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1.
Environ Sci Technol ; 57(13): 5391-5403, 2023 04 04.
Article in English | MEDLINE | ID: mdl-36943504

ABSTRACT

Decarbonization of transportation fuels represents one of the most vexing challenges for climate change mitigation. Biofuels derived from corn starch have offered modest life cycle greenhouse gas (GHG) emissions reductions over fossil fuels. Here we show that capture and storage of CO2 emissions from corn ethanol fermentation achieves ∼58% reduction in the GHG intensity (CI) of ethanol at a levelized cost of 52 $/tCO2e abated. The integration of an oxyfuel boiler enables further CO2 capture at modest cost. This system yields a 75% reduction in CI to 15 gCO2e/MJ at a minimum ethanol selling price (MESP) of $2.24/gallon ($0.59/L), a $0.31/gallon ($0.08/L) increase relative to the baseline no intervention case. The levelized cost of carbon abatement is 84 $/tCO2e. Sensitivity analysis reveals that carbon-neutral or even carbon-negative ethanol can be achieved when oxyfuel carbon capture is stacked with low-CI alternatives to grid power and fossil natural gas. Conservatively, fermentation and oxyfuel CCS can reduce the CI of conventional ethanol by a net 44-50 gCO2/MJ. Full implementation of interventions explored in the sensitivity analysis would reduce CI by net 79-85 gCO2/MJ. Integrated oxyfuel and fermentation CCS is shown to be cost-effective under existing U.S. policy, offering near-term abatement opportunities.


Subject(s)
Greenhouse Effect , Greenhouse Gases , Carbon Dioxide , Ethanol , Carbon , Natural Gas
2.
Environ Sci Technol ; 54(11): 6900-6907, 2020 06 02.
Article in English | MEDLINE | ID: mdl-32374592

ABSTRACT

We have developed a new class of sodium carbonate/silicone composite sorbents that selectively capture carbon dioxide (CO2) and can purify biogas to natural gas pipeline-quality biomethane. These nontoxic composites can be three-dimensionally printed or extruded at low costs, can have high specific CO2 sorption rates (in excess of 5 µmol s-1 g-1 bar-1) and high selectivity due to their chemical mechanism, and can be regenerated with low-energy air stripping. Therefore, these composite sorbents combine the high selectivity of liquid sorbents with the high specific sorption rates and low regeneration energies found in many solid sorbents. We characterized these composite sorbents with X-ray computed tomography, scanning electron microscopy (SEM), and X-ray diffraction (XRD). Furthermore, we measured composite sorption capacities of up to 0.62 mol CO2 kg-1 and recorded breakthrough curves in a flow-through, fixed-bed reactor using both simulated biogas and locally sourced industrial biogas. Additional tests of the composite sorbent were carried out with pure CO2 in a sealed pressure drop apparatus. This experimental data was used to validate a numerical model of the setup and to simulate an industrial-scale biogas upgrading process. Finally, we performed a preliminary technoeconomic analysis for this upgrading process and found that this composite sorbent can upgrade biogas at a lower cost (∼$0.97 per GJ) than other currently implemented techniques.


Subject(s)
Biofuels , Carbonates , Carbon Dioxide , Natural Gas
3.
Proc Natl Acad Sci U S A ; 115(19): 4875-4880, 2018 05 08.
Article in English | MEDLINE | ID: mdl-29686063

