. The physicochemical properties of fresh and spent RCS were characterized using various techniques (Fourier transform infrared spectroscopy, X-ray diffraction, scanning electron microscopy/energy-dispersive X-ray spectroscopy, and thermogravimetric analysis). In addition, when stored at 5 and 25 °C for 90 days, the RCS had outstanding stability. The developed RCS could be applied to food packaging as an intelligent indicator of meat spoilage.

9.
Chemosphere ; 308(Pt 1): 136267, 2022 Dec.
Artículo en Inglés | MEDLINE | ID: mdl-36055586

RESUMEN

Low cost Fe2O3-based sorbents with an exceptional selectivity toward the targeted As(V) pollutant have gained extensive attention in water treatment. However, their structural features often influence removal performance. In this respect, we present herein a rational design of silica-supported Fe2O3 sorbents with an enhanced morphological structure based on a simple temperature-induced process. Low-hydrothermal temperature synthesis (60 and 100 °C) provided a large silica-cluster size with a close packed structure (S-60 and S-100), contributing to an increase in mass transport resistance. Fe2O3/S-60 with 6.2-nm pore width silica achieved a maximum As(V) uptake capacity (qm) of only 3.5 mg g-1. Supporting Fe2O3 on S-100 with an approximately two-fold increase in the pore size (13 nm) did not lead to any evident enhancement in qe (3.7 mg g-1). However, expanding the pore window up to 22.6 nm (S-140) and 39.5 nm (S-180), along with changing from close-packed to sponge-like loose structures induced by high-temperature synthesis (140 °C and 180 °C), resulted in substantial increases in qm. Fe2O3/S-140 had 1.7 and 1.6 times higher qm (5.9 mg g-1) than Fe2O3/S-100 and Fe2O3/S-60, respectively. The highest qm (7.4 mg g-1) was achieved for Fe2O3/S-180, which was attributed to its relatively small-sized silica cluster and the largest cavities that facilitated easier access by As(V) to adsorbing sites.


Asunto(s)
Contaminantes Químicos del Agua , Purificación del Agua , Adsorción , Dióxido de Silicio/química , Temperatura , Contaminantes Químicos del Agua/análisis , Purificación del Agua/métodos
10.
Chemosphere ; 308(Pt 2): 136356, 2022 Dec.
Artículo en Inglés | MEDLINE | ID: mdl-36087737

RESUMEN

Purification of As(V)-contaminated water through adsorption by Fe2O3-based materials is a promising technology due to its low-cost and high efficiency. Dispersing the Fe2O3 phase on silica supports can improve both the adsorption rate and capacity due to the reduction in Fe2O3 particle sizes and the prevention of clumping of the Fe2O3 particles. However, the clusters in conventional silica materials largely impede the diffusion of As(V) to reach the Fe2O3 sites dispersed inside the clusters. Here, by applying a gelatin template strategy, the structure of silica materials was tailored by changing the gelatin-to-silica ratio (0, 0.6, 1.2 and 1.8) and hydrothermal temperature (60 °C, 100 °C and 140 °C). The silica cluster size could be reduced using either a low gelatin-to-silica ratio (0.6) or a low hydrothermal temperature (60 °C). Increasing the gelatin-to-silica ratio to 1.2 created porous silica spheres with a hollow structure. The Fe2O3-loaded hollow porous silica spheres with a shell thickness of 280 nm had twice the maximum As(V) adsorption capacity (7.66 mg g-1) compared to the Fe2O3-loaded silica product prepared in the absence of gelatin (3.82 mg g-1). The maximum As(V) adsorption capacity could be further enhanced to 9.94 mg g-1 by reducing the shell thickness to 80 nm through increasing the gelatin-to-silica ratio to 1.8 and the hydrothermal temperature to 140 °C. In addition, the best Fe2O3-loaded hollow porous silica spheres had rapid As(V) adsorption and showed excellent durability as the As(V) removal efficiency slightly decreased to 98.9% subsequent to five adsorption-regeneration cycles.


