IR monitoring of absorbent composition and degradation during pilot plant operation
- Authors: Puxty, Graeme , Bennett, Robert , Conway, Will , Webster-Gardiner, Mike , Yang, Qi , Pearson, Pauline , Cottrell, Aaron , Huang, Sanger , Feron, Paul , Reynolds, Alicia , Verheyen, Vincent
- Date: 2020
- Type: Text , Journal article
- Relation: Industrial and Engineering Chemistry Research Vol. 59, no. 15 (2020), p. 7080-7086
- Full Text: false
- Reviewed:
- Description: The monitoring of the absorbent during the operation of CO2 separation processes is a necessary and challenging task. The most common absorbent used is an aqueous amine solution. Traditional approaches to analysis such as titration and chromatography are time-consuming and only provide limited information. This hinders the ability of process operators to rapidly respond to changes in operating conditions. In this work, a combination of infrared (IR) spectroscopy and principle component regression (PCR) analyses have been demonstrated as a rapid and reliable technique to determine the composition of an absorbent during a pilot plant campaign at a brown coal power station. The concentration of amine, a degradation product, CO2, and water was monitored throughout the campaign by a method that provided results in minutes. The results were verified by independent sample analysis using acid-base titration, high-performance liquid chromatography (HPLC), and 13C NMR spectroscopy. It was necessary to use spectral windowing when building the IR-PCR model, but this resulted in a robust and reliable method that has been demonstrated to work in a real-world process environment. © 2019 American Chemical Society.
- Description: The authors wish to acknowledge the financial assistance provided by the Brown Coal Innovation Australia, Ltd., a private member-based company with funding contracts through the Australian National Low Emissions Coal Research and Development, Ltd. (ANLEC R&D) and the Victorian State Government. The work described here was made possible through the PICA project, a collaboration between AGL Loy Yang, IHI, and CSIRO that aims to advance post-combustion CO 2 -capture technology in Australia.
Increasing hydrogen energy efficiency by heat integration between fuel cell, hydride tank and electrolyzer
- Authors: Ghayur, Adeel , Verheyen, Vincent
- Date: 2019
- Type: Text , Conference proceedings , Conference paper
- Relation: 2019 IEEE Asia-Pacific Conference on Computer Science and Data Engineering, CSDE 2019
- Full Text: false
- Reviewed:
- Description: Chemical processes offer untapped potential to increase overall system efficiencies by synergizing renewable hydrogen storage with dispatchable renewable energy facilities. In this study an Energy Storage Facility model is developed and simulation conducted to examine this potential. The model incorporates a Solid Oxide Fuel Cell (SOFC) integrated with a Magnesium Hydride (MgH2) Tank and an alkaline electrolyzer linked to the power grid. Surplus grid power is converted to hydrogen and stored as magnesium hydride. This storage process generates waste heat which is used to partially offset the water heating requirement of the electrolyzer. Simulation results demonstrate 20% reduction in parasitic heat energy consumption using this waste heat. Stored hydrogen provides power on demand via the SOFC. Waste heat from SOFC fulfils the desorption heat demand of the MgH2 Tank. Simulation results reveal waste heat from the SOFC is just enough to preheat oxygen and hydrogen and desorb hydrogen from the MgH2 tank. These results are encouraging, warranting further investigation into metal hydride storage to help Australia's transition towards renewable energy resources. © 2019 IEEE.
Soluble organic components of winery wastewater and implications for reuse
- Authors: Mosse, Kim , Verheyen, Vincent , Cruickshank, Alicia , Patti, Antonio , Cavagnaro, Timothy
- Date: 2013
- Type: Text , Journal article
- Relation: Agricultural Water Management Vol. 120, no. (2013), p. 5-10
- Full Text: false
- Reviewed:
- Description: Sustainable reuse of winery wastewaters (WWW) via land application is of interest given the increasing industrialization of wine production. However, before WWW reuse can become widespread, its chemical composition and consequently its potential long-term impact need to be investigated. In this study, soluble materials in influent and effluent waters from different WWW treatment plants were analyzed at the molecular level using Solid Phase Micro Extraction Gas Chromatography/Mass Spectrometry (SPME GC–MS). The analytical focus was on key compound classes with potential for environmental harm, the majority of which were reduced by all treatments considered here. The effluents retained considerable quantities of recalcitrant phenolic compounds, which is of concern due to their potential phytotoxicity and proven resistance to aerobic degradation. This research highlights the importance of understanding the nature of organic material in WWW to ensure sustainable reuse.
