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All sourcesNASA NTRSDOE OSTI
DOE OSTI2018

Final Technical Report

In September 2010, RTI and the DOE/NETL signed a cooperative agreement (DE-FE000489) to design, build, and operate a pre-commercial syngas cleaning system that would capture up to 90% of the CO 2 in the syngas slipstream, and demonstrate the ability to reduce syngas contaminants to meet DOE’s specifications for chemical production application. This pre-commercial syngas cleaning system is operated at Tampa Electric Company’s (TEC) 250-MWe integrated gasification combined cycle (IGCC) plant at Polk Power Station (PPS), located near Tampa, Florida. The syngas cleaning system consists of the following units: Warm Gas Desulfurization Process (WDP) - this unit processes a syngas flow equivalent of 50 MWe of power (50 MWe equivalent corresponds to about 2.0 MM scfh of syngas on dry basis) to produce a desulfurized syngas with a total sulfur (H 2 S+COS) concentration ~ 10 ppmv. Water Gas Shift (WGS) Reactor - this unit converts sufficient CO into CO 2 to enable 90% capture of the CO 2 in the syngas slipstream. This reactor uses conventional commercial shift catalyst technologies. Low Temperature Gas Cooling (LTGC) - this unit cools the syngas for the low temperature activated MDEA process and separates any condensed water. Activated MDEA Process (aMDEA) - this unit employs a non-selective separation for the CO 2 and H 2 S present in the raw syngas stream. Because of the selective sulfur removal by the upstream WDP unit, the CO 2 capture target of 90% CO 2 can be achieved with the added benefit that total sulfur concentration in the CO 2 product is < 100 ppmv. An additional advantage of the activated MDEA process is that the non-selective sulfur removal from the treated syngas reduces sulfur in the treated gas to very low sub-ppmv concentrations, which are required for chemical production applications. Testing to date of this pre-commercial syngas cleaning system has shown that the technology has great potential to provide clean syngas from coal and petcoke-based gasification at increased efficiency and at significantly lower capital and operating costs than conventional syngas cleanup technologies. However, before the technology can be deemed ready for scale-up to a full commercial-scale demonstration, additional R&D testing is needed at the site to address the following critical technical risks: WDP sorbent stability and performance; Impact of WDP on downstream cleanup and conversion steps; Metallurgy and refractory; Syngas cleanup performance and controllability; Carbon capture performance and additional syngas cleanup The proposed plan to acquire this additional R&D data involves: Operation of the units to achieve an additional 3,000 hours of operation of the system within the performance period, with a target of achieving 1,000 hours of those hours via continuous operation of the entire integrated pre-commercial demonstration system; Rapid turnaround of repairs and/or modifications required as necessary to return any specific unit to operating status with documentation and lessons learned to support technology maturation, and; Proactive performance of maintenance activities during any unplanned outages and if possible while operating.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Selective sulfur removal from semi-dry flue gas desulfurization coal fly ash for concrete and carbon dioxide capture applications

High-sulfur mixed fly ash residues from semi-dry flue gas desulfurization units in coal-fired power plants are unsuitable for use as supplementary cementitious material (SCM) for concrete production or carbon dioxide utilization. In this work, we explore the potential for upcycling a representative spray dry absorber ash (10.44 wt% SO 3 ) into concrete-SCM by selective sulfur removal via weak acid dissolution while simultaneously exploring the possibility for CO 2 capture. Towards this effort, parametric studies varying liquid-to-solid ratio, acidity, and CO 2 pressure were conducted in a batch reactor to establish the sulfur removal characteristics in de-ionized water, nitric acid, and carbonic acid, respectively. The dissolution studies show that the leaching of sulfur from calcium sulfite hemihydrate, which is the predominant S phase, is rapid and achieves a concentration plateau within 5 min, and subsequently, appears to be controlled by the primary mineral solubility. Here, preferential S removal was sufficient to meet SCM standards (e.g., 5.0 wt% as per ASTM C618) using all three washing solutions with 0.62–0.72 selectivity (S^), defined as the molar ratio of S to Ca in the leachate, for a raw fly ash with bulk S^ = 0.3. Acid dissolution with 1.43 meq/g of ash or under 5 atm CO 2 retained > 18 wt% CaO and other Si-, Al-rich phases in the fly ash. Based on the experimental findings, two sulfur removal schemes were suggested for either integration with CO 2 capture and utilization processes using flue gas or to produce fly ash for use as a SCM.