ABSTRACT

Capture and permanent geologic sequestration of biogenic CO2 emissions may provide critical flexibility in ambitious climate change mitigation. However, most bioenergy with carbon capture and sequestration (BECCS) technologies are technically immature or commercially unavailable. Here, we evaluate low-cost, commercially ready CO2 capture opportunities for existing ethanol biorefineries in the United States. The analysis combines process engineering, spatial optimization, and lifecycle assessment to consider the technical, economic, and institutional feasibility of near-term carbon capture and sequestration (CCS). Our modeling framework evaluates least cost source-sink relationships and aggregation opportunities for pipeline transport, which can cost-effectively transport small CO2 volumes to suitable sequestration sites; 216 existing US biorefineries emit 45 Mt CO2 annually from fermentation, of which 60% could be captured and compressed for pipeline transport for under $25/tCO2 A sequestration credit, analogous to existing CCS tax credits, of $60/tCO2 could incent 30 Mt of sequestration and 6,900 km of pipeline infrastructure across the United States. Similarly, a carbon abatement credit, analogous to existing tradeable CO2 credits, of $90/tCO2 can incent 38 Mt of abatement. Aggregation of CO2 sources enables cost-effective long-distance pipeline transport to distant sequestration sites. Financial incentives under the low-carbon fuel standard in California and recent revisions to existing federal tax credits suggest a substantial near-term opportunity to permanently sequester biogenic CO2 This financial opportunity could catalyze the growth of carbon capture, transport, and sequestration; improve the lifecycle impacts of conventional biofuels; support development of carbon-negative fuels; and help fulfill the mandates of low-carbon fuel policies across the United States.

4.
Environ Sci Technol ; 49(8): 5142-50, 2015 Apr 21.
Article in English | MEDLINE | ID: mdl-25811231

ABSTRACT

Amine scrubbing, a mature post-combustion carbon capture and storage (CCS) technology, could increase ambient concentrations of fine particulate matter (PM2.5) due to its ammonia emissions. To capture 2.0 Gt CO2/year, for example, it could emit 32 Gg NH3/year in the United States given current design targets or 15 times higher (480 Gg NH3/year) at rates typical of current pilot plants. Employing a chemical transport model, we found that the latter emission rate would cause an increase of 2.0 µg PM2.5/m(3) in nonattainment areas during wintertime, which would be troublesome for PM2.5-burdened areas, and much lower increases during other seasons. Wintertime PM2.5 increases in nonattainment areas were fairly linear at a rate of 3.4 µg PM2.5/m(3) per 1 Tg NH3, allowing these results to be applied to other CCS emissions scenarios. The PM2.5 impacts are modestly uncertain (±20%) depending on future emissions of SO2, NOx, and NH3. The public health costs of CCS NH3 emissions were valued at $31-68 per tonne CO2 captured, comparable to the social cost of carbon itself. Because the costs of solvent loss to CCS operators are lower than the social costs of CCS ammonia, there is a regulatory interest to limit ammonia emissions from CCS.


Subject(s)
Ammonia/analysis , Carbon Sequestration , Particulate Matter/analysis , Carbon Dioxide , Environment , Environmental Pollution/analysis , Environmental Pollution/economics , Seasons , Uncertainty , United States
5.
Environ Sci Technol ; 48(11): 6247-55, 2014 Jun 03.
Article in English | MEDLINE | ID: mdl-24824160

ABSTRACT

Carbon capture and sequestration (CCS) is a technology that provides a near-term solution to reduce anthropogenic CO2 emissions to the atmosphere and reduce our impact on the climate system. Assessments of carbon sequestration resources that have been made for North America using existing methodologies likely underestimate uncertainty and variability in the reservoir parameters. This paper describes a geostatistical model developed to estimate the CO2 storage resource in sedimentary formations. The proposed stochastic model accounts for the spatial distribution of reservoir properties and is implemented in a case study of the Oriskany Formation of the Appalachian sedimentary basin. Results indicate that the CO2 storage resource for the Pennsylvania part of the Oriskany Formation has substantial spatial variation due to heterogeneity of formation properties and basin geology leading to significant uncertainty in the storage assessment. The Oriskany Formation sequestration resource estimate in Pennsylvania calculated with the effective efficiency factor, E=5%, ranges from 0.15 to 1.01 gigatonnes (Gt) with a mean value of 0.52 Gt of CO2 (E=5%). The methodology is generalizable to other sedimentary formations in which site-specific trend analyses and statistical models are developed to estimate the CO2 sequestration storage capacity and its uncertainty. More precise CO2 storage resource estimates will provide better recommendations for government and industry leaders and inform their decisions on which greenhouse gas mitigation measures are best fit for their regions.