Characterization of trace organic compounds in recycled water used for irrigation on turf and comparison with rain
- Authors: Heaven, M. , Verheyen, Vincent , Cruickshank, Alicia , Wild, Karl , Watkins, Mark , Nash, David
- Date: 2012
- Type: Text , Journal article
- Relation: Agricultural Water Management Vol. 103, no. (2012), p. 176-181
- Full Text: false
- Reviewed:
- Description: Wastewaters are increasingly being reused in public spaces to supplant the use of potable water. In this study we investigated possible trace organic contaminants in wastewater from a dairy factory applied to a recreation reserve. Samples were taken of recycled dairy factory wastewater used to irrigate the reserve and from the subsurface drainage system after irrigation and after rainfall. Using gas chromatography–mass spectrometry, it was found that irrigation drainage mostly contained different compounds to those in rainfall drainage. This drainage water was found to contain residues of three agrochemicals (dicamba, 0.4 ± 0.07
Rapid determination of ultra-trace concentrations of mercury in plants and soils by cold vapour inductively coupled plasma-optical emission spectrometry
- Authors: Hellings, Jacqueline , Adeloju, Samuel , Verheyen, Vincent
- Date: 2013
- Type: Text , Journal article
- Relation: Microchemical Journal Vol. 111, no. 62-66 (2013), p.62-66
- Full Text: false
- Reviewed:
- Description: A method is described for rapid and reliable determination of ultra-trace concentrations of mercury in plant and soil samples by cold vapour inductively coupled plasma-optical emission spectrometry (CV-ICP-OES). Under the established optimum conditions, a detection limit of 3 ng g− 1 was achieved. Rapid decomposition of soil and plant samples were achieved with microwave digestion with a 3:1 HNO3:HCl mixture for only 10 min, enabling close to 100% recovery of mercury. Choice of sample storage condition and nature of sample (dried, wet or frozen) had significant influence on mercury concentrations found in plant and soil samples. Storage of samples as frozen, followed by digestion without drying or on as received basis gave optimum recovery of mercury in the samples. Verification of the effectiveness of the CV-ICP-OES method for reliable mercury determination in plants and soil with microwave digested certified soil and spiked plant samples gave close to 100% and 95–103% recoveries, respectively. The CV-ICP-OES method was successfully applied to the determination of mercury in plant and soil samples from a local Australian forest. The mercury concentrations found in plants range from 23.5 to 78.5 ng g− 1, while those found in soils range from 30.1 to 61.7 ng g− 1.
Characterization of organic particulates present in milk factory process waters used for reuse along with aerobically digested effluent wastewater
- Authors: Verheyen, Vincent , Cruickshank, Alicia , Wild, Karl , Heaven, M. , McGee, R. , Watkins, Mark , Nash, David
- Date: 2010
- Type: Text , Journal article
- Relation: Bioresource Technology Vol. 102, no. 2 (2010), p. 2118-2125
- Full Text: false
- Reviewed:
- Description: Wastewater from a dairy processor is being reused and recycled both within the plant and for irrigation. Flash pyrolysis GC–MS was used to examine nitrogen and phenol containing compounds (M.W. = 35 to 450 g/mol) in the particulate fraction of the milk condensate, combined clean wastewater and aerobic bioreactor effluent. For comparison, the particulates were also prepared for standard GC–MS analyses using conventional solvent extraction methods. Compounds detected by pyrolysis GC–MS were found mostly in the bioreactor with the amino acid arginine (220 mg/kg) and the amino acid derivative 1-methyl-5-oxo-L-proline methyl ester (130 mg/kg) found at the highest concentrations. In comparison, sterols detected in the effluent were found at higher concentrations when using solvent extraction indicating some degradation with pyrolysis GC–MS. However, with few exceptions, particulates were generally found not to act as passive collectors capable of concentrating less water soluble chemicals.