01 COAL, LIGNITE, AND PEAT↗
DOE OSTI2011

Mountaineer Commerical Scale Carbon Capture and Storage (CCS) Project

The Final Technical documents all work performed during the award period on the Mountaineer Commercial Scale Carbon Capture & Storage project. This report presents the findings and conclusions produced as a consequence of this work. As identified in the Cooperative Agreement DE-FE0002673, AEP's objective of the Mountaineer Commercial Scale Carbon Capture and Storage (MT CCS II) project is to design, build and operate a commercial scale carbon capture and storage (CCS) system capable of treating a nominal 235 MWe slip stream of flue gas from the outlet duct of the Flue Gas Desulfurization (FGD) system at AEP's Mountaineer Power Plant (Mountaineer Plant), a 1300 MWe coal-fired generating station in New Haven, WV. The CCS system is designed to capture 90% of the CO{sub 2} from the incoming flue gas using the Alstom Chilled Ammonia Process (CAP) and compress, transport, inject and store 1.5 million tonnes per year of the captured CO{sub 2} in deep saline reservoirs. Specific Project Objectives include: (1) Achieve a minimum of 90% carbon capture efficiency during steady-state operations; (2) Demonstrate progress toward capture and storage at less than a 35% increase in cost of electricity (COE); (3) Store CO{sub 2} at a rate of 1.5 million tonnes per year in deep saline reservoirs; and (4) Demonstrate commercial technology readiness of the integrated CO{sub 2} capture and storage system.

29 ENERGY PLANNING, POLICY, AND ECONOMY↗
DOE OSTI2025

A comparative TEA of a two-step process using chemical solvents for producing an ultra-sweet natural gas

Here, a comprehensive Techno-Economic Analysis (TEA) was performed to evaluate the economic feasibility of a novel two-step process (TSP) developed in Aspen Plus V12.1 to desulfurize and decarbonize a raw natural gas containing (2 mol% H 2 S and 5 mol% CO 2 ) into an ultra-sweet natural gas containing (1.72 ppmv H 2 S and 4.19 ppmv CO 2 ). The raw natural gas flow rate used in the TSP was 117.74 kg/s at 60 °C and 50 bar. The TSP combines an H 2 S desulfurization step using potassium carbonate (K 2 CO 3 ) and a CO 2 capture step using 3 different chemical solvents, monoethanolamine (MEA), sodium glycinate (SGS), and potassium glycinate (PGS). Both steps employ fixed-bed absorbers packed with Mellapak 250Y structured packing. The hydraulics and mass transfer characteristics for the TSP were calculated, indicating normal operation with higher gas-side (k G ) than liquid-side (k L ) mass transfer coefficients. The TEA of TSP indicated that PGS had the most promising economic feasibility among the 3 solvents as it exhibited the lowest Levelized Cost of CO 2 capture (LCOC) of $\$$47.54/ton.CO 2 at a Capital Expenditure (CAPEX) of $\$$24.98 million, and an Operating Expenditure (OPEX) of $\$$12.20 million/year. Also, the TSP could produce one MMSCF of ultra-sweet natural gas at a total cost of $\$$339.55.

03 NATURAL GAS↗
DOE OSTI2015

A Review of Major Non-Power-Related Carbon Dioxide Stream Compositions

A critical component in the assessment of long-term risk from geologic sequestration of carbon dioxide (CO2) is the ability to predict mineralogical and geochemical changes within storage reservoirs as a result of rock-brine-CO2 reactions. Impurities and/or other constituents in CO2 source streams selected for sequestration can affect both the chemical and physical (e.g., density, viscosity, interfacial tension) properties of CO2 in the deep subsurface. The nature and concentrations of these impurities are a function of both the industrial source(s) of CO2, as well as the carbon capture technology used to extract the CO2 and produce a concentrated stream for subsurface injection and geologic sequestration. This article reviews the relative concentrations of CO2 and other constituents in exhaust gases from major non-energy-related industrial sources of CO2. Assuming that carbon capture technology would remove most of the incondensable gases N2, O2, and Ar, leaving SO2 and NOx as the main impurities, the authors then summarize the relative proportions of the remaining impurities assumed to be present in CO2 source streams that could be targeted for geologic sequestration. The summary is presented relative to five potential sources of CO2: 1) Flue Gas with Flue Gas Desulfurization, 2) Combustion Stack from Coke Production, 3) Portland Cement Kilns, 4) Natural Gas Combustion, and 5) Lime Production.

Carbon dioxide, CO2 source streams, CO2 impurities↗
DOE OSTI2021

Subtask 2.6 – Optimization of Aerosol Mitigation Technology for Postcombustion CO 2 Capture