Subject(s)
Carbon Dioxide/chemistry , Carbon Sequestration , Geologic Sediments/chemistry , Models, Theoretical , Carbon Dioxide/analysis , Ecology , Pennsylvania , Stochastic Processes
6.
Environ Sci Technol ; 44(8): 2897-903, 2010 Apr 15.
Article in English | MEDLINE | ID: mdl-20337473

ABSTRACT

Geologic sequestration (GS) of carbon dioxide (CO2) is contingent upon securing the legal right to use deep subsurface pore space. Under the assumption that compensation might be required to use pore space for GS, we examine the cost of acquiring the rights to sequester 160-million metric tons of CO2 (the 30-year emissions output for an 800 megawatt power plant operating with a 60% capacity factor and at 90% capture efficiency) using a probabilistic model to simulate the temporal-spatial distribution of subsurface CO2 plumes in several brine-filled sandstones in Pennsylvania and Ohio. For comparison, the Frio Sandstone in the Texas Gulf Coast and the Mt. Simon Sandstone in Illinois were also analyzed. The predicted median values of CO2 plume footprints range from 4500 km(2) to 11,000 km(2) for the Ohio and Pennsylvania sandstones compared to 320 km(2) and 300 km(2) for the thicker Frio and Mt. Simon Sandstones, respectively. We use these footprints to bound the cost to use pore space in Pennsylvania and Ohio and, alternatively, the cost of piping CO2 from Pennsylvania and Ohio to the Mt. Simon or Frio Sandstones for sequestration. The results suggest that pore space acquisition costs could be significant and that using thin local formations for sequestration may be more expensive than piping CO2 to thicker formations at distant sites.


Subject(s)
Carbon Dioxide/chemistry , Compensation and Redress , Geology , Ownership , Models, Theoretical , United States
7.
Environ Sci Technol ; 43(21): 8027-32, 2009 Nov 01.
Article in English | MEDLINE | ID: mdl-19924918

ABSTRACT

Enhanced oil recovery (EOR) has been identified as a method of sequestering CO(2) recovered from power plants. In CO(2)-flood EOR, CO(2) is injected into an oil reservoir to reduce oil viscosity, reduce interfacial tension, and cause oil swelling which improves oil recovery. Previous studies suggest that substantial amounts of CO(2) from power plants could be sequestered in EOR projects, thus reducing the amount of CO(2) emitted into the atmosphere. This claim, however, ignores the fact that oil, a carbon rich fuel, is produced and 93% of the carbon in petroleum is refined into combustible products ultimately emitted into the atmosphere. In this study we analyze the net life cycle CO(2)emissions in an EOR system. This study assesses the overall life cycle emissions associated with sequestration via CO(2)-flood EOR under a number of different scenarios and explores the impact of various methods for allocating CO(2) system emissions and the benefits of sequestration.


Subject(s)
Carbon Dioxide/analysis , Conservation of Energy Resources/methods , Oils/chemistry , Coal , Electricity , Greenhouse Effect , Petroleum , Power Plants
8.
Environ Sci Technol ; 42(8): 2718-22, 2008 Apr 15.
Article in English | MEDLINE | ID: mdl-18497113

ABSTRACT

Governments worldwide should provide incentives for initial large-scale GS projects to help build the knowledge base for a mature, internationally harmonized GS regulatory framework. Health, safety, and environmental risks of these early projects can be managed through modifications of existing regulations in the EU, Australia, Canada, and the U.S. An institutional mechanism, such as the proposed Federal Carbon Sequestration Commission in the U.S., should gather data from these early projects and combine them with factors such as GS industrial organization and climate regime requirements to create an efficient and adaptive regulatory framework suited to large-scale deployment. Mechanisms to structure long-term liability and fund long-term postclosure care must be developed, most likely at the national level, to equitably balance the risks and benefits of this important climate change mitigation technology. We need to do this right. During the initial field experiences, a single major accident, resulting from inadequate regulatory oversight, anywhere in the world, could seriously endanger the future viability of GS. That, in turn, could make it next to impossible to achieve the needed dramatic global reductions in CO2 emissions over the next several decades. We also need to do it quickly. Emissions are going up, the climate is changing, and impacts are growing. The need for safe and effective CO2 capture with deep GS is urgent.


Subject(s)
Carbon Dioxide , Geology , Greenhouse Effect , Geological Phenomena , Government Regulation , Insurance
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