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Colloidal carbon interference in the treatability of pulp and paper wastewater by MBR

- Scholes, Emily, Brook-Carter, Phillip, Verheyen, Vincent

  • Authors: Scholes, Emily , Brook-Carter, Phillip , Verheyen, Vincent
  • Date: 2019
  • Type: Text , Journal article
  • Relation: Journal of Environmental Chemical Engineering Vol. 7, no. 5 (2019), p. 1-9
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  • Description: Pulp and paper wastewaters are challenging to treat due to their variability, complexity and toxicity. Membrane Bioreactor’s (MBR’s) provide high-quality filtrates but are subject to periods of low filterability / high capillary suction time (CST) which potentially limit their use in this application. There is a paucity of published literature concerning long-term operational issues in full-scale, industrial MBR’s. We hypothesised that either changes of bacterial population, alteration/reduction of bacterial metabolism or bacterial production of extra-cellular polymers (ESPs) increased CST and reduced filterability. This study, conducted over two years at the 16.4MLD Gippsland Water Factory, was structured to inform this bacterial centric hypothesis. However, no shifts in bacterial population were seen as causative of high CST and microbial stress levels and biological activity were observed to be low during high CST and no sign of toxicity was found. The strongest correlator with CST was the concentration of colloidal Total Organic Carbon of the mixed liquor suspended solids (MLSS) supernatant (following centrifugation). The carbonaceous colloids accumulated in the supernatant were named ‘Non-Centrifugable Total Organic Carbon’ (NCTOC). Their accumulation in the MLSS was found be due to their biologically refractory nature and their retention by the MBR membrane. The accumulation of NCTOC typically followed a period where the influent had a high colour and a high sodium to calcium ratio, which is consistent with a pulping by-product called ‘Black Liquor’. Additional experiments with Black Liquor allowed us to conclude that high CST can be produced by addition of Black Liquor.

Soluble organic components of winery wastewater and implications for reuse

- Mosse, Kim, Verheyen, Vincent, Cruickshank, Alicia, Patti, Antonio, Cavagnaro, Timothy

  • 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
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  • 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.

Isolation and characterisation of recalcitrant organic components from an estuarine sediment core

- Mylotte, Rosaleen, Verheyen, Vincent, Reynolds, Alicia, Dalton, Catherine, Patti, Antonio, Chang, Rung, Burdon, James, Hayes, Michael

  • Authors: Mylotte, Rosaleen , Verheyen, Vincent , Reynolds, Alicia , Dalton, Catherine , Patti, Antonio , Chang, Rung , Burdon, James , Hayes, Michael
  • Date: 2015
  • Type: Text , Journal article
  • Relation: Journal of Soils and Sediments Vol. 15, no. 1 (2015), p. 211-224
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  • Description: Purpose The purpose of this research was to isolate humic substances and humin from an estuarine sediment core using a novel sequential extraction procedure to characterise the isolates, to determine their compositions and to understand how the organic matter (OM) changes with time. Materials and methods The sediments were exhaustively extracted using the following media: 0.1 M NaOH; 0.1 M NaOH + 6 M urea; and dimethylsulphoxide (DMSO) + H2SO4 (94:6 v/v). Pyrolysis gas chromatography mass spectroscopy (pyGC/MS), and nuclear magnetic resonance (NMR) spectroscopy were the analytical tools that gave the most significant data for the characterisation of the organic isolates. Results and discussion The results indicate subtle molecular compositional differences in relation to the alkaline and alkaline-urea isolates. The humic acids (HAs) and fulvic acids (FAs) are readily solvated in aqueous alkaline media compared to the aqueous insoluble hydrophobic humin (HU) components. In addition to aliphatic hydrocarbons, peptide materials make considerable contributions to the component structures of the isolates. Aryl and O-aryl C units characteristic of lignin, and of cutan structures from plants, indicate contributions from terrestrial OM to the organic components in the HU, especially from the base of the core. The evidence suggests that components of terrestrial plant materials and of microbial biomass are preferentially preserved with time and make the major contributions to the OM retained over long time scales. The data acquired provide detailed information about the origins, compositions, nature and the associations of the OM in the estuarine sediment core. Such information provides a greater understanding of the role of these organic components in the carbon (C) sink. Conclusions Humic acids and FAs are mineralised with time whereas HU is highly recalcitrant and represents a long-term sink for organic C. Humin is a separate organic entity and does not conform to the definitions of a humic substance. Terrestrial OM is preserved over long time scales in the environment. Protein makes significant contributions to all the organic isolates and its preservation suggests encapsulation in hydrophobic domains, or interactions with clay minerals.