Asunto(s)
Dióxido de Silicio , Aguas Residuales , Compuestos Férricos/química , Gelatina , Porosidad , Dióxido de Silicio/química , Aguas Residuales/química , Agua
11.
ACS Omega ; 7(16): 14264-14275, 2022 Apr 26.
Artículo en Inglés | MEDLINE | ID: mdl-35573207

RESUMEN

Catalytic methane decomposition has been considered suitable for the green and sustainable production of high-purity H2 to help reduce greenhouse gas emissions. This research developed a copper-modified nickel-supported mesocellular silica NiCu/MS(x) catalyst synthesized at different calcination temperatures to improve the activity and stability in the CH4 decomposition reaction at 600 °C. Ni and Cu metals were loaded on a mesocellular silica (MS) support using a co-impregnation method and calcined at different temperatures (500, 600, 700, and 800 °C). The NiCu/MS(600) catalyst not only had the highest H2 yield (32.78%), which was 1.47-3.87 times higher than those of the other NiCu/MS(x) catalysts, but also showed better stability during the reaction. Calcination at 600 °C helps improve the active nickel dispersion, the reducibility of the NiCu catalyst, and the interaction of the NiCu-MS support, leading to the formation of fishbone and platelet carbon nanofibers via a tip-growth mechanism, resulting in the NiCu metals remaining active during the reaction.

12.
Chemosphere ; 300: 134613, 2022 Aug.
Artículo en Inglés | MEDLINE | ID: mdl-35430200

RESUMEN

Arsenic (As) contamination in aqueous media is a major concern due to its adverse impacts on humans and the ecosystem more broadly because of its non-biodegradability. Consequently, an effective and selective sorbent is needed urgently to scavenge As pollutant. Herein, the adsorption behaviors of As(V) by Fe2O3 and Fe2O3 supported on different silica materials, consisting of unimodal mesoporous silica (Fe2O3/U-SiO2) and dual meso-macroporous silica (Fe2O3/B-SiO2), were compared to examine their structure-efficiency relationships in the elimination of As(V). Fe2O3/B-SiO2 was much faster at As(V) removal and had an impressively higher uptake capability, reaching nearly 50% and 2.5 mg g-1 within 5 min compared to bare Fe2O3 (6% and 0.3 mg g-1) and Fe2O3/U-SiO2 (11.9% and 0.59 mg g-1). These better results were because of the highly dispersed Fe2O3 nanoparticles on the B-SiO2 support that provided abundant reactive sites as well as a macropore structure facilitating As(V) diffusion into adsorptive sites. The maximum adsorptive capacity of Fe2O3/B-SiO2 (4.7 mg As per 1 g adsorbent) was 1.3- and 1.7-fold greater than for Fe2O3/U-SiO2 and Fe2O3, respectively. The outstanding performance and reusability of Fe2O3/B-SiO2 with its ease of production, economical and environmentally friendly features made it even more attractive for As(V) remediation. The explored relationship between the structure of SiO2-supported Fe2O3 sorbents and their performance in removing As(V) could be informative for the future design of highly efficient adsorbents for the decontamination of water.


Asunto(s)
Arsénico , Contaminantes Ambientales , Contaminantes Químicos del Agua , Adsorción , Arsénico/química , Ecosistema , Compuestos Férricos/química , Humanos , Dióxido de Silicio , Agua/química , Contaminantes Químicos del Agua/análisis
13.
Sci Rep ; 12(1): 2595, 2022 02 16.
Artículo en Inglés | MEDLINE | ID: mdl-35173240

RESUMEN

The oxidative coupling of methane (OCM) converts CH4 to value-added chemicals (C2+), such as olefins and paraffin. For a series of MnTiO3-Na2WO4 (MnTiO3-NW) and MnOx-TiO2-Na2WO4 (Mn-Ti-NW), the effect of loading of MnTiO3 or MnOx-TiO2, respectively, on two different supports (sol-gel SiO2 (SG) and commercial fumed SiO2 (CS)) was examined. The catalyst with the highest C2+ yield (21.6% with 60.8% C2+ selectivity and 35.6% CH4 conversion) was 10 wt% MnTiO3-NW/SG with an olefins/paraffin ratio of 2.2. The catalyst surfaces with low oxygen-binding energies were associated with high CH4 conversion. Stability tests conducted for over 24 h revealed that SG-supported catalysts were more durable than those on CS because the active phase (especially Na2WO4) was more stable in SG than in CS. With the use of SG, the activity of MnTiO3-NW was not substantially different from that of Mn-Ti-NW, especially at high metal loading.

