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Elements; October 2008; v. 4; no. 5; p. 305-310; DOI: 10.2113/gselements.4.5.305
© 2008 Mineralogical Society of America
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Carbon Dioxide Sequestration A Solution to a Global Problem

Eric H. Oelkers1 and David R. Cole2

1 Biogéochimie et Géochimie Expérimentale
LMTG-Université de Toulouse-CNRS-IRD-OMP
14 av. Edouard Belin, 31400 Toulouse, France
E-mail: oelkers{at}lmtg.obs-mip.fr
2 Chemical Science Division, Oak Ridge National Laboratory
Oak Ridge, TN 37831, USA
E-mail: coledr{at}ornl.gov


   ABSTRACT
TOP
 ABSTRACT
CO2 AND GLOBAL CLIMATE...
 THE GLOBAL CARBON CYCLE
 CO2 AND OCEAN ACIDIFICATION
 THE HUMAN IMPACT ON...
 CO2 SEQUESTRATION EFFORTS
 PERSPECTIVES
 REFERENCES
 
Human and industrial development over the past hundred years has led to a huge increase in fossil fuel consumption and CO2 emissions, causing a dramatic increase in atmospheric CO2 concentration. This increased CO2 is believed to be responsible for a significant rise in global temperature over the past several decades. Global-scale climate modeling suggests that the temperature increase will continue, at least over the next few hundred years, leading to glacial melting and rising sea levels. Increased atmospheric CO2 also leads to ocean acidification, which will have drastic consequences for marine ecosystems. In an attempt to solve these problems, many have proposed the large-scale sequestration of CO2 from our atmosphere. This introductory article presents a summary of some of the evidence linking increasing atmospheric CO2 concentration to global warming and ocean acidification and our efforts to stem this rise though CO2 sequestration.

KEYWORDS: global carbon cycle, CO2 sequestration, global warming, ocean acidification


   CO2 AND GLOBAL CLIMATE CHANGE
TOP
 ABSTRACT
 CO2 AND GLOBAL CLIMATE...
THE GLOBAL CARBON CYCLE
 CO2 AND OCEAN ACIDIFICATION
 THE HUMAN IMPACT ON...
 CO2 SEQUESTRATION EFFORTS
 PERSPECTIVES
 REFERENCES
 
Few subjects have been more polarizing over the past decade than global warming. A large body of evidence demonstrates that global temperatures are rising. Eleven of the past 12 years rank among the 12 warmest since the 1850s, when temperature began to be regularly recorded (IPCC 2005). This temperature increase has been linked to more-intense precipitation events, including hurricanes (Groisman et al. 2005), a decrease in ocean thermohaline circulation (where higher-density, cold, saline water drags ocean currents down) (Broecker 1997), and rising sea levels in response to glacial melting (e.g. Manabe and Stouffer 1994; Rignot 1998). Rising sea level can lead to the flooding of vast stretches of the coast. It has been estimated that an increase in sea level of just 4 meters would displace over 300 million people and flood 1.7 x 106 km2 of land (equivalent to the combined land area of France, Spain, Germany, and Italy) (Rowley et al. 2007). A temperature increase can also have significant effects on global ecosystems (Cole and Monger 1994), including plant distribution (McKenney et al. 2007), and has already led to the extinction of numerous species, particularly in polar and mountain-top environments (Parmesan 2006). Other investigations suggest that an increase in global temperature can significantly increase the number and extent of diseases that can infect humans (Patz et al. 1996).


Figure 1
Residents of the Gulf Coast of the USA flood the highways in an attempt to escape the wrath of Hurricane Rita in September, 2005. Loss of life, widespread property damage, and disruption of gasoline supplies are stark reminders of how fragile we are in the face of Nature's fury. Many climatologists suggest that the severity and frequency of hurricanes, the duration of droughts, and flooding due to record precipitation may be related to global warming. Increasing atmospheric greenhouse gases, such as CO2, are thought to be a principal driver of global climate change. PHOTO WIKIMEDIA COMMONS COURTESY SHINODA 28107

