| 1. |
- Bäckström, Daniel, 1985, et al.
(författare)
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Particle composition and size distribution in coal flames - The influence on radiative heat transfer
- 2015
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Ingår i: Experimental Thermal and Fluid Science. - : Elsevier BV. - 0894-1777 .- 1879-2286. ; 64, s. 70-80
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Tidskriftsartikel (refereegranskat)abstract
- Radiative heat transfer in a 77 kWth swirling lignite flame has been studied. The aim is to characterize different particle types present in a coal flame and to determine their influence on the radiative heat transfer. The study combines extractive particle measurements, radiative intensity measurements and detailed radiation modelling. The size distribution of the extracted particles was measured with a low pressure impactor and some of the size fractions were analysed with SEM–EDX. The measured total radiative intensity is compared with the modelled intensity based on the particle measurements in the same cross-section of the flame. The particle properties were calculated with Mie theory and the gas properties with a statistical narrow-band model. The results show that the contribution of coal/char particles dominates the radiative heat transfer in the investigated cross-section of the flame. The methodology applied in this work shows promising results for characterization of particle radiation in flames of practical size.
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| 2. |
- Boy, M., et al.
(författare)
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Interactions between the atmosphere, cryosphere, and ecosystems at northern high latitudes
- 2019
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Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 19:3, s. 2015-2061
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Tidskriftsartikel (refereegranskat)abstract
- The Nordic Centre of Excellence CRAICC (Cryosphere-Atmosphere Interactions in a Changing Arctic Climate), funded by NordForsk in the years 2011-2016, is the largest joint Nordic research and innovation initiative to date, aiming to strengthen research and innovation regarding climate change issues in the Nordic region. CRAICC gathered more than 100 scientists from all Nordic countries in a virtual centre with the objectives of identifying and quantifying the major processes controlling Arctic warming and related feedback mechanisms, outlining strategies to mitigate Arctic warming, and developing Nordic Earth system modelling with a focus on short-lived climate forcers (SLCFs), including natural and anthropogenic aerosols. The outcome of CRAICC is reflected in more than 150 peer-reviewed scientific publications, most of which are in the CRAICC special issue of the journal Atmospheric Chemistry and Physics. This paper presents an overview of the main scientific topics investigated in the centre and provides the reader with a state-of-the-art comprehensive summary of what has been achieved in CRAICC with links to the particular publications for further detail. Faced with a vast amount of scientific discovery, we do not claim to completely summarize the results from CRAICC within this paper, but rather concentrate here on the main results which are related to feedback loops in climate change-cryosphere interactions that affect Arctic amplification.
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| 3. |
- Davidsson, Kent, 1967, et al.
(författare)
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Potassium, chlorine, and sulfur in ash, particles, deposits, and corrosion during wood combustion in a circulating fluidized-bed boiler
- 2007
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Ingår i: Energy & Fuels. - : American Chemical Society (ACS). - 1520-5029 .- 0887-0624. ; 21:1, s. 71-81
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Tidskriftsartikel (refereegranskat)abstract
- The effect of the addition of chlorine and/or sulfur to the fuel on fly ash composition, deposit formation, and superheater corrosion has been studied during biomass combustion in a circulating fluidized-bed boiler. The chlorine (HCl (aq)) and sulfur (SO2 (g)) were added in proportions of relevance for the potassium chemistry. The composition of the bottom and the fly ashes was analyzed. Gas and particle measurements were performed downstream of the cyclone before the convection pass and the flue gas composition was recorded in the stack with a series of standard instruments and an FTIR analyzer. At the position downstream of the cyclone, a deposit probe was situated, simulating a superheater tube. Deposits on the probe and initial corrosion were examined. It is concluded that addition of sulfur and chlorine increases the formation of submicron particles leading to deposition of potassium sulfate and chloride. The results compare well with earlier work based on laboratory-scale experiments concerning effects of chlorine and sulfur on potassium chemistry.
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| 4. |
- Tan, W., et al.
