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1.
ACS Omega ; 9(32): 35060-35068, 2024 Aug 13.
Article in English | MEDLINE | ID: mdl-39157098

ABSTRACT

A bubbling fluidized bed reactor is designed to investigate the high-temperature calcination and decomposition characteristics of phosphogypsum (PG). The reactor employs electric heating, and a lifting discharge tube is installed in the middle of the air distributor to allow flexible switching between batch and continuous feeding modes. The batch test results show that the solid-phase bed materials with a PG particle size of 0.27-0.55 mm and a coal particle size of 0.55-0.83 mm are found to have uniformly mixed at a PG/coal mass ratio of 5:1 and calcined at a high temperature of 1100 °C for 30 min. PG completely decomposes to yield mainly CaS and a small amount of Ca2(SiO4) as the solid-phase products. For the above-mentioned optimal process parameters, a 120 min thermal-state continuous test is conducted. Feeding and discharging are performed at intervals of 30 min to maintain the stability of the static bed height inside the reactor. The results indicate that the PG decomposition rate is higher than 92% in the batch and continuous tests. However, the continuous decomposition of PG has significant process advantages, such as a higher CaS yield (71.20%) compared to that in the batch mode (64.49%). Furthermore, PG undergoes agglomeration and bonding within the particles when heated, intensifying the formation of a Ca2(SiO4) eutectic.

2.
Sci Total Environ ; 927: 172047, 2024 Jun 01.
Article in English | MEDLINE | ID: mdl-38575006

ABSTRACT

In this paper, different emerging post-combustion technologies, i.e., monoethanolamine (MEA), aqueous ammonia, pressure swing adsorption (PSA), temperature swing adsorption (TSA), membrane and calcium looping, were applied to an ultra-supercritical coal-fired power plant for carbon capture. A 'cradle-to-grave' life cycle assessment (LCA) was conducted to evaluate the technical performance and environmental impacts of the power plant with six emerging carbon capture technologies. Carbon capture significantly influences the impact categories directly associated with flue gas emission. The application of carbon capture reduced the GWP in the range of 49-75 %. TAP also reduced in the range of 18-51 %. However, the human toxicity potential, eutrophication potential, ecotoxicity potential and particulate matter formation potential increased due to energy and resource consumption in the upstream and downstream processes. For the life cycle water consumption potential, it decreased by 8 % with calcium looping, whereas it increased in the range of 36-75 % with other post-combustion technologies. The highest reduction in GWP and the least reduction in power efficiency was observed in calcium looping because of the high-temperature heat recovery from flue gas and elimination of complex solvent manufacturing. The plant with aqueous ammonia and membrane separation had the second and third highest reductions in GWP. In addition, the lowest values for TAP, FEP, and MEP were obtained in the membrane system. With MEA for CO2 capture, the total GWP value of the plant is slightly higher than these three technologies mentioned above, and the highest HTPc, FETP, and METP can be observed in this case. TSA and PSA have the most significant environmental impacts in most categories due to higher energy requirements.

3.
ACS Omega ; 7(5): 4381-4388, 2022 Feb 08.
Article in English | MEDLINE | ID: mdl-35155931

ABSTRACT

Oxygen carriers can significantly enhance the performance of chemical looping combustion at low energy-cost CO2 capture. Based on the density functional theory, a microscopic model of the metal Fe, Al-doped NiO oxygen carrier was established. The results indicate that the intermediate state energy and the reaction energy reduce due to electronic interaction of the Al-doped surface. With the progress of the reaction, the NiO-Al surface promotes the oxidation process of CO, indicating that the activity of the NiO surface enhanced, which is attributed to the electronic and steric effects of the Al-O structure. For the decomposition of CO on the OC surface, doping with other atoms is beneficial to suppress the carbon deposition, which is related to the steric hindrance caused by doping with other atoms. Besides, doping with iron and aluminum atoms is more conducive to the movement of OC bulk crystal lattice oxygen to the surface, thereby promoting subsequent reactions. Therefore, it is feasible to improve the reactivity of the Ni-based OC by doping metal Al, and its modification effect is closely related to the characteristics of the components.

4.
Sci Total Environ ; 795: 148904, 2021 Nov 15.
Article in English | MEDLINE | ID: mdl-34328951

ABSTRACT

Surface oxygen activities always play an important role in various heterogeneous reaction processes. In this study, the surface oxygen activity of studied perovskite oxides is greatly enhanced after the composition and morphology are tuned. It is worth noting that the surface oxygen activity is enhanced correspondingly, accompanied by higher surface area, better reducibility, and superior low-temperature reactivity of studied catalysts. The sample introduced with nickel atom and nanorods structure possesses higher surface oxygen activity and vacancies with superior performance including T10 at 221 °C and T90 at 243 °C, nearly 90 °C elevations. Double perovskite oxides, especially with nanorods structure are verified to be composed of more surface active oxygen, which could be related to low-temperature redox ability and superior oxygen vacancies. Based on the DFT calculation, introducing nickel element is confirmed to be able to efficiently boost the generation of oxygen vacancies and adsorption of oxygen molecular, in accord with the analysis of characterization. To sum up, the strategy of introducing the nickel atom and nanorods structure could effectively tune the surface oxygen activity and generate more oxygen vacancies, which would be beneficial to the catalytic performance of toluene catalytic oxidation correspondingly.

5.
Environ Sci Pollut Res Int ; 26(12): 12123-12135, 2019 Apr.
Article in English | MEDLINE | ID: mdl-30827023

ABSTRACT

Cobalt oxides have been considered as a kind of highly efficient catalyst for the oxidation of volatile organic compounds (VOCs). In this work, lanthanum-cobalt composite oxides were prepared by using the co-precipitation method, and toluene was used as the model compound. Diversified techniques including XRD, SEM, Raman spectra, XPS, H2-TPR, and N2 adsorption-desorption were applied to investigate the physicochemical properties of as-prepared materials. The composite catalysts showed different morphology including larger specific surface area and higher pore volume which would accelerate the adsorption of toluene and improve the amount of active sites on surface. Moreover, the addition of lanthanum could enhance the low-temperature reducibility, and it could be also beneficial to expose more Co3+ and adsorbed oxygen species on the surface of catalysts which could accelerate the oxidation of toluene and lower onset oxidation temperature. 0.05La-Co (with a molar ratio of lanthanum against cobalt is 0.05) showed the best catalytic performance. The complete conversion of toluene was achieved at 225 °C under the condition of toluene concentration = 1000 ppm and SV = 20,000 ml·g-1·h-1. Stability test over 0.05La-Co was conducted at 225 °C and it could maintain the 100% conversion of toluene for 720 min, indicating the excellent stability of as-prepared catalysts. Undoubtedly, lanthanum-cobalt composite oxide is a kind of promising material for the catalytic oxidation of VOCs.


Subject(s)
Cold Temperature , Models, Chemical , Toluene/chemistry , Adsorption , Catalysis , Cobalt/chemistry , Lanthanum/chemistry , Oxidation-Reduction , Oxides/chemistry , Oxygen/chemistry , Surface Properties , Temperature , Volatile Organic Compounds/chemistry
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