Many attribute this recent global warming to human influence on atmospheric composition (e.g. Crowley 2000; Karl and Trenberth 2003). Global circulation models suggest that much of the observed global temperature increase stems from an increase in atmospheric CO2 (Manabe and Stouffer 1994; Johns et al. 2003). These models are apparently confirmed by correlations between historic CO2 concentration and temperature. An example of one such correlation is shown in FIGURE 1. A strong connection exists between temperature and atmospheric CO2 content, as shown by data covering the past 400,000 years from Antarctic ice cores. Perhaps most disconcerting is that there may be a positive feedback between increasing atmospheric CO2 concentration and climate. This positive feedback results from a decreasing ability of the terrestrial biosphere to act as a carbon sink as temperature increases (Cox et al. 2000). As a result of the combined effects of human CO2 emissions and this positive feedback, global climate models predict average temperature increases of 2 to 5°C by 2100 (Johns et al. 2003). Reducing the impact of CO2 emissions on the atmosphere and global climate change is thus considered one of the main challenges of this century (e.g. Gunter et al. 1996; Lackner 2003; Pacala and Socolow 2004; Oelkers and Schott 2005; Broecker 2005; Schrag 2007).


Figure 2
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  		FIGURE 1 Atmospheric CO2 concentration (in ppm per volume) compared with global temperature as derived from Antarctic ice-core data over the past 400,000 years. DATA FROM PETIT ET AL. (1999)

 
The link between increased atmospheric CO2 content and global warming is not without its controversies. Some evidence suggests that increased atmospheric CO2 content in the past followed, rather than led, global warming events. In a high-resolution analysis of Antarctic ice-core data, Stott et al. (2007) observed that the beginning of the rise in CO2 content lagged the increase in global temperature by 700 to 1000 years. The possibility that increased atmospheric CO2 follows global warming is consistent with the retrograde solubility of CO2 in seawater. As temperature increases, the solubility of CO2 in the oceans decreases. Thus, with increasing temperature, CO2 would exolve from the oceans, increasing the proportion of CO2 in the atmosphere. There are indications that global warming and polar-ice melting could provoke a new ice age. Global cooling could be triggered by the decreasing salinity of the oceans as the glaciers melt; decreased ocean salinity could dramatically decrease thermohaline ocean circulation, leading to slowing of the currents that carry warm Gulf of Mexico water north of Britain and Norway, thus cooling the North Atlantic (Rahmstorf and Ganopolski 1999; McManus et al. 2004).


Figure 3
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  		FIGURE 2 Atmospheric CO2 concentration (in ppm) measured at the Mauna Loa observatory over the past 50 years

 
It has also been argued that celestial factors have a significant effect on climate. Marsh and Svensmark (2003) presented evidence suggesting that variations in solar activity have had an important influence on the Earth's climate in the past. Veizer (2005) reviewed models advocating cosmic-ray flux as the principal driver of global temperature variation. Hays et al. (1976) proposed that variations in the Earth's orbit could affect global temperature. Model results of Stott et al. (2003), however, suggest that although solar forcing likely played a large role in controlling global mean temperatures during the first half of the twentieth century, greenhouse gas increases were responsible for most of the warming observed during the last 60 years.


   THE GLOBAL CARBON CYCLE
TOP
 ABSTRACT
 CO2 AND GLOBAL CLIMATE...
 THE GLOBAL CARBON CYCLE
CO2 AND OCEAN ACIDIFICATION
 THE HUMAN IMPACT ON...
 CO2 SEQUESTRATION EFFORTS
 PERSPECTIVES
 REFERENCES
 
Carbon dioxide is a trace gas in the Earth's atmosphere. Its current overall concentration is ~385 parts per million (ppm) by volume or 582 ppm by mass. Pre-industrial levels are estimated at ~280 ppm by volume. The variation in CO2 concentration measured at the Mauna Loa, Hawai'i, observatory is shown in FIGURE 2. This concentration has increased from roughly 325 ppm in 1970 to 380 ppm at the beginning of this century. The smaller seasonal variation stems from biological activity: CO2 is consumed by biota during the summer and released in the winter. In urban areas, CO2 is generally higher, and indoors it can reach 10 times the background outdoor concentration. The mass of the Earth's atmosphere is 5.14 x 1018 kg (Trenberth et al. 1988), so the total mass of carbon dioxide can be estimated to be ~3.0 x 1015 kg, which is 3000 gigatons (Gt) of CO2 or 800 Gt of carbon (1 Gt = 109 metric tons).