(författare)
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Atmospheric Chemistry of 2-Amino-2-methyl-1-propanol: A Theoretical and Experimental Study of the OH-Initiated Degradation under Simulated Atmospheric Conditions
- 2021
-
Ingår i: Journal of Physical Chemistry A. - : American Chemical Society (ACS). - 1089-5639 .- 1520-5215. ; 125:34, s. 7502-7519
-
Tidskriftsartikel (refereegranskat)abstract
- The OH-initiated degradation of 2-amino-2-methyl-1-propanol [CH3C(NH2)(CH3)CH2OH, AMP] was investigated in a large atmospheric simulation chamber, employing time-resolved online high-resolution proton-transfer reaction-time-of-flight mass spectrometry (PTR-ToF-MS) and chemical analysis of aerosol online PTR-ToF-MS (CHARON-PTR-ToF-MS) instrumentation, and by theoretical calculations based on M06-2X/aug-cc-pVTZ quantum chemistry results and master equation modeling of the pivotal reaction steps. The quantum chemistry calculations reproduce the experimental rate coefficient of the AMP + OH reaction, aligning k(T) = 5.2 x 10(-12) x exp (505/T) cm(3) molecule(-1) s(-1) to the experimental value k(exp,300K) = 2.8 x 10(-11) cm(3) molecule(-1) s(-1). The theoretical calculations predict that the AMP + OH reaction proceeds via hydrogen abstraction from the -CH3 groups (5-10%), -CH2- group, (>70%) and -NH2 group (5-20%), whereas hydrogen abstraction from the -OH group can be disregarded under atmospheric conditions. A detailed mechanism for atmospheric AMP degradation was obtained as part of the theoretical study. The photo-oxidation experiments show 2-amino-2-methylpropanal [CH3C(NH2)(CH3)CHO] as the major gas-phase product and propan-2-imine [(CH3)(2)C=NH], 2-iminopropanol [(CH3)(CH2OH)C=NH], acetamide [CH3C(O)NH2], formaldehyde (CH2O), and nitramine 2-methyl-2-(nitroamino)-1-propanol [AMPNO(2), CH3C(CH3)(NHNO2)-CH2OH] as minor primary products; there is no experimental evidence of nitrosamine formation. The branching in the initial H abstraction by OH radicals was derived in analyses of the temporal gas-phase product profiles to be B-CH3/B-CH2/B-NH2 = 6:70:24. Secondary photo-oxidation products and products resulting from particle and surface processing of the primary gas-phase products were also observed and quantified. All the photo-oxidation experiments were accompanied by extensive particle formation that was initiated by the reaction of AMP with nitric acid and that mainly consisted of this salt. Minor amounts of the gas-phase photo-oxidation products, including AMPNO(2), were detected in the particles by CHARON-PTR-ToF-MS and GCxGC-NCD. Volatility measurements of laboratory-generated AMP nitrate nanoparticles gave Delta H-vap = 80 +/- 16 kJ mol(-1) and an estimated vapor pressure of (1.3 +/- 0.3) x 10(-5) Pa at 298 K. The atmospheric chemistry of AMP is evaluated and a validated chemistry model for implementation in dispersion models is presented.
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| 5. |
- Andersson, Patrik U, 1970, et al.
(författare)
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Carbon dioxide interactions with crystalline and amorphous ice surfaces
- 2004
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Ingår i: Journal of Physical Chemistry A. - : American Chemical Society (ACS). - 1089-5639 .- 1520-5215. ; 108:21, s. 4627-4631
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Tidskriftsartikel (refereegranskat)abstract
- Carbon dioxide interactions with crystalline and amorphous water ice have been studied by time-resolved molecular beam techniques. CO2 collisions at thermal kinetic energies with ice in the temperature range 100-160 K result in efficient trapping on the ice surface followed by desorption. The desorption kinetics on crystalline ice at 100-125 K are well described by the Arrhenius equation with an activation energy of 0.22 +/- 0.02 eV and a preexponential factor of 10(13.32+/-0.57) s(-1). Below 120 K, CO2 populates strongly bonded sites on amorphous ice, resulting in surface residence times on the order of minutes at 100 K, and the desorption data can in this case not be explained by a simple first-order process. The results are compared to previous studies of gas-ice interactions, and the implications for heterogeneous processes in the terrestrial atmosphere are discussed.