Growing concerns over the impact of CO 2 emissions from combustion sources on global climate change have prompted numerous research and development projects aimed at developing cost-effective technologies for CO 2 capture. One family of technologies being demonstrated at pilot and full scale globally is postcombustion CO 2 capture (PCCC) systems that employ amine-based solvents. The captured CO 2 can be compressed and permanently stored underground or used for enhanced oil recovery (EOR). The proximity of North Dakota’s lignite-fired fleet of power plants to potential CO 2 storage options creates a unique atmosphere for PCCC within the state. However, the aerosols present in lignite flue gas present a challenge for large-scale PCCC at North Dakota power plants. Aerosols can negatively impact the long-term performance of amine-based solvents for CO 2 capture. Amine-based solvents are volatile, and aerosols provide nucleation sites where amine vapors can condense. Because aerosols cannot be easily captured at the column outlet using conventional technologies, the amine-laden aerosols escape the system and lead to accelerated solvent losses. Moreover, aerosol components can chemically react with amines to form degradation products that can permanently deactivate the amine, cause fouling, and lead to hazardous emissions. Many of the elements that have been shown to catalyze solvent degradation are present in lignite coals and can exacerbate solvent replacement economics. Understanding this issue is critical to the implementation of solvent-based CO 2 capture systems as applied to lignite-fired generation systems. The Energy & Environmental Research Center (EERC) designed and carried out this project to optimize aerosol mitigation technology for PCCC at a lignite-fired power plant. To meet the goal of this project, the following objectives were identified: Determine the effectiveness of a wet electrostatic precipitator (WESP) on collection of aerosols at a low-rank coal-fired power station. Determine the impact of aerosols on the efficiency and degradation products of amine-based carbon capture systems fired with low-rank fuels. Work was conducted at Minnkota Power Cooperative’s (MPC’s) Milton R. Young (MRY) Station Unit 2 using a slipstream of flue gas from the outlet of the plant’s flue gas desulfurization (FGD) unit. To gather initial data for sizing and specifying a WESP for this system, a temporary pilot-scale WESP was rented and installed on-site. Several different conditions were tested to examine the impact of flow rate, voltage, and current on WESP performance. The WESP was effective at removing large particulate (>200 nm) but caused an increase in fine particulate (<75 nm). Fine particulate material at the inlet and outlet of the WESP was collected, analyzed, and showed that crystalline sulfates carried over from the plant’s FGD unit were being converted to fine aerosols and SO 2 was being converted to SO 3 through the WESP. Additionally, the high moisture content of the flue gas stream at this sample location also contributed to an overall increase in aerosol mass under some of the test conditions. Using the results from the rented WESP, the project team installed a smaller-scale WESP upstream of the EERC’s slipstream CO 2 capture system. Flue gas was routed through a pilot-scale FGD unit to remove SO 2 to very low levels (~1 ppm) and then through a direct contact cooler (DCC) to further cool the gas and to remove moisture. The gas exiting the DCC was then routed through the new WESP before passing to the CO 2 absorber columns. Fluor’s amine-based solvent was used to scrub CO 2 from the slipstream through a set of two absorber columns. The rich solvent was regenerated in a stripper column by heating to drive off captured CO 2 . The system operated using a catch-and-release method where the CO 2 was separated to provide data on the process, but the captured CO 2 was released back into the host site stack. Aerosols and sulfur species were measured at multiple locations throughout the pilot-scale system. The inlet FGD and DCC removed much of the particulate matter and gaseous sulfur upstream of the WESP. With this configuration, the WESP achieved >95% particulate capture. The new WESP did not show any of the increases in SO 3 or other aerosol species that had been consistently observed with the larger-scale WESP installed immediately downstream of the plant’s full-scale FGD unit. Particulate samples captured and analyzed from the WESP inlet did not show any presence of crystalline sulfate materials, indicating that the pilot-scale FGD and DCC were efficient at reducing carryover from the plant’s full-scale FGD unit. A set of parametric tests were conducted on the new WESP to assess the impacts of flow rate, voltage, number of online WESP fields, and gas-phase sulfur content on aerosol and sulfur transformations. The results showed that the WESP performed similarly well at all sets of conditions. Sulfur and particulate matter exiting the WESP were further reduced through the absorber column as the amine-based solvent captured some of the residual contaminants. Solvent analysis showed that these species were slowly concentrating in the solvent over the duration of the test. When the WESP was taken offline and the sulfur slip through the FGD allowed to rise, the sulfate content in the solvent rose sharply, showing that the extra FGD and WESP were effective at reducing sulfate and cation uptake. This would be expected to extend amine-based solvent life by slowing the formation of heat-stable salts and other degradation products. This subtask was cofunded through the EERC–U.S. Department of Energy Joint Program on Research and Development for Fossil Energy-Related Resources Cooperative Agreement No. DE-FE0024233. Nonfederal funding was provided by the North Dakota Industrial Commission and MPC.

01 COAL, LIGNITE, AND PEAT↗
DOE OSTI2013

Effects of O{sub 2} and SO{sub 2} on the Capture Capacity of a Primary-Amine Based Polymeric CO{sub 2} Sorbent