Structural characterisation of Middle Jurassic, high-volatile bituminous Walloon Subgroup coals and correlation with the coal seam gas content
- Authors: Chaffee, Alan , Lay, Galinda , Marshall, Marc , Jackson, William , Fei, Yi , Verheyen, Vincent , Cassidy, Peter , Scott, Steven
- Date: 2010
- Type: Text , Journal article
- Relation: Fuel Vol. 89, no. 11 (2010), p. 3241-3249
- Full Text: false
- Reviewed:
- Description: The structure of a suite of high-volatile, bituminous Surat Basin, Queensland coals has been investigated by a combination of analytical probes. These included elemental analyses, pyrolysis-gas chromatography-mass spectroscopy and Fourier transform infrared spectroscopy, together with a study of their liquefaction products in both tetralin and solvent free-tin catalysed hydrogenations. Samples were gathered across a 300 m depth interval intersected by the sampling well. Most techniques revealed clear but subtle differences in structure as a function of depth. The oils produced by solvent free-tin catalysed hydrogenation, however, showed very distinct dependence with depth and the waxy content, as indicated by 1H-NMR, could be correlated with the coal seam gas content
Thermochemolysis of winery wastewater particulates-molecular structural implications for water reuse
- Authors: Mosse, Kim , Verheyen, Vincent , Cruickshank, Alicia , Patti, Antonio , Cavagnaro, Timothy
- Date: 2012
- Type: Text , Journal article
- Relation: Journal of Analytical and Applied Pyrolysis Vol. 97, no. 164-170 (2012), p.
- Full Text: false
- Reviewed:
- Description: Environmental concerns have increased the interest in winery wastewater remediation and reuse. These practices require more detailed understanding of wastewater composition to ensure optimum usage, and to minimize the risk of long term soil degradation and grape contamination. Particulate organic matter is an important contributor to the carbon burden in winery wastewaters. This article investigates the molecular structure of particulates from the most common winery wastewater treatment processes via infrared spectroscopic and thermochemolysis-gas chromatography/mass spectrometry techniques. Study of the organic composition of both influent and effluent particles enabled further insight into which compounds could prove problematic during treatment and on discharge. The yield and molecular structure of desorbed or “guest” compounds were found to strongly correlate with those produced during pyrolytic cracking. These “guest” compounds and macromolecular fragments form a continuum whose separation is based on molecular size. Polyphenolic and lignin derived compounds tended to survive the water treatment processes within assemblages of microbial detritus. No evidence was found for particles adsorbing and concentrating other unrelated organics such as anthropogenic chemicals from winery wastewaters. Any release of particulates will require careful management to prevent localized accumulation of recalcitrant compounds to toxic levels.
Soluble, semivolatile phenol and nitrogen compounds in milk-processing wastewaters
- Authors: Verheyen, Vincent , Cruickshank, Alicia , Wild, Karl , Heaven, M. , McGee, R. , Watkins, Mark , Nash, David
- Date: 2009
- Type: Text , Journal article
- Relation: Journal of Dairy Science Vol. 92, no. 7 (2009), p.