The atmosphere, however, is one of the smallest global CO2 reservoirs. The world's oceans contain ~39,000 Gt of carbon, while soils, vegetation and detritus contain ~2000 Gt C and carbonate rocks (limestone, marble, chalk) ~65,000,000 Gt C. So, in total, the atmosphere only contains roughly 0.001% of the carbon present in the atmosphere-ocean-upper crust system. Moreover, the mass of carbon in the lower crust and mantle far exceeds that found in these near-surface reservoirs (Holland 1978). There are huge exchanges among these reservoirs (FIG. 3). Each year, the atmosphere exchanges an estimated 90 Gt C with the surface ocean and 110 Gt C with vegetation (Houghton 2007). These numbers imply that the residence time of CO2 in the atmosphere is no more than ~4 years. CO2 exchange currently sequesters roughly half the annual anthropogenic global CO2 emissions into the oceans and soils. This large-scale natural sequestration provides confidence that it may be feasible to remove CO2 from the atmosphere and sequester it in other reservoirs in quantities sufficient to moderate the effects of anthropogenic CO2 emission (Lal 2008).


Figure 4
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  		FIGURE 3 Schematic diagram of part of the global carbon cycle. Fluxes (arrows) are reported in units of gigatons of carbon per year (Gt C/year), whereas masses of the various reservoirs are presented in Gt C.

 

   CO2 AND OCEAN ACIDIFICATION
TOP
 ABSTRACT
 CO2 AND GLOBAL CLIMATE...
 THE GLOBAL CARBON CYCLE
 CO2 AND OCEAN ACIDIFICATION
THE HUMAN IMPACT ON...
 CO2 SEQUESTRATION EFFORTS
 PERSPECTIVES
 REFERENCES
 
CO2 exchange between the atmosphere and the ocean is so rapid that the increase in the atmospheric concentration of CO2 has already had substantial effects on marine chemistry (Caldeira and Wickett 2003). The pH of the ocean's surface water has already decreased by 0.1 units compared to pre-industrial values (Haugan and Drange 1996). Model calculations indicate that continued anthropogenic CO2 emissions could lead to a pH decrease in the oceans by as much as 0.3 to 0.4 units by the end of this century (Orr et al. 2005). This pH decrease would destabilize calcite and aragonite, the minerals that form the shells of many marine organisms (Andersson et al. 2006). As a consequence, it has been suggested that calcifying organisms, including corals, coralline algae, molluscs and foraminifera, would have difficulties building their skeletons. This could have drastic implications for marine ecosystems, including disaster for some planktonic species, which would affect the entire food chain, and vast expanses of coral reefs (Andersson et al. 2006).


Figure 5
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  		FIGURE 4 Annual global human CO2 emissions to the atmosphere since 1751. AFTER MARLAND ET AL. (2007)

 

   THE HUMAN IMPACT ON THE GLOBAL CARBON CYCLE
TOP
 ABSTRACT
 CO2 AND GLOBAL CLIMATE...
 THE GLOBAL CARBON CYCLE
 CO2 AND OCEAN ACIDIFICATION
 THE HUMAN IMPACT ON...
CO2 SEQUESTRATION EFFORTS
 PERSPECTIVES
 REFERENCES
 
Many people are not aware of just how much CO2 each of us produces. Many car drivers fill their gas tank at least twice a month. Each fill-up uses about 50 litres of gasoline. The density of gasoline is roughly 730 grams per litre, so the mass of each fill-up is about 36.5 kilograms. Gasoline is a mixture of hydrocarbons, including alkanes (straight chain molecules) such as heptane (C7H16) and aromatic (ring) compounds such as benzene (C6H6); gasoline can be represented by the general formula CH2. When burned, it produces energy by the reaction:

Formula

The molecular weight of CH2 is 14 g/mole, and that of CO2 is 44 g/mole, so ~3.1 kg CO2 is produced for every kilogram of gasoline burned. It follows that each 50 litre tank of gasoline produces about 113 kg CO2, which, for 24 annual fill-ups, translates to roughly 2.7 metric tons of CO2 per year! If this CO2 were stored mineralogically by creation of calcite (CaCO3), in accord with the reaction:

Formula
the mass of waste increases even more; the molecular weight of calcite is 100, so each kilogram of CO2 would create 2.3 kg of calcite. To fix the CO2 produced annually by this car in mineral form, where it would be geologically stable, one would need to produce 6.2 metric tons of calcite, a volume of 2.3 m3.