Post combustion CO{sub 2} capture is most commonly carried out using an amine solution that results in a high parasitic energy cost in the stripper unit due to the need to heat the water which comprises a majority of the amine solution. It is also well known that amine solvents suffer from stability issues due to amine leaching and poisoning by flue gas impurities. Solid sorbents provide an alternative to solvent systems that would potentially reduce the energy penalty of carbon capture. However, the cost of using a particular sorbent is greatly affected by the usable lifetime of the sorbent. This work investigated the stability of a primary amine-functionalized ion exchange resin in the presence of O{sub 2} and SO{sub 2}, both of which are constituents of flue gas that have been shown to cause degradation of various amines in solvent processes. The CO{sub 2} capture capacity was measured over multiple capture cycles under continuous exposure to two simulated flue gas streams, one containing 12 vol% CO{sub 2}, 4% O{sub 2}, 84% N{sub 2}, and the other containing 12.5 vol% CO{sub 2}, 4% O{sub 2}, 431 ppm SO{sub 2}, balance N{sub 2} using a custom-built packed bed reactor. The resin maintained its CO{sub 2} capture capacity of 1.31 mol/kg over 17 capture cycles in the presence of O{sub 2} without SO{sub 2}. However, the CO{sub 2} capture capacity of the resin decreased rapidly under exposure to SO{sub 2} by an amount of 1.3 mol/kg over 9 capture cycles. Elemental analysis revealed the resin adsorbed 1.0 mol/kg of SO{sub 2}. Thermal regeneration was determined to not be possible. The poisoned resin was, however, partially regenerated with exposure to 1.5M NaOH for 3 days resulting in a 43% removal of sulfur, determined through elemental analysis, and a 35% recovery of CO{sub 2} capture capacity. Evidence was also found for amine loss upon prolonged (7 days) continuous exposure to high temperatures (120 C) in air. It is concluded that desulfurization of the flue gas stream prior to CO{sub 2} capture will greatly improve the economic viability of using this solid sorbent in a post-combustion CO{sub 2} capture process.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2017

Hybrid Encapsulated Ionic Liquids for Post-Combustion Carbon Dioxide (CO 2 ) Capture

Ionic liquids (ILs) and Phase Change Ionic Liquids (PCILs) are excellent materials for selective removal of carbon dioxide from dilute post-combustion streams. However, they are typically characterized as having high viscosities, which impairs their effectiveness due to mass transfer limitations, caused by the high viscosities. In this project, we are examining the benefits of encapsulating ILs and PCILs in thin polymeric shells to produce particles of approximately 100 to 600 µm in diameter that can be used in a fluidized bed absorber. The particles are produced by microencapsulation of the ILs and PCILs in CO 2 -permeable polymer shells. Here we report on the encapsulation of the IL and PCIL materials, thermodynamic testing of the encapsulated materials, mass transfer measurements in both a fluidized bed and a packed bed, determination of the effect of impurities (SO 2 , NO x and water) on the free and encapsulated IL and PCIL, recyclability of the CO 2 uptake, selection and synthesis of kg quantities of the IL and PCIL, identification of scale-up methods for encapsulation and production of a kg quantity of the PCIL, construction and shakedown of the laboratory scale unit to test the encapsulated particles for CO 2 capture ability and efficiency, use of our mass transfer model to predict mass transfer and identify optimal properties of the encapsulated particles, and initial testing of the encapsulated particles in the laboratory scale unit. We also show our attempts at developing shell materials that are resistant to water permeation. Overall, we have shown that the selected IL and PCIL can be successfully encapsulated in polymer shells and the methods scaled up to production levels. The IL/PCIL and encapsulated IL/PCIL react irreversibly with SO 2 and NO x so the CO 2 capture unit would need to be placed after the flue gas desulfurization and NO x reduction units. However, the reaction with CO 2 in the presence of water is completely reversible. Therefore, it is not necessary to exclude water from the capsules. Mass transfer in the fluidized and packed beds confirm that the fluidized bed arrangement is preferred and that the mass transfer can be predicted accurately by the rate based model that we have developed. Absorption and desorption experiments in the laboratory scale unit show good uptake and recyclability.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Novel Algae Technology for CO2 Utilization

The United States, the world’s largest energy user and second largest CO2 emitter, is heavily dependent on fossil energy. In 2014, U.S. coal burning utilities emitted ~1562 million (MM) tons/year (TPY) of CO2 into the atmosphere, accounting for 76% of the total US power sector emissions1. Hence, reducing the CO2 emission footprint from coal plants is widely viewed as a key element in mitigating global warming. Despite significant interest, implementation of CO2 capture technologies has been constrained by the high capture cost which significantly increases the total cost of electricity. Not only is capturing CO2 with traditional technologies expensive, but generally the CO2 has little value and additional expense must be incurred for sequestration. This project funded by a SBIR grant from the U.S. D.O.E. to Helios-NRG in collaboration with the State University of New York at Buffalo (UB) and Membrane Technology and Research Inc. (MTR) aimed to develop a novel, algae based technology to capture CO2 from the effluent of coal-based power plants and convert it to renewable bio-fuels and higher value co-products such as animal feed and nutraceuticals with the potential to enable a substantial reduction in the net cost of carbon capture. The Phase 2 project was aimed at further demonstrating the technical feasibility of the proposed multi-stage continuous (MSC) flow CO2 capture system and the generation of high-value co-products to offset the CO2 capture cost. The project was completed and the project objectives were met and exceeded. A first-of-a-kind integrated, laboratory scale MSC process unit was fabricated and tested in a greenhouse. The tests were conducted with the preferred algae species identified in Phase I and simulated flue gas containing contaminants at levels typically present in the post flue gas desulfurization (FGD) stream, including ~12% CO2, acid gas (SOX, NOX), and a large number of heavy metals. The tests were successful and demonstrated a 25g/m2/day seasonal average algae productivity and an 80% CO2 capture efficiency. Two new algae species were identified for high-value nutraceutical production. Studies to improve growth rate and nutraceutical content of these algae species were performed and a pathway for further improvements was identified. A new dewatering technology called DeAqua was further advanced. Significant improvement in the performance index was achieved. The anti-fouling membrane was developed and fabricated into a module. The fabricated membrane module was tested with algae slurry and demonstrated improved fouling resistant properties, that can potentially reduce the cost and energy of the critical dewatering step. Test data were used to simulate operation of the overall process. The preliminary economic analysis was updated and modelled based on a 5000-acre algae farm. To the extent possible, the financial and operating assumptions used were the same as those used in the DOE’s 2022 projections for algae technology for CO2 capture and utilization. The results showed the proposed technology’s potential to significantly reduce the cost of CO2 capture compared to current options and that the high value products generated from the CO2 captured can make a step change in the cost of carbon capture. Plans to advance the technology to Phase 2B were developed and potential end-user partners were identified.