- Full Text: false
- Reviewed:
- Description: Potable water is an essential and major input in processing our food supplies, and the continued growth in food manufacturing is placing increased pressure on this limited resource. Recycling and reuse of factory wastewater can lessen potable water use but requires a detailed understanding of wastewater properties. This study uses solid-phase extraction techniques with gas chromatography-mass spectrometry analysis to investigate trace-level semivolatile organic species in various waste and reference waters associated with the Burra Foods milk-processing plant located in Southeastern Australia. Our focus was on contaminants containing phenolic and heterocyclic nitrogen functional groups, which, because of their toxicity and persistence, may limit options for water recycling and reuse. Effluent from the wastewater treatment plant of the factory showed both the highest soluble carbon burden (47 mg/kg) and concentrations of target compounds. The target species found in these effluents included methyl phenol (13 mg/kg), hydroxy indole (9.8 mg/kg), synthetic tolyltriazoles (5.1 mg/kg) and alkyl phenol ethoxylates (0.2 mg/kg). Given the environmental stability of the tolyltriazoles, they may act as chemical markers where these effluents are used for purposes such as irrigation. Milk evaporator condensate waters, in contrast to the effluent, contained very few target species, with only low levels of pyrrolidine and piperidine derivatives such as ethylglutarimide (450 mug/L) detected. Although there were fewer target microcontaminants overall in the potable and creek reference waters, these samples had characteristic profiles. The potable water analysis revealed hydroxy cineole (2.1 microg/L) and the creek analysis revealed dichlorohydroxyacetophenone (0.3 microg/L), which were not detected in other waters. The compounds found in the wastewaters are likely to have been derived from milk or synthetic chemicals used in factory operations. The presence of nitrogen compounds in all the different milk-processing waters suggest their likely source was milk, probably milk phosphoproteins subjected to thermal, chemical, or microbial degradation. Our benign results for the condensates suggest it may be possible to substitute condensate for potable water with minimal pretreatment, both within the plant and in other applications, such as irrigation of recreation turf.
Towards commercial scale postcombustion capture of CO2 with monoethanolamine solvent: key considerations for solvent management and environmental impacts
- Authors: Cruickshank, Alicia , Verheyen, Vincent , Adeloju, Samuel , Meuleman, Erik , Feron, Paul
- Date: 2012
- Type: Text , Journal article
- Relation: Environmental Science & Technology Vol. 46, no. 7 (2012), p. 3643-3654
- Full Text: false
- Reviewed:
- Description: Chemical absorption with aqueous amine solvents is the most advanced technology for postcombustion capture (PCC) of CO2 from coal-fired power stations and a number of pilot scale programs are evaluating novel solvents, optimizing energy efficiency, and validating engineering models. This review demonstrates that the development of commercial scale PCC also requires effective solvent management guidelines to ensure minimization of potential technical and environmental risks. Furthermore, the review reveals that while solvent degradation has been identified as a key source of solvent consumption in laboratory scale studies, it has not been validated at pilot scale. Yet this is crucial as solvent degradation products, such as organic acids, can increase corrosivity and reduce the CO2 absorption capacity of the solvent. It also highlights the need for the development of corrosion and solvent reclamation technologies, as well as strategies to minimize emissions of solvent and degradation products, such as ammonia, aldehydes, nitrosamines and nitramines, to the atmosphere from commercial scale PCC. Inevitably, responsible management of aqueous and solid waste will require more serious consideration. This will ultimately require effective waste management practices validated at pilot scale to minimize the likelihood of adverse human and environmental impacts from commercial scale PCC.