Solubilisation of Victorian brown coal in 'distillable' DIMCARB

- Qi, Ying, Tikkoo, Tarun, Verheyen, Vincent, Ranganathan, Vijayaraghavan, MacFarlane, Douglas, Chaffee, Alan

  • 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
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  • 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.

Simulation of an SO2 tolerant amine based post-combustion CO2 capture process

- Cousins, Ashleigh, Puxty, Graeme, Pearson, Pauline, Weiland, Ralph, Garg, Bharti, Li, Kangkang, Verheyen, Vincent, Feron, Paul

  • Authors: Cousins, Ashleigh , Puxty, Graeme , Pearson, Pauline , Weiland, Ralph , Garg, Bharti , Li, Kangkang , Verheyen, Vincent , Feron, Paul
  • Date: 2018
  • Type: Text , Journal article
  • Relation: Chemical Engineering Transactions Vol. 69, no. (2018), p. 817-822
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  • Description: Removal of multiple contaminants from flue gas streams in a single process step offers the potential to lower the cost of emissions reduction technologies. An example is the CS-Cap process, developed by CSIRO, which removes both the SO2 and CO2 from combustion flue gases. In order to further develop this process, a rate based simulation is required of not only the CO2 capture section, but also the absorption of SO2 into aqueous amine absorbents. ProTreat® simulation software was used to simulate CSIRO's Loy Yang CO2 capture pilot plant. This pilot plant has previously been used for proof-of-concept operation of the CS-Cap process. The model simulates various scenarios and flue gas conditions to determine the effect on the operating requirements of the SO2 capture stage. It reveals that the recirculating absorbent flow rates required in the SO2 capture loop are of similar magnitude to those required in the CO2 capture stage. Manipulating the operating parameters of the SO2 capture section will affect the properties, particularly sulfate concentration, of the slip stream sent for disposal/treatment. This could potentially allow the properties of the waste stream to be tailored for the particular downstream treatment used. In addition, condensation of water from the inlet flue gas stream is identified as an issue requiring further investigation. © Copyright 2018, AIDIC Servizi S.r.l.

Techno-economic analysis of a succinic acid biorefinery coproducing acetic acid and dimethyl ether

- Ghayur, Adeel, Verheyen, Vincent, Meuleman, Erik

  • Authors: Ghayur, Adeel , Verheyen, Vincent , Meuleman, Erik
  • Date: 2019
  • Type: Text , Journal article
  • Relation: Journal of Cleaner Production Vol. 230, no. (2019), p. 1165-1175
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  • Description: The production of platform chemicals via carbon negative technologies will play an important role in global efforts to mitigate climate change. Succinic acid biorefineries are commercially mature carbon negative technologies that are plagued with large waste streams in the form of hemicellulose and gypsum. Here, a techno-economic analysis assesses the viability of a succinic acid biorefinery wherein hemicellulose is converted to acetic acid and dimethyl ether, and gypsum generation is avoided. Succinic acid is a feedstock for biodegradable plastics, acetic acid replaces petroleum-derived sources, and dimethyl ether is ideally suited as an energy storage vector. Our novel biorefinery concept presents an innovative integration of commercial technologies including water-splitting bipolar membrane electrodialysis for acid purification. The modelled multiproduct biorefinery (Multi Case)annually consumes 650,000 metric tonnes (t)of pulp logs, 135,000t of methanol, 1,700,000t of water, 42,000t of CO2 and 89 MW of electricity to produce 220,000t of succinic acid, 115,000t of acetic acid and 900t of dimethyl ether. All the parasitic electricity and heat duties are fulfilled within the biorefinery. Results show a CAPEX of AUD $635,000,000, OPEX of $180,000,000 and a succinic acid Minimum Selling Price of $990/t. Sensitivity and uncertainty analyses of the Multi Case biorefinery model show it is also resilient to price fluctuations.