Maloney, James↗
DOE OSTI2017

Technoeconomic Optimization of Waste Heat Driven Forward Osmosis for Flue Gas Desulfurization Wastewater Treatment

With the Environmental Protection Agency’s recent Effluent Limitation Guidelines for Steam Electric Generators, power plants are having to install and operate new wastewater technologies. Many plants are evaluating desalination technologies as possible compliance options. However, the desalination technologies under review that can reduce wastewater volume or treat to a zero-liquid discharges standard have a significant energy penalty to the plant. Waste heat, available from the exhaust gas or cooling water from coal-fired power plants, offers an opportunity to drive wastewater treatment using thermal desalination technologies. One such technology is forward osmosis (FO). Forward osmosis utilizes an osmotic pressure gradient to passively pull water from a saline or wastewater stream across a semi-permeable membrane and into a more concentrated draw solution. This diluted draw solution is then fed into a distillation column, where the addition of low temperature waste heat can drive the separation to produce a reconcentrated draw solution and treated water for internal plant reuse. The use of low-temperature waste heat decouples water treatment from electricity production and eliminates the link between reducing water pollution and increasing air emissions from auxiliary electricity generation. In order to evaluate the feasibility of waste heat driven FO, we first build a model of an FO system for flue gas desulfurization (FGD) wastewater treatment at coal-fired power plants. This model includes the FO membrane module, the distillation column for draw solution recovery, and waste heat recovery from the exhaust gas. We then add a costing model to account for capital and operating costs of the forward osmosis system. We use this techno-economic model to optimize waste heat driven FO for the treatment of FGD wastewater. We apply this model to three case studies: the National Energy Technology Laboratory (NETL) 550 MW model coal fired power plant without carbon capture and sequestration, the NETL 550 MW model coal fired power plant with carbon capture and sequestration, and Plant Bowen in Eularhee, Georgia. For each case, we identify the design that minimizes the cost of wastewater treatment given the safely recoverable waste heat. We benchmark the cost minimum waste-heat forward osmosis solutions to two conventional options that rely on electricity, reverse osmosis and mechanical vapor recompression. Furthermore, we quantify the environmental damages from the emissions of carbon dioxide and criteria air pollutants for each treatment option. With this information we can assess the trade-offs between treatment costs, energy consumption, and air emissions between the treatment options.

20 FOSSIL-FUELED POWER PLANTS↗
DOE OSTI2015

Cost and Performance Baseline for Fossil Energy Plants Supplement: Sensitivity to CO 2 Capture Rate in Coal-Fired Power Plants

The cost and performance of various plants designed to meet a range of carbon dioxide (CO 2 ) emissions are evaluated in this report by varying the CO 2 capture rate. The base cases for these designs are the supercritical (SC) pulverized coal (PC) plant from the National Energy Technology Laboratory’s (NETL) report “Cost and Performance Baseline for Fossil Energy Plants, Volume 1a: Bituminous Coal (PC) and Natural Gas to Electricity, Revision 3” and the General Electric Energy (GEE) integrated gasification combined cycle (IGCC) plant in NETL’s report, “Cost and Performance Baseline for Fossil Energy Plants, Volume 1b: Bituminous Coal (IGCC) to Electricity, Revision 2 – Year Dollar Update.” The chosen SC PC plants were based on the Case B12B, differing only in the addition of a bypass flow path that allows for an appropriate portion of the flue gas stream exiting the desulfurization step to be directed towards the stack, which reduces the amount CO 2 captured in the Cansolv process. The chosen IGCC plants were based on the Case B5B, differing by bypassing (either partially or entirely) the water gas shift reactors and thereby reducing the amount of CO 2 captured in the Selexol process. The major components of the underlying CO 2 capture technology in the plants were preserved with minimal modifications to the overall processes. The SC PC cases include up-to-date cost and performance information from recent vendor quotes whereas the IGCC performance and cost are based upon the older quotes used for the Revision 2 report, with standard adjustments made to update the costs to 2011 dollars.