Solubilisation of Victorian brown coal in 'distillable' DIMCARB
- Authors: Qi, Ying , Tikkoo, Tarun , Verheyen, Vincent , Ranganathan, Vijayaraghavan , MacFarlane, Douglas , Chaffee, Alan
- Date: 2013
- Type: Text , Conference paper
- Relation: 30th Annual International Pittsburgh Coal Conference 2013, PCC 2013
- Full Text: false
- Reviewed:
- Description: Victorian (Australia) brown coal is an abundant and cheap energy resource. There is intense interest in identifying new opportunities for its efficient and clean use, for example by solubilisation to produce high quality fuel or chemicals. Ionic liquids (ILs) have been applied increasingly in recent years to solubilize and recover cellulose, lignin and other components from complex biomass mixtures. Conventional ILs are not distillable and it can be difficult to separate the soluble product from the solvent. However, there is a group of ILs, produced by the association of a secondary amine and CO2 that are 'distillable' in that they will dissociate back to the respective amine and CO2 at moderate temperature to facilitate recovery. They can then be re-associated (recycled) by condensation at lower temperature. The simplest form of such ILs, DIMCARB, consists of dimethylamine associated with CO2 at a molar ratio of 2:1. DIMCARB has previously been found to be superior (in terms of solubility) to other ILs in this group for the extraction of a Victorian brown coal. In this study the extractability of a woody coal sample was compared with a run-of-mine (ROM) sample, both without pretreatment. The wet coal was mixed with DIMCARB at a dry mass ratio of 1 to 20 for 24 hours at room temperature. The soluble product was recovered by centrifuge and acid washed to remove residual DIMCARB. An extraction yield of 25% was achieved for the ROM sample, while for the woody coal the yield was only 10%. The recovered products were characterized by a range of chemical techniques including FTIR and Pyrolysis GC-MS. The lower solubility of the woody coal seems to be associated with a high degree of oxygen containing aromatic components. The nature of this difference and the selectivity of the extraction are discussed.
Dynamic modelling and optimisation of flexible operation in post-combustion CO2 capture plants - A review
- Authors: Bui, Mai , Gunawan, Indra , Verheyen, Vincent , Feron, Paul , Meuleman, Erik , Adeloju, Samuel
- Date: 2014
- Type: Text , Journal article , Review
- Relation: Computers and Chemical Engineering Vol. 61, no. (2014), p. 245-265
- Full Text: false
- Reviewed:
- Description: The drive for efficiency improvements in post-combustion CO2 capture (PCC) technologies continues to grow, with recent attention being directed towards flexible operation of PCC plants. However, there is a lack of research into the effect of process disturbances when operating flexibly, justifying a need for validated dynamic models of the PCC process. This review critically examines the dynamic PCC process models developed to date and analyses the different approaches used, as well as the model complexity and their limitations. Dynamic process models coupled with economic analysis will play a crucial role in process control and optimisation. Also discussed are key areas that need to be addressed in future dynamic models, including the lack of reliable dynamic experimental data for their validation, development of feasible flexible operation and process control strategies, as well as process optimisation by integrating accurate process models with established economic analysis tools. © 2013 Elsevier Ltd.
Ambient temperature solubilisation of brown coal in ammonium carbamate ionic liquids
- Authors: Qi, Ying , Verheyen, Vincent , Vijayaraghavan, Ranganathan , MacFarlane, Douglas , Chaffee, Alan
- Date: 2016
- Type: Text , Journal article
- Relation: Fuel Vol. 166, no. (2016), p. 106-115
- Full Text: false
- Reviewed:
- Description: Coal solubilisation is often a necessary step for the alternative utilisation of the cheap and abundant brown coal resources in the State of Victoria, Australia, such as producing high quality fuel or chemicals. A series of ionic liquids (ILs), ammonium carbamates, formed by the association of carbon dioxide (CO2) with low molecular weight secondary amines, were investigated as solvents for the solubilisation of Victorian brown coal. The ionic liquid was mixed with a Loy Yang coal at a mass ratio of 20 to 1 (dry basis) for 24 h at ambient temperature. The solubilisation yields of the coal using three such ILs from dimethyl-, diallyl- and dipropyl-amines, respectively, were between 18% and 23%. Repeated solubilisation of the coal with fresh solvent achieved higher yields, with the highest at 66% by the carbamate formed from dimethylamine (DIMCARB). The variations in chemical structure between the products were compared by elemental analysis and a variety of spectroscopic techniques (FTIR, Solid State 13C NMR and Py-GC-MS). The soluble products of the initial solubilisation were more aliphatic than their parent coal. The less polar ILs formed from diallyl- and dipropyl-amines (DACARB and DPCARB) appeared to be more selective for high molecular weight triterpenoids than DIMCARB. Subsequent treatment tended to dissolve more aromatic components. © 2015 Elsevier Ltd. All rights reserved.