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| 6. |
- Bartels-Rausch, Thorsten, et al.
(författare)
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Ice structures, patterns, and processes: A view across the icefields
- 2012
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Ingår i: Reviews of Modern Physics. ; 84:2, s. 885-944
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Forskningsöversikt (refereegranskat)abstract
- From the frontiers of research on ice dynamics in its broadest sense, this review surveys the structures of ice, the patterns or morphologies it may assume, and the physical and chemical processes in which it is involved. Open questions in the various fields of ice research in nature are highlighted, ranging from terrestrial and oceanic ice on Earth, to ice in the atmosphere, to ice on other Solar System bodies and in interstellar space.
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| 7. |
- Castarède, Dimitri, et al.
(författare)
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Development and characterization of the Portable Ice Nucleation Chamber 2 (PINCii)
- 2023
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Ingår i: Atmospheric Measurement Techniques. - 1867-1381. ; 16:16, s. 3881-3899
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Tidskriftsartikel (refereegranskat)abstract
- The Portable Ice Nucleation Chamber 2 (PINCii) is a newly developed continuous flow diffusion chamber (CFDC) for measuring ice nucleating particles (INPs). PINCii is a vertically oriented parallel-plate CFDC that has been engineered to improve upon the limitations of previous generations of CFDCs. This work presents a detailed description of the PINCii instrument and the upgrades that make it unique compared with other operational CFDCs. The PINCii design offers several possibilities for improved INP measurements. Notably, a specific icing procedure results in low background particle counts, which demonstrates the potential for PINCii to measure INPs at low concentrations ( < 10 L (-1)). High-spatial-resolution wall-temperature mapping enables the identification of temperature inhomogeneities on the chamber walls. This feature is used to introduce and discuss a new method for analyzing CFDC data based on the most extreme lamina conditions present within the chamber, which represent conditions most likely to trigger ice nucleation. A temperature gradient can be maintained throughout the evaporation section in addition to the main chamber, which enables PINCii to be used to study droplet activation processes or to extend ice crystal growth. A series of both liquid droplet activation and ice nucleation experiments were conducted at temperature and saturation conditions that span the spectrum of PINCii's operational conditions ( 50 <= temperature <= 15 degrees C and 100 <= relative humidity with respect to ice <= 160 %) to demonstrate the instrument's capabilities. In addition, typical sources of uncertainty in CFDCs, including particle background, particle loss, and variations in aerosol lamina temperature and relative humidity, are quantified and discussed for PINCii.
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| 8. |
- Johansson, Sofia M., 1983, et al.
(författare)
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Understanding water interactions with organic surfaces: environmental molecular beam and molecular dynamics studies of the water-butanol system
- 2019
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Ingår i: Physical Chemistry Chemical Physics. - : Royal Society of Chemistry (RSC). - 1463-9076 .- 1463-9084. ; 21:3, s. 1141-1151
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Tidskriftsartikel (refereegranskat)abstract
- The interactions between water molecules and condensed n-butanol surfaces are investigated at temperatures from 160 to 240 K using the environmental molecular beam experimental method and complementary molecular dynamics (MD) simulations. In the experiments hyperthermal water molecules are directed onto a condensed n-butanol layer and the flux from the surface is detected in different directions. A small fraction of the water molecules scatters inelastically from the surface while losing 60-90% of their initial kinetic energy in collisions, and the angular distributions of these molecules are broad for both solid and liquid surfaces. The majority of the impinging water molecules are thermalized and trapped on the surface, while subsequent desorption is governed by two different processes: one where molecules bind briefly to the surface (residence time < 10 s), and another where the molecules trap for a longer time = 0.8-2.0 ms before desorbing. Water molecules trapped on a liquid n-butanol surface are substantially less likely to escape from the surface compared to a solid layer. The MD calculations provide detialed insight into surface melting, adsorption, absorption and desorption processes. Calculated angular distributions and kinetic energy of emitted water molecules agree well with the experimental data. In spite of its hydrophobic tail and enhanced surface organization below the melting temperature, butanol's hydrophilic functional groups are concluded to be surprisingly accessible to adsorbed water molecules; a finding that may be explained by rapid diffusion of water away from hydrophobic surface structures towards more strongly bound conformational structures.