01 COAL, LIGNITE, AND PEAT↗
DOE OSTI2015

High Temperature Syngas Cleanup Technology Scale-up and Demonstration Project

Gasification is a technology for clean energy conversion of diverse feedstocks into a wide variety of useful products such as chemicals, fertilizers, fuels, electric power, and hydrogen. Existing technologies can be employed to clean the syngas from gasification processes to meet the demands of such applications, but they are expensive to build and operate and consume a significant fraction of overall parasitic energy requirements, thus lowering overall process efficiency. RTI International has developed a warm syngas desulfurization process (WDP) utilizing a transport-bed reactor design and a proprietary attrition-resistant, high-capacity solid sorbent with excellent performance replicated at lab, bench, and pilot scales. Results indicated that WDP technology can improve both efficiency and cost of gasification plants. The WDP technology achieved ~99.9% removal of total sulfur (as either H 2 S or COS) from coal-derived syngas at temperatures as high as 600°C and over a wide range of pressures (20-80 bar, pressure independent performance) and sulfur concentrations. Based on the success of these tests, RTI negotiated a cooperative agreement with the U.S. Department of Energy for precommercial testing of this technology at Tampa Electric Company’s Polk Power Station IGCC facility in Tampa, Florida. The project scope also included a sweet water-gas-shift process for hydrogen enrichment and an activated amine process for 90+% total carbon capture. Because the activated amine process provides some additional non-selective sulfur removal, the integration of these processes was expected to reduce overall sulfur in the syngas to sub-ppmv concentrations, suitable for most syngas applications. The overall objective of this project was to mitigate the technical risks associated with the scale up and integration of the WDP and carbon dioxide capture technologies, enabling subsequent commercial-scale demonstration. The warm syngas cleanup pre-commercial test unit was designed and constructed on schedule and under budget and was operated for approximately 1,500 total hours utilizing ~20% of the IGCC’s total syngas as feed (~1.5 MM scfh of dry syngas). The WDP system reduced total sulfur levels to ~10 ppmv (~99.9% removal) from raw syngas that contained as high as 14,000 ppmv of total sulfur. The integration of WDP with the activated amine process enabled further reduction of total sulfur in the final treated syngas to the anticipated sub-ppmv concentrations (>99.99% removal), suitable for stringent syngas applications such as chemicals, fertilizers, and fuels. Techno-economic assessments by RTI and by third parties indicate potential for significant (up to 50%) capital and operating cost reductions for the entire syngas cleanup block when WDP technology is integrated with a broad spectrum of conventional and emerging carbon capture or acid gas removal technologies. This final scientific/technical report covers the pre-FEED, FEED, EPC, commissioning, and operation phases of this project, as well as system performance results. In addition, the report addresses other parallel-funded R&D efforts focused on development and testing of trace contaminant removal process (TCRP) sorbents, a direct sulfur recovery process (DSRP), and a novel sorbent for warm carbon dioxide capture, as well as pre-FEED, FEED, and techno-economic studies to consider the potential benefit for use of WDP for polygeneration of electric power and ammonia/urea fertilizers.

01 COAL, LIGNITE, AND PEAT↗
DOE OSTI2023

Synthetic Calcium Carbonate Production by Carbon Dioxide (CO 2 ) Mineralization of Industrial Waste Brines

The global scale of CO 2 emission has crossed 36 B tons, and the United State represents 14% of the total emissions. In light of the high cost associated with current CO 2 capture processes ($60-to-150 per ton of CO 2 ), carbon capture and utilization (CCU), wherein CO 2 is converted to beneficial products, provides a pragmatic path to overcome the economic barrier for CO 2 emissions control. In particular, CO 2 mineralization offers an attractive route as it produces high-value mineral carbonates that sequester CO 2 in a stable form. For instance, fine precipitated calcium carbonate, a valuable product with unit price in the range of $230-280/t and a global market projected to reach 99 M tons in 2020, can be produced by capturing CO 2 within aqueous Ca 2+ solution. However, two critical challenges need to be overcome—(i) the need for costly processes such as electrolysis or addition of alkali hydroxides to maintain alkalinity during mineralization, and (ii) the geographic availability of Ca-rich solutions (or brines) which often renders efficient integration with power plants impractical. To simultaneously address these challenges, this project developed two novel routes to enable carbonate production based on efficient CO 2 mineralization. In one variation, the project developed a new alkaline carbonation process to capture CO 2 and produce calcite precipitates from coal ashes. Herein, coal ash is carbonated first in a sodium carbonate solution. The carbonation reaction produces sodium hydroxide and raises the solution pH. This high-pH hydroxide solution is then used for CO 2 capture, which converts the sodium hydroxide solution back to sodium carbonate to repeat the carbonation cycle. The carbonated ash residue is refined with a CO 2 pressure swing step to produce high-purity precipitated calcium carbonate. In another variation, Ca-rich produced water brine serves as the Ca-source to mineralize CO 2 . An H + /Na + ion-exchange cycle was designed to provision alkalinity during mineralization and regenerate the ion-exchange reagent in brines with high salinity. Ca-depleted brines can then be treated within a centralized water treatment facility. Both variations beneficially utilize reject streams—such as coal ashes and brines from oil and gas extraction or CO 2 storage operations—that are available at substantial quantities in the vicinity of coal power plants within the U.S. In addition to technology development, this project included techno-economic and life-cycle analysis to identify technically and economically appropriate solutions for power plants in different geographic locations. Taken together, the project provides a unique route to integrate CO 2 emissions control and waste handling/treatment for coal power plants, while producing a high-value product to offset the economic burden associated with waste management. The developed processes utilize post-desulfurization flue gas from coal-fired power plants as is. The CO 2 conversion reactions are performed in alkaline brines at ambient pressure from the flue gas, thereby minimizing the energy burden. By beneficiation of industrial waste streams with low energy input, the processes offers significant technical advantages in energy and CO 2 footprint over the current paradigm of precipitated calcium carbonate production, which involves calcination of limestone at processing temperatures in excess of 800 °C. Overall, this project developed viable CO 2 mineralization processes while strategically maximizing the economic benefit.