Biological and chemical treatment technologies for waste amines from CO₂ capture plants
- Authors: Ghayur, Adeel , Verheyen, Vincent , Meuleman, Erik
- Date: 2018
- Type: Text , Journal article
- Relation: Journal of Environmental Management Vol. 241, no. (2018), p. 514-524
- Full Text: false
- Reviewed:
- Description: Amine-based carbon dioxide capture is the most mature technology for reducing flue gas CO₂ emissions. It has been postulated and observed during commercialisation of this technology that significant quantities of waste amines are produced. Further industrial implementation of this technology requires adequate disposal or valorisation options for this waste. This review presents an analysis of seven biological and chemical technologies for waste amine amelioration or valorisation. Of these, the biological treatments are identified as being more mature for industrial application with the capacity for marketable product generation. Slow speed is the main drawback of the biological processes but this does not hinder their commercial viability. Using waste amine for NOx reduction in power stations is a secondary option, where it seems probable that the amount of waste amine generated in the CO₂ capture plant is sufficient to fulfil the DeNOx requirements of the flue gas. This route, however, requires investigation into the impact of waste amine impurities on the power station and the CO₂ capture plant operations.
- Description: Amine-based carbon dioxide capture is the most mature technology for reducing flue gas CO emissions. It has been postulated and observed during commercialisation of this technology that significant quantities of waste amines are produced. Further industrial implementation of this technology requires adequate disposal or valorisation options for this waste. This review presents an analysis of seven biological and chemical technologies for waste amine amelioration or valorisation. Of these, the biological treatments are identified as being more mature for industrial application with the capacity for marketable product generation. Slow speed is the main drawback of the biological processes but this does not hinder their commercial viability. Using waste amine for NOx reduction in power stations is a secondary option, where it seems probable that the amount of waste amine generated in the CO capture plant is sufficient to fulfil the DeNOx requirements of the flue gas. This route, however, requires investigation into the impact of waste amine impurities on the power station and the CO capture plant operations.
Comparison of sample preparation methods for the GC–MS analysis of monoethanolamine (MEA) degradation products generated during post-combustion capture of CO2
- Authors: Reynolds, Alicia , Verheyen, Vincent , Adeloju, Samuel , Chaffee, Alan , Meuleman, Erik
- Date: 2016
- Type: Text , Journal article
- Relation: International Journal of Greenhouse Gas Control Vol. 52, no. (2016), p. 201-214
- Full Text: false
- Reviewed:
- Description: As the development of chemical absorption technology for post-combustion capture (PCC) of CO2 from coal-fired power station flue gases proceeds towards commercial deployment, the focus on establishing a thorough understanding of the degradation of the aqueous amine absorbents is increasing. However, there is a need to develop and demonstrate robust analytical methods that are capable of measuring the concentrations of amine degradation products in aqueous monoethanolamine (MEA) matrix during pilot-scale PCC. In this study, sample cleanup and derivatisation methods that enable reliable and robust analysis of MEA degradation products by GC–MS are described. Two sample cleanup methods were evaluated: dehydration (by rotary evaporation and molecular sieves) and cation exchange. The cation exchange sample preparation method was preferred for the analysis of organic degradation products in these samples because it achieved higher recovery and repeatability of GC–MS measurements than those obtained with the dehydration method. Furthermore, the cation exchange method resulted in less continued amine degradation during subsequent analysis steps because of its ability to separate acidic analytes from basic analytes, as well as to remove some inorganic interferences. Further improvement of the sensitivity, repeatability and accuracy of this GC–MS analytical method can be accomplished by: (a) increasing the scale of the cation exchange and/or derivatisation procedures; (b) optimizing the derivatisation reaction conditions; and (c) using a narrower bore (e.g. 0.25 mm ID) GC–MS column. The proposed cation exchange and derivatisation procedures can be readily adopted for the quantification of organic degradation products in other aqueous amine absorbents to provide important insights into the degradation of amine absorbents during PCC of CO2. © 2016 Elsevier Ltd