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| 9. |
- Romero Lejonthun, Liza, 1973, et al.
(författare)
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Chlorine interactions with water ice studied by molecular beam techniques.
- 2006
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Ingår i: The journal of physical chemistry. B. - : American Chemical Society (ACS). - 1520-6106 .- 1520-5207. ; 110:46, s. 23497-501
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Tidskriftsartikel (refereegranskat)abstract
- The kinetics of chlorine interactions with ice at temperatures between 103 and 165 K have been studied using molecular beam techniques. The Cl(2) trapping probability is found to be unity at thermal incident energies, and trapping is followed by rapid desorption. The residence time on the surface is less than 25 microg at temperatures above 135 K and approaches 1 s around 100 K. Rate constants for desorption are determined for temperatures below 135 K. The desorption kinetics follow the Arrhenius equation, and activation energies of 0.24 +/- 0.03 and 0.31 +/- 0.01 eV, with corresponding preexponential factors of 10(12.08+/-1.19) and 10(16.52+/-0.38) s(-1), are determined. At least two different Cl(2) binding sites are concluded to exist on the ice surface. The observed activation energies are likely to be the Cl(2)-ice binding energies for these states, and the Cl(2)-surface interactions are concluded to be stronger than earlier theoretical estimates. The surface coverage of Cl(2) on ice under stratospheric conditions is estimated to be negligible, in agreement with earlier work.
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| 10. |
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| 11. |
- Öjekull, Jenny, 1973, et al.
(författare)
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Dissociative recombination of ammonia clusters studied by storage ring experiments
- 2006
-
Ingår i: Journal of Chemical Physics. - : AIP Publishing. - 0021-9606 .- 1089-7690. ; 125:19, s. 194306-
-
Tidskriftsartikel (refereegranskat)abstract
- Dissociative recombination of ammonia cluster ions with free electrons has been studied at the heavy-ion storage ring CRYRING (Manne Siegbahn Laboratory, Stockholm University). The absolute cross sections for dissociative recombination of H+(NH3)(2), H+(NH3)(3), D+(ND3)(2), and D+(ND3)(3) in the collision energy range of 0.001-27 eV are reported, and thermal rate coefficients for the temperature interval from 10 to 1000 K are calculated from the experimental data and compared with earlier results. The fragmentation patterns for the two ions H+(NH3)(2) and D+(ND3)(2) show no clear isotope effect. Dissociative recombination of X+(NX3)(2) (X=H or D) is dominated by the product channels 2NX(3)+X [0.95 +/- 0.02 for H+(NH3)(2) and 1.00 +/- 0.02 for D+(ND3)(2)]. Dissociative recombination of D+(ND3)(3) is dominated by the channels yielding three N-containing fragments (0.95 +/- 0.05).
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| 12. |
- Öjekull, Jenny, 1973, et al.
(författare)
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Dissociative recombination of H+(H2O)3 and D+(D2O)3 water cluster ions with electrons: Cross sections and branching ratios
- 2007
-
Ingår i: The Journal of chemical physics. - : AIP Publishing. - 0021-9606 .- 1089-7690. ; 127, s. 194301-194309
-
Tidskriftsartikel (refereegranskat)abstract
- Dissociative recombination (DR) of the water cluster ions H+(H2O)3 and D+(D2O)3 with electrons has been studied at the heavy-ion storage ring CRYRING (Manne Siegbahn Laboratory, Stockholm University). For the first time, absolute DR cross sections have been measured for H+(H2O)3 in the energy range of 0.001–0.8 eV, and relative cross sections have been measured for D+(D2O)3 in the energy range of 0.001–1.0 eV. The DR cross sections for H+(H2O)3 are larger than previously observed for H+(H2O)n (n=1,2), which is in agreement with the previously observed trend indicating that the DR rate coefficient increases with size of the water cluster ion. Branching ratios have been determined for the dominating product channels. Dissociative recombination of H+(H2O)3 mainly results in the formation of 3H2O+H (probability of 0.95±0.05) and with a possible minor channel resulting in 2H2O+OH+H2 (0.05±0.05). The dominating channels for DR of D+(D2O)3 are 3D2O+D (0.88±0.03) and 2D2O+OD+D2 (0.09±0.02). The branching ratios are comparable to earlier DR results for H+(H2O)2 and D+(D2O)2, which gave 2X2O+X (X=H,D) with a probability of over 0.9.