14.
ACS Omega ; 7(2): 1785-1793, 2022 Jan 18.
Artículo en Inglés | MEDLINE | ID: mdl-35071872

RESUMEN

Oxidative coupling of methane (OCM) is a reaction to directly convert methane into high value-added hydrocarbons (C2+) such as ethylene and ethane using molecular oxygen and a catalyst. This work investigated lanthanum oxide catalysts for OCM, which were promoted with alkaline-earth metal oxides (Mg, Ca, Sr, and Ba) and prepared by the solution-mixing method. The synthesized catalysts were characterized using X-ray powder diffraction, CO2-programmed desorption, and X-ray photoelectron spectroscopy. The comparative performance of each promoter showed that promising lanthanum-loaded alkaline-earth metal oxide catalysts were La-Sr and La-Ba. In contrast, the combination of La with Ca or Mg did not lead to a clear improvement of C2+ yield. The most promising LaSr50 catalyst exhibited the highest C2+ yield of 17.2%, with a 56.0% C2+ selectivity and a 30.9% CH4 conversion. Catalyst characterization indicated that their activity was strongly associated with moderate basic sites and surface-adsorbed oxygen species of O2 -. Moreover, the catalyst was stable over 25 h at a reactor temperature of 700 °C.

15.
Sci Rep ; 11(1): 23042, 2021 11 29.
Artículo en Inglés | MEDLINE | ID: mdl-34845268

RESUMEN

Glycerol is a low-cost byproduct of the biodiesel manufacturing process, which can be used to synthesize various value-added chemicals. Among them, 1,2-propanediol (1,2-PDO) is of great interest because it can be used as an intermediate and additive in many applications. This work investigated the hydrogenolysis of glycerol to 1,2-PDO over Co-Cu bimetallic catalysts supported on TiO2 (denoted as CoCu/TiO2) in aqueous media. The catalysts were prepared using the co-impregnation method and their physicochemical properties were characterized using several techniques. The addition of appropriate Cu increased the glycerol conversion and the 1,2-PDO yield. The highest 1,2-PDO yield was achieved over a 15Co0.5Cu/TiO2 catalyst at 69.5% (glycerol conversion of 95.2% and 1,2-PDO selectivity of 73.0%). In the study on the effects of operating conditions, increasing the reaction temperature, initial pressure, and reaction time increased the glycerol conversion but decreased the selectivity to 1,2-PDO due to the degradation of formed 1,2-PDO to lower alcohols (1-propanol and 2-propanol). The reaction conditions to obtain the maximum 1,2-PDO yield were a catalyst-to-glycerol ratio of 0.028, a reaction temperature of 250 °C, an initial H2 pressure of 4 MPa, and a reaction time of 4 h.

16.
RSC Adv ; 11(7): 3990-3996, 2021 Jan 19.
Artículo en Inglés | MEDLINE | ID: mdl-35424344

RESUMEN

An external magnetic field has recently been applied in reaction processes to promote movement and avoid agglomeration of magnetic particles, and also reduce the activation energy through improving the gas-solid contact. In this work, the effect of an external magnetic field on reactant gas diffusivity and reactivity in CO hydrogenation within a confined-space catalyst was investigated for the first time using a conventional reactor packed with a bimetallic 5Fe-5Co/ZSM-5 molecular sieve catalyst. The synergistic effect between magnetic field and limited mass transfer within zeolite cavities improved the mass transfer ability and reaction phenomena of the reactant molecules, leading to enhancement of catalytic activity with tailored reaction pathways. As a result, CO conversion and CH4 selectivity were increased by factors of 1.9 and 1.3 compared to those without a magnetic field. These synergistic interactions are able to provide an innovative challenge for green and sustainable chemical processes and separation processes by means of selective reactant and product mass transfer designed for selective catalytic conversion in the future.

17.
ACS Omega ; 5(23): 13612-13620, 2020 Jun 16.
Artículo en Inglés | MEDLINE | ID: mdl-32566826

RESUMEN

Na2WO4-TiO2-MnO x /SiO2 (SM) catalysts with alkali (Li, K, Rb, Cs) or alkali earth (Mg, Ca, Sr, Ba) oxide additives, which were prepared using incipient wetness impregnation, were investigated for oxidative coupling of methane (OCM) to value-added hydrocarbons (C2+). A screening test that was performed on the catalysts revealed that SM with Sr (SM-Sr) had the highest yield of C2+. X-ray photoelectron spectroscopy analyses indicated that the catalysts with a relatively low binding energy of W 4f7/2 facilitated a high CH4 conversion. A combination of crystalline MnTiO3, Mn2O3, α-cristobalite, Na2WO4, and TiO2 phases was identified as an essential component for a remarkable improvement in the activity of the catalysts in the OCM reaction. In attempts to optimize the C2+ yield, 0.25 wt % Sr onto SM-Sr achieved the highest C2+ yield at 22.9% with a 62.5% C2+ selectivity and a 36.6% CH4 conversion. A stability test of the optimal catalyst showed that after 24 h of testing, its activity decreased by 18.7%.