Towards commercial scale postcombustion capture of CO2 with monoethanolamine solvent: key considerations for solvent management and environmental impacts

- Cruickshank, Alicia, Verheyen, Vincent, Adeloju, Samuel, Meuleman, Erik, Feron, Paul

  • 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
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  • 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.

Modelling a biorefinery concept producing carbon fibre-polybutylene succinate composite foam

- Ghayur, Adeel, Verheyen, Vincent

  • Authors: Ghayur, Adeel , Verheyen, Vincent
  • Date: 2019
  • Type: Text , Journal article
  • Relation: Chemical Engineering Science Vol. 209, no. (2019), p. 1-7
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  • Description: In this study, a novel biorefinery concept producing carbon fibre-poly(butylene succinate) composite foam (CPC foam) from lignocellulose and CO 2 is modelled. The biodegradable nature of poly(butylene succinate) would allow for easy carbon fibre recovery from the CPC foam for reuse at the end of product lifecycle, thus allowing for a circular materials flow. Technical simulation results show the biorefinery consumes 417 kg of biomass, 33 kg of CO 2 , 86 kg of methanol, 23 kg of acetic anhydride, 130 kWh of electricity and 1166 kW of heat per hour. The facility generates 72 kg of CPC foam, 82 kg of carbon fibre, 24 kg of tetrahydrofuran and 50 kg of dimethyl ether (DME). DME is used to fulfil parasitic electricity requirement. These results demonstrate the technical viability of this biorefinery although, research is needed to reduce parasitic energy demand. This carbon negative biorefinery avoids carcinogens and halogens for polymeric materials synthesis by utilising green chemistry principles and lignocellulose feedstock.

Characterization of organic compounds in biochars derived from municipal solid waste

- Taherymoosavi, Sarasadat, Verheyen, Vincent, Munroe, Paul, Joseph, Stephen, Reynolds, Alicia

  • Authors: Taherymoosavi, Sarasadat , Verheyen, Vincent , Munroe, Paul , Joseph, Stephen , Reynolds, Alicia
  • Date: 2017
  • Type: Text , Journal article
  • Relation: Waste Management Vol. 67, no. (2017), p. 131-142
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  • Description: Municipal solid waste (MSW) generation has been growing in many countries, which has led to numerous environmental problems. Converting MSW into a valuable biochar-based by-product can manage waste and, possibly, improve soil fertility, depending on the soil properties. In this study, MSW-based biochars, collected from domestic waste materials and kerbsides in two Sydney's regions, were composted and pyrolysed at 450 °C, 550 °C and 650 °C. The characteristics of the organic components and their interactions with mineral phases were investigated using a range of analytical techniques, with special attention given to polycyclic aromatic hydrocarbons and heavy metal concentrations. The MSW biochar prepared at 450 °C contained the most complex organic compounds. The highest concentration of fixed C, indicating the stability of biochar, was detected in the high-temperature-biochar. Microscopic analysis showed development of pores and migration of mineral phases, mainly Ca/P/O-rich phases, into the micro-pores and Si/Al/O-rich phases on the surface of the biochar in the MSW biochar produced at 550 °C. Amalgamation of organic phases with mineral compounds was observed, at higher pyrolysis temperatures, indicating chemical reactions between these two phases at 650 °C. XPS analysis showed the main changes occurred in C and N bonds. During heat treatment, N-C/C=N functionalities decomposed and oxidized N configurations, mainly pyridine-N-oxide groups, were formed. The majority of the dissolved organic carbon fraction in both MSW biochar produced at 450 °C and 550 °C was in the form of building blocks, whereas LMW acids was the main fraction in high-temperature-biochar (59.9%). © 2017 Elsevier Ltd

A technology review for regeneration of sulfur rich amine systems

- Garg, Bharti, Verheyen, Vincent, Pearson, Pauline, Feron, Paul, Cousins, Ashleigh