Structural elucidation of humic acids extracted from Pakistani lignite using spectroscopic and thermal degradative techniques
- Authors: Nasir, Saqib , Sarfaraz, Tahira , Verheyen, Vincent , Chaffee, Alan
- Date: 2011
- Type: Text , Journal article
- Relation: Fuel Processing Technology Vol. 92, no. 5 (2011/05/01/ 2011), p. 983-991
- Full Text: false
- Reviewed:
- Description: The present paper describes the characterization of Pakistan lignite coal, derived humic acids (HAL) and nitrohumic acids (NHA) along with the standard leonardite humic acids (LHA). The study utilized chromatographic and spectroscopic techniques to characterize the structure of coal and derived materials. Pyrolysis coupled to gc/ms was conducted with and without methylating agent (tetramethyl ammonium hydroxide). The pyrolysis study resulted in releasing mainly fatty acid methyl esters, different series of hydrocarbons and α, ω-dicarboxylic acid methyl esters. Triterpenoids, syringic and ρ-coumaric compounds and aromatic compounds derived from lignin moieties were also detected. Fourier transform infrared (FT-IR) and NMR data helped to evaluate the influence of coal rank on regeneration and nitration processes with respect to chemical structural composition of coal and derived materials. FT-IR spectra of four materials were similar except that NHA showed an absorption band at 1532cm−1, thus confirming the presence of -NO2 groups. 13C NMR indicated higher aromaticity and less hydroxylalkyl material in HAL than NHA. The elemental composition and acid functional group content of four materials were also reported. The combination of results from different analytical techniques gives an improved understanding of the Pakistan coal nature and helpful for its future utilization.
Evaluation of methods for monitoring MEA degradation during pilot scale post-combustion capture of CO
- Authors: Reynolds, Alicia , Verheyen, Vincent , Adeloju, Samuel , Chaffee, Alan , Meuleman, Erik
- Date: 2015
- Type: Text , Journal article
- Relation: International Journal of Greenhouse Gas Control Vol. 39, no. (2015), p. 407-419
- Full Text: false
- Reviewed:
- Description: Amine degradation is an important and current focus in the development of chemical absorption technology based on the use of aqueous amines for post-combustion capture (PCC) of CO
Monoethanolamine degradation during Pilot-Scale post-combustion capture of CO₂ from a brown coal-fired power station
- Authors: Reynolds, Alicia , Verheyen, Vincent , Adeloju, Samuel , Chaffee, Alan , Meuleman, Erik
- Date: 2015
- Type: Text , Journal article
- Relation: Energy & Fuels Vol. 29, no. 11 (2015), p. 7441-7455
- Full Text: false
- Reviewed:
- Description: The use of aqueous amines, such as monoethanolamine (MEA, 2-aminoethanol), for post-combustion capture (PCC) of CO2 from fossil-fuel-fired power station flue gases leads to undesirable reactions with oxygen, SO2, and NO2. This study has used a gas chromatography with mass spectrometry detection (GC-MS) method to measure the changes in concentrations of organic compounds in samples of a 30% (w/w) aqueous MEA absorbent obtained from CSIRO's PCC pilot plant operating at AGL's Loy Yang brown coal-fired power station in Latrobe Valley, Victoria, Australia. This aqueous MEA absorbent was previously used for more than 700 h of PCC, and the collected samples represent a further 834 h of PCC operation. These data provide a new perspective on the close, interdependent relationships between corrosion and amine degradation reactions. Other important outcomes include confirmation that (a) organic degradation products identified during laboratory-scale trials were also produced during pilot-scale PCC and (b) N-(2-hydroxyethyl)imidazole (HEI) is a suitable molecular marker for oxidative degradation of MEA. This investigation has also highlighted areas that require further research, including (a) determination of oxidative degradation mechanisms in both the presence and absence of dissolved transition metals, (b) determination of parameters that limit oxidative degradation during pilot-scale PCC, (c) investigation of the antioxidative or oxygen-scavenging properties of partially oxidized amine absorbents during PCC, and (d) measurement of the concentrations of glycine, glycolic acid, and other potential organic acids during PCC. [ABSTRACT FROM AUTHOR]