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| 13. |
- Öjekull, Jenny, 1973, et al.
(författare)
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Dissociative recombination of NH4+ and ND4+ ions : Storage ring experiments and ab initio molecular dynamics
- 2004
-
Ingår i: Journal of Chemical Physics. - : AIP Publishing. - 0021-9606 .- 1089-7690. ; 120:16, s. 7391-7399
-
Tidskriftsartikel (refereegranskat)abstract
- The dissociative recombination (DR) process of NH4+ and ND4+ molecular ions with free electrons has been studied at the heavy-ion storage ring CRYRING (Manne Siegbahn Laboratory, Stockholm University). The absolute cross sections for DR of NH4+ and ND4+ in the collision energy range 0.001-1 eV are reported, and thermal rate coefficients for the temperature interval from 10 to 2000 K are calculated from the experimental data. The absolute cross section for NH4+ agrees well with earlier work and is about a factor of 2 larger than the cross section for ND4+. The dissociative recombination of NH4+ is dominated by the product channels NH3+H (0.85+/-0.04) and NH2+2H (0.13+/-0.01), while the DR of ND4+ mainly results in ND3+D (0.94+/-0.03). Ab initio direct dynamics simulations, based on the assumption that the dissociation dynamics is governed by the neutral ground-state potential energy surface, suggest that the primary product formed in the DR process is NH3+H. The ejection of the H atom is direct and leaves the NH3 molecule highly vibrationally excited. A fraction of the excited ammonia molecules may subsequently undergo secondary fragmentation forming NH2+H. It is concluded that the model results are consistent with gross features of the experimental results, including the sensitivity of the branching ratio for the three-body channel NH2+2H to isotopic exchange.
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| 14. |
- Andersson, Patrik U, 1970, et al.
(författare)
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Formation of Highly Rovibrationally Excited Ammonia from Dissociative Recombination of NH4
- 2010
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Ingår i: Journal of Physical Chemistry Letters. - : American Chemical Society (ACS). - 1948-7185. ; 1:17, s. 2519-2523
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Tidskriftsartikel (refereegranskat)abstract
- The internal energy distribution of ammonia formed in the dissociative recombination (DR) of NH4+ with electrons has been studied by an imaging technique at the ion storage ring CRYRING. The DR process resulted in the formation of NH3 + H (0.90 ± 0.01), with minor contributions from channels producing NH2 + H2 (0.05 ± 0.01) and NH2 + 2H (0.04 ± 0.02). The formed NH3 molecules were highly internally excited, with a mean rovibrational energy of 3.3 ± 0.4 eV, which corresponds to 70% of the energy released in the neutralization process. The internal energy distribution was semiquantitatively reproduced by ab initio direct dynamics simulations, and the calculations suggested that the NH3 molecules are highly vibrationally excited while rotational excitation is limited. The high internal excitation and the translational energy of NH3 and H will influence their subsequent reactivity, an aspect that should be taken into account when developing detailed models of the interstellar medium and ammonia-containing plasmas.
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| 15. |
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| 16. |
- Andersson, Patrik U, 1970, et al.
(författare)
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Water Condensation on Graphite Studied by Elastic Helium Scattering and Molecular Dynamics Simulations
- 2007
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Ingår i: Journal of Physical Chemistry C. - : American Chemical Society (ACS). - 1932-7447 .- 1932-7455. ; 111:42, s. 15258-15266
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Tidskriftsartikel (refereegranskat)abstract
- Formation of water/ice layers on graphite has been studied in the temperature range from 90 to 180 K by elastic helium scattering, light scattering, and molecular dynamics simulations. Combined helium- and light-scattering experiments show that an ice film that wets the graphite surface is formed at surface temperatures of 100-140 K, whereas three-dimensional ice structures are formed at 140-180 K. Desorption of adsorbed water molecules competes with water incorporation into the ice film, and the ice formation rate is strongly temperature dependent. At 150 K, ice-layer formation takes place at the same time scale as layer reconstruction, and its properties are sensitive to the water deposition rate. The experimental results are compared with kinetics models, and the Johnston-Mehl-Avrami-Kolmogorov model is concluded to well describe the ice-layer formation kinetics in the whole temperature range. Molecular dynamics simulations of water-cluster formation on graphite at 90-180 K show that water molecules and small clusters are highly mobile on the surface, which rapidly results in the nucleation of large and less mobile clusters on the surface. Clusters formed at low temperature tend to have the most molecules in direct contact with the uppermost graphite layer, while multilayer cluster structures are preferred at high temperatures. The results are discussed and compared with earlier studies of water ice formation on solid surfaces.