  • Authors: Garg, Bharti , Verheyen, Vincent , Pearson, Pauline , Feron, Paul , Cousins, Ashleigh
  • Date: 2018
  • Type: Text , Journal article , Review
  • Relation: International Journal of Greenhouse Gas Control Vol. 75, no. (2018), p. 243-253
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  • Description: Reducing the capital cost of post combustion CO2 capture by eliminating flue gas desulfurisation (FGD) pre-treatment, requires management of the amines preferential SO2 absorption. Novel technologies such as CS-Cap restrict the impact of SO2 to only a small fraction of the amine inventory resulting in high sulfate burden amines. Traditional thermal reclamation of these spent absorbents has advantages regarding simplicity, but ranks poorly for industrial ecology around PCC. These amines require low energy regeneration technologies compatible with their physico-chemical properties that also maximise the potential for valorising by-products. This review summarises the sulfur chemistry and outlines several amine reclamation processes. It assesses the status of established and novel regeneration technologies for their applicability to high sulfur loaded amines. Should deep sulfur removal be required, a hybrid approach with initial bulk removal (as product) followed by a polishing step to further reduce sulfur is prospective. A preliminary estimation of the relative cost of using standard reclamation methods for treating Sulfur loaded CS-Cap absorbent revealed the cost would increase due to its higher sulfate burden despite comparable treatment volumes. Research gaps are identified which would enable better comparison between the costs of traditional FGD versus higher reclamation costs for combined capture technologies.

Further developments in dynamic modelling of CO2 capture from flue gas

- Dickinson, Jillian, Puxty, Graeme, Percy, Andrew, Verheyen, Vincent

  • Authors: Dickinson, Jillian , Puxty, Graeme , Percy, Andrew , Verheyen, Vincent
  • Date: 2015
  • Type: Text , Conference paper
  • Relation: 8th Vienna International Conference on Mathematical Modelling: MATHMOD 2015 p. 1-6
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  • Description: Mathematical modelling of CO2 capture from industrial flue gas by absorption into amine solutions such as monoethanolamine (MEA) has been undertaken for decades and steady state, rate-based and dynamic models have been constructed to predict the changes in the process. Recently, dynamic models have been used to predict the effect that physical operational changes have on the absorption process. As more is learnt about the chemistry of MEA and CO2 it becomes evident that the absorption system is losing available MEA, by degradation and by vaporization into the gaseous phase. This paper describes a dynamic model of the absorber column that can be used to predict the reduction of available MEA, the loss of MEA to the atmosphere, and the build-up of heat stable salts. The proposed mathematical model consists of a system of partial differential equations to represent the change of each component with height of the column and with time. It has been validated with data from a pilot capture plant located at the brown coal fired Loy Yang power station in Australia.

Chemical characterization of MEA degradation in PCC pilot plants operating in Australia

- Cruickshank, Alicia, Verheyen, Vincent, Adeloju, Samuel, Meuleman, Erik, Chaffee, Alan, Cottrell, Aaron, Feron, Paul

  • Authors: Cruickshank, Alicia , Verheyen, Vincent , Adeloju, Samuel , Meuleman, Erik , Chaffee, Alan , Cottrell, Aaron , Feron, Paul
  • Date: 2013
  • Type: Text , Journal article
  • Relation: Energy Procedia Vol. 37, no. (2013), p. 877-882
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  • Description: An important step towards commercial scale post-combustion CO2 capture from coal-fired power stations is understanding solvent degradation. Laboratory scale trials have identified three main solvent degradation pathways for 30% MEA: oxidative degradation, carbamate polymerization and formation of heat stable salts. This paper probes the semi-volatile organic compounds produced from a single batch of 30% MEA which was used to capture CO2 from a black coal-fired power station (Tarong, Queensland, Australia) for approximately 700 hours, followed by 500 hours at the brown coal-fired power station (Loy Yang, Victoria, Australia). Comparisons are made between the compounds identified in this aged solvent system with MEA degradation reactions described in literature. Most of semi-volatile compounds tentatively identified by GC/MS have previously been reported in laboratory scale degradation trials. Our preliminary results show low levels of degradation products were present in samples after its use in the pilot plant at Tarong (black coal) and consequent 13 months storage, but much higher concentrations were later found in the same solvent during its at use in the pilot plant at Loy Yang Power (brown coal). Further work includes identifying the cause of poor GC/MS repeatability and investigating the relative rates of reactions described in literature. The impact of inorganic anions and dissolved metals on MEA degradation will also be explored.