18.
ACS Omega ; 5(5): 2334-2344, 2020 Feb 11.
Artículo en Inglés | MEDLINE | ID: mdl-32064395

RESUMEN

Thermal treatment during catalyst preparation is one of the important factors affecting the characteristics and performance of a catalyst. To improve the catalytic performance of an alumina-supported copper catalyst prepared by an impregnation method for dimethyl ether (DME) synthesis from CO2, the effects of the use of hot air and infrared drying as well as calcination at 600 and 900 °C to prepare alumina supports were investigated. Infrared drying could shorten the required drying time by 75% when compared with hot air drying. Infrared drying could also help maintain the pore size and pore volume of the supports, leading to their larger surface areas. Different drying techniques were additionally noted to result in different sizes and shapes of the pores as well as to different copper distributions and intensities of acid sites of the catalyst. An increase in the calcination temperature resulted in a decrease in the surface area of the supports because of particle aggregation. The drying technique exhibited a more significant effect than calcination temperature on the space-time yield of DME. A catalyst utilizing the support prepared by infrared drying and then calcined at 600 °C exhibited the highest yield of DME (40.9 gDME kgcat -1 h-1) at a reaction temperature of 300 °C. Stability of the optimal catalyst, when monitored over a 24 h period, was noted to be excellent.

19.
ACS Omega ; 5(4): 1911-1918, 2020 Feb 04.
Artículo en Inglés | MEDLINE | ID: mdl-32039327

RESUMEN

Surface functionalities of activated carbon can be affected by the presence of heteroatoms such as oxygen, sulfur, and nitrogen. In this work, nitrogen-doped activated carbons (NACs) were prepared from shrimp shells, and the effects of the mixing ratio (raw material to an activating agent) on the porous texture and surface functionalities were investigated. It was found that, with increasing the mixing ratio (resulting in increasing N/C), the development of mesoporosity was significantly observed. This led to decreasing microporosity and specific surface areas (SSAs). The obtained NACs exhibited nitrogen functionalities in the forms of pyridinic and pyrrolic groups. It was found that although the pyridinic-N has a detrimental effect on the SSA, it does favor the pseudocapacitance, leading to an enhancement in the ion storage capability regardless of the low SSA.

20.
ACS Omega ; 4(19): 18076-18086, 2019 Nov 05.
Artículo en Inglés | MEDLINE | ID: mdl-31720510

RESUMEN

Deactivation of catalysts due to rapid blocking of active surfaces and pores is a major problem for methane cracking. The removal of the template using different calcination methods contributes to the different characteristics of catalyst support. Therefore, silica supports were prepared with the sol-gel method, where sodium silicate and chitosan are a silica source and a template, respectively. Calcination using a microwave muffle furnace (MWF) was preferred over the conventional electric muffle furnace at the heating rates of 2 and 17 °C/min (CEF2 and CEF17, respectively) in order to remove the chitosan template. A nickel nitrate precursor was loaded onto the obtained silica supports by the incipient wetness impregnation method. The properties of the silica support and the Ni/SiO2 catalysts were characterized by means of N2-sorption, X-ray diffraction, scanning electron microscopy-energy-dispersive X-ray, field emission transmission electron microscopy, and H2 temperature-programmed reduction. The catalytic activity was evaluated using a fixed-bed reactor at 550 °C with a CH4/N2 ratio of 1:4 in the feed. The amount and the allotropes of carbon deposited on the spent catalysts were investigated using thermogravimetric/differential thermal analysis. The results showed that the SiO2-MWF support had a higher surface area and a larger pore volume of a mesoporous structure with larger interparticle channels than that of the SiO2-CEF supports. This leads to the higher dispersion of Ni metal particles over and inside the interparticle channels of the SiO2-MWF support. This provided a higher metal-support interaction, resulting in lower rates of methane conversion and carbon deposition on the catalyst surface than those of Ni/SiO2-CEF catalysts. However, it displayed a lower bed pressure. It was found that the carbon fibers deposited on all the catalysts were multiwalled carbon nanotubes (MWCNTs). Additionally, the base-growth mechanism of MWCNTs was only exhibited by the Ni/SiO2-MWF catalyst.

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