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| 17. |
- Andersson, Viktor, 1994, et al.
(författare)
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A Novel Method for On-Line Characterization of Alkali Release and Thermal Stability of Materials Used in Thermochemical Conversion Processes
- 2022
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Ingår i: Energies. - : MDPI AG. - 1996-1073. ; 15:12
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Tidskriftsartikel (refereegranskat)abstract
- Alkali metal compounds are released during the thermal conversion of biofuels and fossil fuels and have a major impact on the efficiency of conversion processes. Herein, we describe a novel method for the simultaneous characterization of alkali release and mass loss from materials used in combustion and gasification processes including solid fuels, fluidized bed materials, and catalysts for gas reforming. The method combines the thermogravimetric analysis of selected samples with the on-line measurement of alkali release using a surface ionization detector. The technique builds on the careful treatment of alkali processes during transport from a sample to the downstream alkali monitor including the losses of alkali in the molecular form to hot walls, the formation of nanometer-sized alkali-containing particles during the cooling of exhaust gases, aerosol particle growth, and diffusion losses in sampling tubes. The performance of the setup was demonstrated using biomass samples and fluidized bed material from an industrial process. The emissions of alkali compounds during sample heating and isothermal conditions were determined and related to the simultaneous thermogravimetric analysis. The methodology was concluded to provide new evidence regarding the behavior of alkali in key processes including biomass pyrolysis and gasification and ash interactions with fluidized beds. The implications and further improvements of the technique are discussed.
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| 18. |
- Andersson, Viktor, 1983, et al.
(författare)
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Alkali desorption from ilmenite oxygen carrier particles used in biomass combustion
- 2024
-
Ingår i: Fuel. - 0016-2361 .- 1873-7153. ; 359
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Tidskriftsartikel (refereegranskat)abstract
- Oxygen-carrying fluidized bed materials are increasingly used in novel technologies for carbon capture and storage, and to improve the efficiency of fuel conversion processes. Potassium- and sodium-containing compounds are released during biomass combustion and may have both negative and positive effects on conversion processes. Ilmenite is an important oxygen carrier material with the ability to capture alkali in the form of titanates. This is a desirable property since it may reduce detrimental alkali effects including fouling, corrosion, and fluidized bed agglomeration. This study investigates the interactions of alkali-containing compounds with ilmenite particles previously used in an industrial scale (115 MWth) oxygen carrier aided combustion system. The ilmenite samples were exposed to temperatures up to 1000 °C under inert and oxidizing conditions while the alkali release kinetics were characterized using online alkali monitoring. Alkali desorption occurs between 630 and 800 °C, which is attributed to loosely bound alkali at or near the surface of the particles. Extensive alkali release is observed above 900 °C and proceeds during extended time periods at 1000 °C. The release above 900 °C is more pronounced under oxidizing conditions and approximately 9.1 and 3.2 wt% of the alkali content is emitted from the ilmenite samples in high and low oxygen activity, respectively. Detailed material analyses using scanning electron microscopy with energy dispersive X-ray spectroscopy and X-ray photoelectron spectroscopy were conducted before and after temperature treatment, which revealed that the concentrations of potassium, sodium and chlorine decrease at the outermost surface of the ilmenite particles during temperature treatment, and Cl is depleted to a deeper level in oxidizing conditions compared to inert. The implications for ilmenite-ash interactions, oxygen carrier aided combustion and chemical looping systems are discussed.
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| 19. |
- Andersson, Viktor, 1983, et al.