Biological and chemical treatment technologies for waste amines from CO₂ capture plants

- Ghayur, Adeel, Verheyen, Vincent, Meuleman, Erik

  • 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
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  • 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.

Ambient temperature solubilisation of brown coal in ammonium carbamate ionic liquids

- Qi, Ying, Verheyen, Vincent, Vijayaraghavan, Ranganathan, MacFarlane, Douglas, Chaffee, Alan

  • 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
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  • 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.

Oxidative degradation of amine absorbents in carbon capture systems – A dynamic modelling approach

- Dickinson, Jillian, Percy, Andrew, Puxty, Graeme, Verheyen, Vincent

  • Authors: Dickinson, Jillian , Percy, Andrew , Puxty, Graeme , Verheyen, Vincent
  • Date: 2016
  • Type: Text , Journal article
  • Relation: International Journal of Greenhouse Gas Control Vol. 53, no. (2016), p. 391-400
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  • Description: Fossil fuels are used widely for energy production and are likely to continue to play a major role world wide for many years to come. Much work has been done on the technology for capturing CO2 from gaseous industrial effluent. For large-scale applications like coal or natural gas-fired power plants, using amine solvents to capture post-combustion CO2 is the most mature CO2 capture technology. This technique can be used to retrofit existing plants by treating the flue gas after combustion. This paper details a dynamic mathematical model for the absorber column constructed from first principles. The loss of MEA through oxidative degradation has been quantified here for the first time and this is currently not possible using commercial packages. Reaction rate kinetics have been employed to predict the accumulation of oxidation products which is limited by the incomplete knowledge of the dominant reactions between O2 and MEA. When research has produced more detailed information about the products formed during this oxidation, it can be inserted easily into the model. Validation has been performed using data from the CSIRO PCC pilot plant at AGL Loy Yang. A limited parametric study of the impact of operating conditions on oxidation was performed.

Structural elucidation of humic acids extracted from Pakistani lignite using spectroscopic and thermal degradative techniques

- Nasir, Saqib, Sarfaraz, Tahira, Verheyen, Vincent, Chaffee, Alan

  • 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
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  • 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.

Techno-economic evaluation of amine-reclamation technologies and combined CO2/SO2 capture for Australian coal-fired plants

- Garg, Bharti, Haque, Nawshad, Cousins, Ashleigh, Pearson, Pauline, Verheyen, Vincent, Feron, Paul

  • Authors: Garg, Bharti , Haque, Nawshad , Cousins, Ashleigh , Pearson, Pauline , Verheyen, Vincent , Feron, Paul
  • Date: 2020
  • Type: Text , Journal article
  • Relation: International Journal of Greenhouse Gas Control Vol. 98, no. (2020), p.
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  • Description: CSIRO's patented CS-Cap process aims at reducing the costs of amine-based post-combustion capture by combining SO2 and CO2 capture using one absorbent in a single absorber column. By avoiding the need for a separate flue gas desulfurization unit, the process offers potential savings for power plants requiring CO2 capture. High-level cost estimates based on lab and pilot data are presented for two amine reclamation techniques i.e. thermal reclamation and reactive crystallisation. Only regeneration via reactive crystallisation reduces CS-Cap costs below base case FGD/SCR-PCC. Cost estimations suggest a potential reduction of 38–44% in the total plant cost when using the CS-Cap process compared to base case. However, the amine reclaimer operating cost governs the overall cost of the CS-Cap process and is highly sensitive to sulfur content. A 50% reduction is observed when SO2 levels reduce from 700 to 200 ppm. Comparing levelised cost of electricity and CO2 avoided costs for CS-Cap against our base case, low sulfur brown coal has a slight (5–7%) cost advantage; however, confirmation requires pilot data on amine recovery. © 2020

Quantification of aqueous monoethanolamine concentration by gas chromatography for postcombustion capture of

- Reynolds, Alicia, Verheyen, Vincent, Adeloju, Samuel, Chaffee, Alan, Meuleman, Erik