By this simple example, it is easy to imagine how the world's 6.6 billion people can contribute so much CO2 annually to the Earth's atmosphere. Manufacturing, transport of goods, and production of cement all add to the total. Human industrial CO2 emissions, primarily from the use of coal, oil and natural gas, and from the production of cement, currently contribute about 8 Gt C (29 Gt CO2) per year. The evolution of global CO2 emissions over the past 250 years is shown in FIGURE 4. Total human addition to the atmosphere since 1751 is estimated to be 315 Gt C (Marland et al. 2007). Of the current CO2 emissions, 18% originate from burning natural gas, 42% from oil, 36% from coal, and 4% from making cement. In addition, the human population produces an estimated 0.6 gigatons of CO2 per year just by exhaling.

Biofuels have been proposed as a solution, because the CO2 produced by burning came originally from the atmosphere and was fixed by plants via photosynthesis. However, the production and burning of biofuels (1) requires substantial energy for farming, transport and processing, thus producing substantial CO2; (2) requires the use of land, water and fertilizer that could otherwise be used to produce food; and (3) generates aldehydes and other compounds that are dangerous to humans, animals and the Earth's ozone layer.

The global average per capita CO2 emissions over the past 50 years are presented in FIGURE 5. Emissions roughly doubled over two decades, from 0.65 tons in 1950 to 1.2 tons in 1970, and have remained relatively stable since. Per capita emissions vary greatly from country to country. The top 10 emitters for 2004, on a per capita basis, are listed in TABLE 1. Oil-producing countries dominate. The United States and Canada are high on the list, with an average of >5 t C per person per year. Most European countries emit between 1.5 and 3 t C per person per year while less-industrialized Asian and African countries average <0.03 t C per person per year. The top overall CO2 emitters are listed in TABLE 2. Industrialized countries currently lead, and those in a phase of active growth, such as China and India, will increase emissions dramatically as their economies grow.


Figure 6
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  		FIGURE 5 Annual global per capita CO2 emissions to the atmosphere since 1950. After Marland et al. (2007)

 

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  		TABLE 1 TOP 10 CO2-EMITTING COUNTRIES IN 2004 ON A PER CAPITA BASIS (MARLAND ET AL. 2007)

 

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  		TABLE 2 TOP 20 CO2-EMITTING COUNTRIES IN 2004 (MARLAND ET AL. 2007)

 


   CO2 SEQUESTRATION EFFORTS
TOP
 ABSTRACT
 CO2 AND GLOBAL CLIMATE...
 THE GLOBAL CARBON CYCLE
 CO2 AND OCEAN ACIDIFICATION
 THE HUMAN IMPACT ON...
 CO2 SEQUESTRATION EFFORTS
PERSPECTIVES
 REFERENCES
 
CO2 storage and mineralization or immobilization, whether natural or engineered, depend on a complex set of chemical processes to assure capture, transport and final deposition (IPCC 2005). Capture is complicated by the diverse nature of CO2 sources (Rubin 2008 this issue). Roughly 60% of emissions originate from large stationary facilities such as power plants, cement production and oil or gas refineries. Such emissions are commonly a mixture of gases (CO2, NOx, SOx, where x represents an integer), often requiring some sort of separation prior to CO2 storage (Rubin 2008). In the ideal case, capture results in a concentrated CO2 stream that can readily be collected and transported. The rest of the CO2 originates from moving sources such as motor vehicles and airplanes. Capturing CO2 emissions from these sources may require direct removal of CO2 from the atmosphere.

Three major types of carbon storage have been proposed: geological storage, ocean storage, and mineral carbonation. In this issue, each of them is explored in detail in separate articles (Benson and Cole 2008; Adams and Caldeira 2008; Oelkers et al. 2008). In addition, there may be some potential for increasing the amount of CO2 that is stored as biomass in forests and soils.