- Description: The use of aqueous amines, such as monoethanolamine (MEA, 2-aminoethanol), for post-combustion capture (PCC) of
Primary sources and accumulation rates of inorganic anions and dissolved metals in a MEA absorbent during PCC at a brown coal-fired power station
- Authors: Reynolds, Alicia , Verheyen, Vincent , Adeloju, Samuel , Chaffee, Alan , Meuleman, Erik
- Date: 2015
- Type: Text , Journal article
- Relation: International Journal of Greenhouse Gas Control Vol. 41, no. (2015), p. 239-248
- Full Text: false
- Reviewed:
- Description: Post-combustion capture (PCC) of CO2 from fossil fuel-fired power station flue gas is one of many technologies that are being developed to reduce anthropogenic greenhouse gas emissions in the medium term. Wet-gas scrubbing using aqueous amines is currently the most mature PCC technology suitable for separating CO2 from coal-fired power station flue gases. In this study, a series of twelve samples of a degraded 30% (w/w) MEA absorbent were obtained over a six month pilot scale PCC campaign at a brown coal-fired power station in Australia. These samples were used to investigate the accumulation of heat-stable salts, inorganics and minerals. The heat-stable salts concentration increased from 0.80 to 2.29% (w/w, as MEA) and organic acids from the oxidative degradation of MEA were the largest component of heat-stable salts. Acid gases such as SOx and NOx, make-up water, ultra-fine fly-ash and corrosion were all sources of the minerals and inorganics that accumulated in the aqueous MEA absorbent. Corrosion was the single biggest contributor of transition metals and the abrupt change in ratios of Fe, Cr and Mo suggests that the dominant corrosion mechanism may have changed towards the end of the campaign. The rapid accumulation of minerals and inorganics during this PCC campaign highlights the importance of continuing research into the interactions between amine absorbents and inorganic or mineral contaminants. The data presented in this study are an important resource for design of laboratory scale experiments to investigate these physical and chemical interactions between aqueous amines, minerals and inorganics.
Degradation of amine-based solvents
- Authors: Reynolds, Alicia , Verheyen, Vincent , Meuleman, Erik
- Date: 2016
- Type: Text , Book chapter
- Relation: Absorption-Based Post-Combustion Capture of Carbon Dioxide Chapter 16 p. 399-423
- Full Text: false
- Reviewed:
- Description: Degradation of aqueous amines during post-combustion capture (PCC) of CO2 from fossil-fuel flue gases by wet gas scrubbing can lead to reduced energy efficiency, operational instability, increased corrosion, and unwanted emissions to the environment. Oxidative amine degradation and the accumulation of heat-stable salts primarily occur during absorption of CO2, whereas carbamate polymerization (also called thermal degradation) primarily occurs during desorption of CO2 and thermal amine reclamation. Oxidative degradation is closely related to corrosion, catalyzed by dissolved metal ions, and can be exacerbated by intermittent operation of PCC. Other important reactions, such as nitrosation, occur at much slower rates but can produce environmentally sensitive compounds. The ability to measure the concentrations of individual compounds or monitor amine degradation during PCC is important for managing amine degradation during PCC and demonstrating compliance with environmental regulations. Although some suitable analytical methods are available, further work is needed before they could satisfy the rigorous statutory and legal requirements. Strategies for avoiding and managing amine degradation need to be integrated into all PCC activities including: selecting degradation-resistant amines, ensuring adequate pretreatment of CO2-rich flue gas, avoiding severe CO2 absorption and desorption conditions, and the use of anticorrosion and antioxidation additives. Avoiding intermittent operation of PCC processes and choosing nonmetal column packing may also assist in minimizing amine degradation. © 2016 Elsevier Ltd All rights reserved.