  • Authors: Reynolds, Alicia , Verheyen, Vincent , Adeloju, Samuel , Chaffee, Alan , Meuleman, Erik
  • Date: 2014
  • Type: Text , Journal article
  • Relation: Industrial and Engineering Chemistry Research Vol. 53, no. 12 (2014), p. 4805-4811
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  • Description: The availability of reliable analytical methods for measuring amine concentrations is necessary for optimum operation of aqueous amine CO 2 separation systems being employed for postcombustion capture (PCC) of CO2. A GC-FID (gas chromatography with flame ionization detection) method is described for the reliable quantification of 30% (w/w) monoethanolamine (MEA) in severely degraded solvent samples. The observation of intermittent splitting of the MEA peak was a major concern with this approach. The use of a wide-bore column led to improved MEA peak resolution and peak shape. The reliability and robustness of the GC-FID method were assessed by analyzing degraded 30% (w/w) MEA solvent samples from CSIRO's pilot plant at AGL's Loy Yang power station in Victoria, Australia. The results were compared with those obtained by titration and total organic carbon (TOC) measurements of the same samples. The MEA concentrations obtained by the GC-FID and titration methods were statistically similar. In contrast, the MEA concentrations calculated from TOC were consistently higher than those obtained by both GC-FID and titration. © 2014 American Chemical Society.

Simulating combined SO2 and CO2 capture from combustion flue gas

- Verheyen, Vincent, Cousins, Ashleigh, Pearson, Pauline, Puxty, Graeme, Jiang, Kaiqi, Garg, Bharti, Zhai, Rongrong, Ott, Petro, Feron, Paul

  • Authors: Verheyen, Vincent , Cousins, Ashleigh , Pearson, Pauline , Puxty, Graeme , Jiang, Kaiqi , Garg, Bharti , Zhai, Rongrong , Ott, Petro , Feron, Paul
  • Date: 2019
  • Type: Text , Journal article
  • Relation: Greenhouse Gases : Science and Technology Vol. 9, no. 6 (2019), p. 1087-1095
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  • Description: The requirement to pre‐treat flue gas prior to the CO2 capture step is an economic challenge when using aqueous amine absorbents for capturing CO2 from coal‐fired power station flue gases. A potentially lower cost alternative is to combine the capture of both CO2 and SO2 from the flue gas into a single process, removing the requirement for the desulfurization pre‐treatment step. The CSIRO's CS‐Cap process uses a single aqueous amine absorbent to capture both of these acid gases from flue gas streams. This paper covers the initial simulation of this process applied to both brown and black coal flue gases. Removal of absorbed SO2 is achieved via reactive crystallization. This is simulated here using a ‘black box’ process, resulting in a K2SO4 product. Different operating conditions have been evaluated that increase the sulfate concentration of the absorbent in the SO2 capture section of the process, which is expected to increase the efficiency of the reactive crystallization step. This paper provides information on the absorption of SO2 into the amine solution, and heat and mass balances for the wider process. This information will be required for further detailed simulation of the reactive crystallization step, and economic evaluation of the CS‐Cap process. © 2019 Society of Chemical Industry and John Wiley & Sons, Ltd.

Use of MEA oxidation intermediates to monitor oxidation conditions during post-combustion capture of CO2

- Reynolds, Alicia, Verheyen, Vincent

  • Authors: Reynolds, Alicia , Verheyen, Vincent
  • Date: 2019
  • Type: Text , Conference paper
  • Relation: 14th Greenhouse Gas Control Technologies Conference (GHGT-14); Melbourne 21-26 ; October 2018 p.
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  • Description: Amine oxidation is a serious concern for post-combustion capture (PCC) of CO2 from fossil-fuel fired power stations. Organic acids are important oxidation products and have been measured in different ratios at different pilot plants. The concentrations of acetate, formate, glycolate and oxalate were measured in samples of degraded monoethanolamine from a variety of PCC pilot plants as well as laboratory-scale degradation experiments. The results suggest that the ratios of monoethanolamine oxidation intermediates (particularly glycolate and oxalate) have potential as process monitoring tools. Ultimately, ratios of these oxidation intermediates could be used to proactively manage and minimise oxidation of amine-based PCC absorbents by indicating the need for oxygen-scavenger addition or alerting operators to imminent increases in oxidative degradation rates.