01 COAL, LIGNITE, AND PEAT↗
DOE OSTI2021

Topical Report – Findings on Subtask 2.7 – Wet ESP and Aerosol Testing at Coal Creek Station

Growing concerns over the impact of CO 2 emissions from combustion sources on global climate change have prompted numerous research and development projects aimed at developing cost-effective technologies for CO 2 capture. One family of technologies being demonstrated at pilot and full scale globally is postcombustion carbon capture (PCCC) systems that employ amine-based solvents. The captured CO 2 can be compressed and permanently stored underground or used for enhanced oil recovery. The proximity of North Dakota’s lignite-fired fleet of power plants to potential CO 2 storage options creates a unique atmosphere for PCCC within the state. However, the unique components present in lignite flue gas present a challenge for large-scale PCCC at North Dakota power plants by contributing to aerosol formation. Aerosols can negatively impact the long-term performance of amine-based solvents for CO 2 capture. Amine-based solvents are volatile, and flue gas particulate provides nucleation sites where amine vapors can condense as aerosols. Because aerosols cannot be easily captured at the column outlet using conventional technologies, the amine-laden aerosols escape the system and lead to accelerated solvent losses. Moreover, particulate components can chemically react with amines to form degradation products that can permanently deactivate the amine, cause fouling, and lead to hazardous emissions. Many of the elements that have been shown to catalyze solvent degradation are present in lignite coals and can exacerbate solvent replacement economics. Understanding this issue is critical to the implementation of solvent-based CO 2 capture systems as applied to lignite-fired generation systems. The Energy & Environmental Research Center (EERC) designed and carried out this project to fully characterize aerosol behavior with various control technologies installed to better optimize aerosol mitigation technology for CO 2 capture. To meet the goal of this project, the following objectives were identified: Determine the effectiveness of a wet electrostatic precipitator (WESP) on mitigating formation of problematic aerosols at Great River Energy’s Coal Creek Station, upstream of the PCCC system. Determine the effectiveness of the Mitsubishi Heavy Industries (MHI) proprietary amine emission reduction unit (AERU) as a postcapture solvent recovery system for reducing aerosol emissions and extending solvent life downstream of the PCCC system. Determine the impact of aerosols on the efficiency and degradation products of both commercial and advanced solvents within the PCCC system. Work was conducted at Coal Creek Station Unit 1 using a slipstream of flue gas from the outlet of the plant’s flue gas desulfurization (FGD) unit. Flue gas was routed through a pilot-scale FGD unit to remove SO 2 to very low levels (~1 ppm) and then through a direct contact cooler (DCC) to further cool the gas and to remove moisture. The gas exiting the DCC was then optionally routed through a WESP before passing to the CO 2 absorber columns. The MHI solvent was used to scrub CO 2 from the slipstream through a set of two absorber columns. The rich solvent was regenerated in a stripper column by heating to drive off captured CO 2 . Flue gas exiting the absorber column was routed to MHI’s proprietary AERU to recover entrained solvent. The system operated using a catch-and-release method where the CO 2 was separated to provide data on the process, but the captured CO 2 was released back into the host site stack. Particulate was measured, collected, and analyzed from multiple locations throughout the pilot-scale system. Unlike the performance observed in prior work, the inlet FGD and DCC did not remove significant particulate matter from the flue gas. This appears to be due to a difference in the nature of the particulate. The DCC seemed to increase particulate size and count, most likely owing to water condensing onto the surfaces of fly ash particles. When the WESP was operated, it achieved >95% particulate capture. Very little particulate matter or indications of solvent were detected at the AERU outlet. When operating with advanced KS 21 solvent, the particulate material at the AERU outlet was even further decreased. Solvent analysis showed that some species derived from flue gas and ash were slowly concentrating in the solvent over the duration of the test. The levels observed were reported to be within expected ranges and were not of concern to MHI. A high-level techno-economic assessment of installing CO 2 capture at Coal Creek Station suggested that, when using a standard monoethanolamine (MEA)-based solution with simple heat integration, the energy penalty to net generation would be 34%. The bulk of this was due to steam losses for regenerating solvent, followed by parasitic electrical demand for CO 2 compression and then by increased parasitic load for pushing flue gas through the absorber column. These demands could be decreased with a more advanced solvent that exhibits lower heat of regeneration and lower pressure drop than does a simple MEA solution. Further energy could be saved with more thorough heat integration to recover useful energy from the steam used for solvent regeneration. Installing a WESP was predicted to increase the cost of electricity by nearly $5/MWh. This would become cost-effective if solvent losses were roughly 10 times the baseline estimate when not using a WESP but could be returned to baseline by installing the WESP. Piping CO 2 for storage in more favorable geology could help with carbon capture and storage economics. Although storing off-site would necessitate construction of a CO 2 transport pipeline, the cost of this pipeline might be more than offset by reducing the number of wells required, the depths of the wells required, and the electrical demand for the CO 2 compressor. Additional factors that favor off-site storage costs include smaller expected CO 2 plume sizes, which translates to less monitoring and fewer landowner agreements. More detailed assessment of the specific geology in the region under and around Coal Creek Station would be needed to accurately assess the costs and benefits of different storage site options. This subtask was cofunded through the Energy & Environmental Research Center–U.S. Department of Energy Joint Program on Research and Development for Fossil Energy-Related Resources Cooperative Agreement No. DE-FE0024233. Nonfederal funding was provided by the North Dakota Industrial Commission.