Geological Storage
Geological storage relies on the injection of CO2 into porous rock formations (Holloway 2001; Friedmann 2007; Benson and Cole 2008). CO2 storage reservoirs include sedimentary basins, depleted oil reservoirs and non-economic coal beds. An impermeable cap rock is essential because CO2 density is generally less than that of water, so buoyancy tends to drive CO2 upwards, back to the surface. Several industrial-scale geologic CO2 storage programs are already underway, including the Norwegian Sleipner project in the North Sea (Korbøl and Kaddour 1995) and the Weyburn project in Canada (Emberley et al. 2004); at these sites, a million tons or more of CO2 is injected into the subsurface each year. CO2 can also be injected into oil field reservoirs in an attempt to enhance petroleum recovery (known as EOR). Despite the apparently large annual injected volume, these projects, and other similar efforts, currently store less than one-ten-thousandth, 0.01%, of the global annual anthropogenic CO2 production.

Ocean Storage
Ocean storage means the injection of captured CO2 into the ocean, usually at depths greater than 1000 metres, where it would be isolated from the atmosphere (Adams and Caldeira 2008). CO2 would subsequently dissolve into the ocean and become part of the global carbon cycle. This storage method has yet to be attempted at a pilot scale. Ocean storage capacity may be enhanced by the formation of CO2 hydrates or by the creation of liquid CO2 lakes on the ocean floor.

Mineral Carbonation
Mineral carbonation aims to create stable carbonate minerals such as magnesite (MgCO3) and calcite (CaCO3) by reacting CO2 with silicate minerals containing magnesium and calcium (Oelkers et al. 2008). Such minerals are stable over geologic timescales, so sequestration by this method would minimise risk of later leakage back to the atmosphere. Mineral carbonation mimics natural weathering, but an industrial-scale operation may require the mining and grinding of suitable Mg- and Ca-bearing silicate minerals and the disposal of vast quantities of end-product carbonate minerals. On the positive side, the resulting material could be used as a building material, as an additive to concrete or paper, or as a soil amendment to improve texture, pH and fertility of low-productivity soils. This enhances overall carbon sequestration by increasing below- and above-ground biomass and soil organic-matter content.

Biomass and Soil
Partial alternatives to these industrial solutions may be to store CO2 in forests and soils. The biomass of forests is both a sink and a source for atmospheric CO2. Vegetation absorbs carbon through photosynthesis. Although some is emitted again during respiration, there is net CO2 storage. The stored carbon eventually returns to the atmosphere when the biomass decays or is burned. Forests can be managed to increase their stored carbon, thus reducing atmospheric CO2 concentrations. The use of forests for CO2 storage will require (1) that forests be managed to grow continuously and (2) that the carbon harvested from forests not be returned to the atmosphere. Management practices to maintain, restore, and increase carbon storage in forest soil include: the use of fertilizer; increased density of agriculture and decreased slash-and-burn practices; the preservation of wetlands, peatlands, and old-growth forest; and the forestation of degraded and nondegraded sites, marginal agricultural lands, and lands subject to severe erosion (Johnson 1992). One solution for storing carbon fixed by, then harvested from, forests is its addition to soils in the form of biochar, which also has the potential to greatly enhance soil fertility (SEE BOX). The potential for forests to sequester CO2, however, is limited. Nilsson and Schopfhauser (1995) estimated that only 345 million hectares are available worldwide for afforestation (planting trees on land that has been without forest cover for more than 50 years); an afforestation program of this scale would fix only 1.5 Gt C/year, which is less than 20% of the current anthropogenic carbon input to the atmosphere. Moreover, even attaining this limited land area for afforestation is challenging due to pressure to use land for other purposes, in particular agriculture and development.


   PERSPECTIVES
TOP
 ABSTRACT
 CO2 AND GLOBAL CLIMATE...
 THE GLOBAL CARBON CYCLE
 CO2 AND OCEAN ACIDIFICATION
 THE HUMAN IMPACT ON...
 CO2 SEQUESTRATION EFFORTS
 PERSPECTIVES
REFERENCES
 
The public desire to address global warming, thus to sequester large quantities of CO2 to stem the increase in atmospheric CO2 content, poses many challenges and opportunities for the geological community. Our geochemistry, mineralogy and petrology community has unique expertise that is essential for designing successful, long-term strategies for storing CO2. This expertise is essential for selecting suitable carbon-storage sites, designing the injection facilities, developing monitoring techniques, predicting the fate of CO2 once injected into the subsurface, and assessing the reactivity of the host material with the CO2 introduced, under a spectrum of diverse environments. This Elements issue is an attempt to further motivate our community to address these challenges.