(författare)
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Alkali interactions with a calcium manganite oxygen carrier used in chemical looping combustion
- 2022
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Ingår i: Fuel Processing Technology. - : Elsevier BV. - 0378-3820 .- 1873-7188. ; 227
-
Tidskriftsartikel (refereegranskat)abstract
- Chemical-Looping Combustion (CLC) of biofuels is a promising technology for cost-efficient CO2 separation and can lead to negative CO2 emissions when combined with carbon capture and storage. A potential challenge in developing CLC technology is the effects of alkali metal-containing compounds released during fuel conversion. This study investigates the interactions between alkali and an oxygen carrier (OC), CaMn0.775Ti0.125Mg0.1O3-δ, to better understand the fate of alkali in CLC. A laboratory-scale fluidized bed reactor is operated at 800–900 °C in oxidizing, reducing and inert atmospheres to mimic CLC conditions. Alkali is fed to the reactor as aerosol KCl particles, and alkali in the exhaust is measured online with a surface ionization detector. The alkali concentration changes with gas environment, temperature, and alkali loading, and the concentration profile has excellent reproducibility over repeated redox cycles. Alkali-OC interactions are dominated by alkali uptake under most conditions, except for a release during OC reduction. Uptake is significant during stable reducing conditions, and is limited under oxidizing conditions. The total uptake during a redox cycle is favored by a high alkali loading, while the influence of temperature is weak. The implications for the understanding of alkali behavior in CLC and further development are discussed.
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| 20. |
- Andersson, Viktor, 1983, et al.
(författare)
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Alkali-wall interactions in a laboratory-scale reactor for chemical looping combustion studies
- 2021
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Ingår i: Fuel Processing Technology. - : Elsevier BV. - 0378-3820 .- 1873-7188. ; 217
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Tidskriftsartikel (refereegranskat)abstract
- Alkali metal-containing compounds are readily released during thermal conversion of solid fuels, and may have both detrimental and beneficial effects on chemical looping combustion. Here, we characterize alkali interactions with the inner walls of a laboratory-scale reactor under oxidizing, reducing and inert conditions at temperatures up to 900 °C. KCl aerosol particles are continuously introduced to the stainless steel reactor and the alkali concentration is measured on-line with a surface ionization detector. Aerosol particles evaporate at temperatures above 500 °C and KCl molecules rapidly diffuse to the reactor wall. Up to 92% of the alkali reaching the wall below 700 °C remains adsorbed, while re-evaporation is important at higher temperatures, where up to 74% remains adsorbed. Transient changes in alkali concentration are observed during repeated redox cycles, which are associated with changes in chemical composition of the wall material. Metal oxides on the reactor wall are partially depleted under reducing conditions, which allow for the formation of a new potassium-rich phase that is stable in a reducing atmosphere, but not under inert conditions. The observed wall effects are concluded to be extensive and include major transient effects depending on gas composition, and the implications for laboratory studies and improved experimental methodology are discussed.
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| 21. |
- Andersson, Viktor, 1983, et al.
(författare)
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Design and first application of a novel laboratory reactor for alkali studies in chemical looping applications
- 2023
-
Ingår i: Fuel Processing Technology. - 0378-3820. ; 252
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Tidskriftsartikel (refereegranskat)abstract
- Alkali compounds are readily released during biomass conversion and their complex interactions with reactor walls and sampling equipment makes detailed investigations challenging. This study evaluates a novel laboratory-scale fluidized bed reactor for chemical looping combustion (CLC) studies. The reactor design is based on detailed consideration of the behavior of alkali-containing molecules and aerosol particles and is guided by computational fluid dynamic simulations. The design allows for interactions between gaseous alkali and a fluidized bed, while minimizing alkali interactions with walls before and after the fluidized bed. The function of the laboratory reactor is demonstrated in experiments using online gas and alkali analysis. Alkali is continuously fed to the reactor as KOH or KCl aerosol with and without a fluidized bed of the oxygen carrier CaMn0.775Ti0.125Mg0.1O3-δ present in inert, reducing and oxidizing conditions at temperatures up to 900 °C. Alkali uptake by the OC is characterized in all conditions, and observed to sensitively depend on gas composition, reactor temperature and type of alkali compound. The experimental setup is concluded to have a significantly improved functionality compared to a previously used reactor, which opens up for detailed studies of interactions between alkali compounds and oxygen carriers used in CLC.