Strege, Joshua↗
DOE OSTI2019

Fine Calcium Carbonate Production by CO2 Mineralization of Industrial Waste Brines

Calcium carbonate production via CO2 mineralization offers an attractive route for carbon capture and utilization. The process sequesters CO2 in a stable form of fine precipitated calcium carbonate, a high-value product with unit price in the range of $230-$280/t and a global market projected to reach 99 M tons in 2020. However, two critical barriers hinders CO2 mineralization—(i) the need for costly processes such as electrolysis or addition of alkali hydroxides to maintain alkalinity during mineralization, and (ii) the geographic location mismatch between Ca-rich solutions (or brines) CO2 generation sources (e.g. power plants) which often renders efficient integration of feedstocks impractical. To simultaneously address these challenges, a new process is developed to integrate CO2 mineralization-based carbonate production into the zero liquid discharge water (ZLD) treatment systems at coal-fired power plants. In this process, Ca-rich streams, such as produced water from oil and gas extraction or carbon storage operations, serves as the Ca-source. An H+/Na+ ion-exchange cycle is designed to provision alkalinity during mineralization and regenerate the ion-exchange reagent in solutions with high salinity. Ca-depleted streams are then treated within a centralized ZLD system. The process beneficially utilizes reject streams that are available at substantial quantities in the vicinity of coal power plants within several U.S regions. In addition, the process utilizes post-desulfurization flue gas from coal-fired power plants as is. The CO2 conversion reactions are performed in alkaline streams at ambient pressure, thereby minimizing the energy burden. By beneficiation of industrial waste streams with low energy input, this process offers significant technical advantages in energy and CO2 footprint over the current paradigm of precipitated calcium carbonate production. Overall, the new process provides a unique route to integrate CO2 emissions control and wastewater treatment for coal power plants, while producing high-value product to offset the economic burden associated with waste management.

Simonetti, Dante↗
DOE OSTI2019

Fine Calcium Carbonate Production by CO2 Mineralization of Industrial Waste Brines

Calcium carbonate production via CO2 mineralization offers an attractive route for carbon capture and utilization. The process sequesters CO2 in a stable form of fine precipitated calcium carbonate, a high-value product with unit price in the range of $230-$280/t and a global market projected to reach 99 M tons in 2020. However, two critical barriers hinders CO2 mineralization—(i) the need for costly processes such as electrolysis or addition of alkali hydroxides to maintain alkalinity during mineralization, and (ii) the geographic location mismatch between Ca-rich solutions (or brines) CO2 generation sources (e.g. power plants) which often renders efficient integration of feedstocks impractical. To simultaneously address these challenges, a new process is developed to integrate CO2 mineralization-based carbonate production into the zero liquid discharge water (ZLD) treatment systems at coal-fired power plants. In this process, Ca-rich streams, such as produced water from oil and gas extraction or carbon storage operations, serves as the Ca-source. An H+/Na+ ion-exchange cycle is designed to provision alkalinity during mineralization and regenerate the ion-exchange reagent in solutions with high salinity. Ca-depleted streams are then treated within a centralized ZLD system. The process beneficially utilizes reject streams that are available at substantial quantities in the vicinity of coal power plants within several U.S regions. In addition, the process utilizes post-desulfurization flue gas from coal-fired power plants as is. The CO2 conversion reactions are performed in alkaline streams at ambient pressure, thereby minimizing the energy burden. By beneficiation of industrial waste streams with low energy input, this process offers significant technical advantages in energy and CO2 footprint over the current paradigm of precipitated calcium carbonate production. Overall, the new process provides a unique route to integrate CO2 emissions control and wastewater treatment for coal power plants, while producing high-value product to offset the economic burden associated with waste management.

Simonetti, Dante↗