BOX 1 CO2 Sequestration in Soils

Carbon is a major component of soils. Globally the mass of soil organic carbon is more than that of carbon in living matter and in the atmosphere combined (Batjes 1996). Approximately 2 gigatonnes (Gt) of carbon is sequestered in soil organic matter annually (Lal 2003). This amounts to a quarter of the 8 Gt of anthropogenic carbon emitted to the atmosphere per year, making soil a substantial CO2 sink. Carbon is added to soils naturally, by the cycling and burial of organic material from plants, animals and microbes, and agriculturally, by spreading manure. Organic carbon is rapidly released to the atmosphere again, though erosion and oxidation.

A way to increase the residence time of carbon in soils is to add it as biochar, which is charcoal produced by smoldering biomass in an oxygen-poor environment. Some heat is produced, but the low concentration of oxygen prevents burning, thus decreasing the amount of CO2 released and stabilising the remaining carbon against further oxidation by bacteria. Evidence for long-term stability of biochar in soils is found in the carbon-rich Terra Preta de Indio black soils of the Amazon region. Glaser (2007) concluded that at least some of the carbon of the Terra Preta stems from biochar added to these soils over 500 years ago. The charcoal improves soil fertility by adding an adsorptive surface for retention of plant nutrients. The Terra Preta is more than twice as productive as nearby soils in the Amazon, and biochar is sold as a soil amendment. This suggests that, if properly managed, biochar addition to soil could sequester substantial quantities of CO2, in a form that would make it stable over hundreds of years. Lehmann (2007) argued that the addition of biochar to soils could sequester ~10% of the annual US fossil fuel emissions, and Gaunt and Lehmann (2008) proposed that converting biomass to charcoal is more effective than using it as biofuel.

REFERENCES

Batjes NH (1996) Total carbon and nitrogen in the soils of the world. European Journal of Soil Science 47: 151-163

Gaunt JL, Lehmann J (2008) Energy balance and emissions associated with biochar sequestration and pyrolysis bioenergy production. Environmental Science & Technology 42: 4152-4158

Glaser B (2007) Prehistorically modified soils of central Amazonia: a model for sustainable agriculture in the twenty-first century. Philosophical Transactions of the Royal Society B362: 187-196

Lal R (2003) Global potential of soil carbon sequestration to mitigate the greenhouse effect. Critical Reviews in Plant Science 22: 151-184

Lehmann J (2007) A handful of carbon. Nature 447: 143-144

The authors are grateful to Vala K. Ragnarsdottir for telling us about the Terra Preta and for providing the references.

 


   ACKNOWLEDGMENTS
 
This issue owes its existence to the discussions and encouragement from our many friends and colleagues. First and foremost, Susan Stipp and Pierrette Tremblay, who worked tirelessly with us to keep us motivated, cleanse texts and figures, and help pull this issue together. We also thank S. Callahan, J. Schott, S. Gislason, P. Bénézeth and O. Pokrovsky for moral and scientific support during the creation of this issue. EHO's efforts were supported by the Centre National de la Recherche Scientifique, the European Commission Marie Curie Grants `MIR' (MEST-CT-2005-021120) and `MIN-GRO' (MRTN-CT-2006-035488). DRC receives support from the U.S. Department of Energy through projects funded by the Office of Basic Energy Sciences and the Office of Fossil Energy under contract DE-AC05-00OR22725 to Oak Ridge National Laboratory, managed and operated by UT-Battelle, LLC.


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 CO2 AND GLOBAL CLIMATE...
 THE GLOBAL CARBON CYCLE
 CO2 AND OCEAN ACIDIFICATION
 THE HUMAN IMPACT ON...
 CO2 SEQUESTRATION EFFORTS
 PERSPECTIVES
 REFERENCES
 

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