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| 22. |
- Andersson, Viktor, 1983, et al.
(författare)
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Gaseous alkali interactions with ilmenite, manganese oxide and calcium manganite under chemical looping combustion conditions
- 2024
-
Ingår i: Fuel Processing Technology. - 0378-3820 .- 1873-7188. ; 254
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Tidskriftsartikel (refereegranskat)abstract
- Alkali species present in biomass pose significant challenges in chemical looping combustion (CLC) processes and other thermal conversion applications. The interactions between different alkali species and three common oxygen carrier (OC) materials that are considered to be state of the art in CLC applications have been investigated. A dedicated fluidized bed laboratory reactor was used to study interactions of KCl, NaCl, KOH, NaOH, K2SO4 and Na2SO4 with manganese oxide, calcium manganite and ilmenite. Alkali vapor was generated by injecting alkali salts under reducing, oxidizing and inert conditions at 900 °C. Gaseous species were measured online downstream of the reactor, and the efficiency of alkali uptake was determined under different conditions. The result show significant alkali uptake by all OCs under the studied conditions. Ilmenite shows near complete alkali uptake in reducing conditions, while manganese oxide and calcium manganite exhibited less effective alkali uptake, but have advantages in terms of fuel conversion and oxidizing efficiency. Alkali chlorides, sulfates and hydroxides show distinctly different behavior, with alkali hydroxides being efficiently captured all three investigate OC materials. The findings contribute to a deeper understanding of alkali behavior and offer valuable guidance for the design and optimization of CLC with biomass.
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| 23. |
- Andersson, Viktor, 1994, et al.
(författare)
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Online Speciation of Alkali Compounds by Temperature-Modulated Surface Ionization: Method Development and Application to Thermal Conversion
- 2024
-
Ingår i: ENERGY & FUELS. - 0887-0624 .- 1520-5029. ; 38:3, s. 2046-2057
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Tidskriftsartikel (refereegranskat)abstract
- A novel method for online speciation of potassium- and sodium-containing compounds has been described and demonstrated. The method is based on a temperature-modulated surface ionization (TMSI) technique and may be used to determine the concentrations of alkali chlorides, hydroxides, carbonates, and sulfates in high-temperature processes. The measurement device is a further development of a surface ionization detector (SID) commonly used for online alkali measurements in combustion, gasification, and pyrolysis research. Discrimination between sodium and potassium compounds is made possible by differences in their aerosol evaporation characteristics as a function of temperature combined with the desorption kinetics of alkali on a hot platinum filament. The method is evaluated in laboratory experiments with known alkali salt concentrations. An experimental procedure where the platinum filament in the SID is regularly shifted between three temperatures is concluded to provide sufficient selectivity and time resolution for common applications. The TMSI method is successfully applied to characterize the emission of alkali compounds during pyrolysis of pine wood. The emissions during low-temperature pyrolysis are dominated by KOH, while similar amounts of KOH and NaOH are subsequently emitted from the remaining char and ash. The ability of real-time characterization of individual sodium and potassium compounds opens up new means to understand and optimize solid fuel conversion of common fuels such as low-grade biomass, waste, and coal.
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| 24. |
- Boman, Johan, 1955, et al.
(författare)
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ASSESSING THE ENVIRONMENT WITH X-RAY FLUORESCENCE
- 2011
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Ingår i: Advances in X-ray Analysis. - 0376-0308. ; 54, s. 266-279
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Tidskriftsartikel (refereegranskat)abstract
- In this paper we will introduce the general benefits of X-Ray Fluorescence spectrometry (XRF) for assessing the condition of the outer environment, especially where ambient aerosol particles are causing environmental disturbances. Examples from recent environmental studies are presented, and energy dispersive XRF is concluded to be a powerful, nondestructive yet easily applicable tool to supply detailed elemental information of particles collected in different applications. The further development and future potential of the method for detailed analysis of aerosol particles are discussed.
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| 25. |
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