Solid sorbents for carbon capture

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Solid sorbents for carbon capture include a diverse range of porous, solid-phase materials, including mesoporous silicas, zeolites, and metal-organic frameworks. These have the potential to function as more efficient alternatives to amine gas treating processes for selectively removing CO2 from large, stationary sources including power stations. [1] While the technology readiness level of solid adsorbents for carbon capture varies between the research and demonstration levels, solid adsorbents have been demonstrated to be commercially viable for life-support and cryogenic distillation applications. While solid adsorbents suitable for carbon capture and storage are an active area of research within materials science, significant technological and policy obstacles limit the availability of such technologies.

Contents

Overview

The combustion of fossil fuels generates over 13 gigatons of CO2 per year. [2] Concern over the effects of CO2 with respect to climate change and ocean acidification led governments and industries to investigate the feasibility of technologies that capture the resultant CO2 from entering the carbon cycle. For new power plants, technologies such as pre-combustion and oxy-fuel combustion may simplify the gas separation process.

However, existing power plants require the post-combustion separation of CO2 from the flue gas with a scrubber. In such a system, fossil fuels are combusted with air and CO2 is selectively removed from a gas mixture also containing N2, H2O, O2 and trace sulphur, nitrogen and metal impurities. While exact separation conditions are fuel and technology dependent, in general CO2 is present at low concentrations (4-15% v/v) in gas mixtures near atmospheric pressure and at temperatures of approximately -60 °C. [3] Sorbents for carbon capture are regenerated using temperature, pressure or vacuum, so that CO2 can be collected for sequestration or utilization and the sorbent can be reused.

The most significant impediment to carbon capture is the large amount of electricity required. [4] Without policy or tax incentives, the production of electricity from such plants is not competitive with other energy sources. [5] The largest operating cost for power plants with carbon capture is the reduction in the amount of electricity produced, [6] because energy in the form of steam is diverted from making electricity in the turbines to regenerating the sorbent. Thus, minimizing the amount of energy required for sorbent regeneration is the primary goal behind much carbon capture research.

Metrics

MIL-53 is a metal-organic framework which shows very strong selectivity for adsorbing CO2 into its pores (visualized as yellow spheres) from a mixture of CO2/N2 when mechanical pressure is applied to influence the pore size aperture. MIL-53ht.png
MIL-53 is a metal-organic framework which shows very strong selectivity for adsorbing CO2 into its pores (visualized as yellow spheres) from a mixture of CO2/N2 when mechanical pressure is applied to influence the pore size aperture.

Significant uncertainty exists around the total cost of post-combustion CO2 capture because full-scale demonstrations of the technology have yet to come online. [8] Thus, individual performance metrics are generally relied upon when comparisons are made between different adsorbents. [9]

Regeneration energy—Generally expressed in energy consumed per weight of CO2 captured (e.g. 3,000 kJ/kg). These values, if calculated directly from the latent and sensible heat components of regeneration, measure the total amount of energy required for regeneration. [10]

Parasitic energy—Similar to regeneration energy, but measures how much usable energy is lost. Owing to the imperfect thermal efficiency of power plants, not all of the heat required to regenerate the sorbent would actually have produced electricity. [11]

Adsorption capacity—The amount of CO2 adsorbed onto the material under the relevant adsorption conditions.

Working capacity—The amount of CO2 that can be expected to be captured by a specified amount of adsorbent during one adsorption–desorption cycle. This value is generally more relevant than the total adsorption capacity.

Selectivity—The calculated ability of an adsorbent to preferentially adsorb one gas over another gas. Multiple methods of reporting selectivity have been reported and in general values from one method are not comparable to values from another method. Similarly, values are highly correlated to temperature and pressure. [12]

Comparison to aqueous amine absorbents

Aqueous amine solutions absorb CO2 via the reversible formation of ammonium carbamate, ammonium carbonate and ammonium bicarbonate. [13] The formation of these species and their relative concentration in solution is dependent upon the specific amine or amines as well as the temperature and pressure of the gas mixture. At low temperatures, CO2 is preferentially absorbed by the amines and at high temperatures CO2 is desorbed. While liquid amine solutions have been used industrially to remove acid gases for nearly a century, amine scrubber technology is still under development at the scale required for carbon capture. [14]

Advantages

Multiple advantages of solid sorbents have been reported. Unlike amines, solid sorbents can selectively adsorb CO2 without the formation of chemical bonds (physisorption). The significantly lower heat of adsorption for solids requires less energy for the CO2 to desorb from the material surface. Also, two primary or secondary amine molecules are generally required to absorb a single CO2 molecule in liquids. For solid surfaces, large capacities of CO2 can be adsorbed. For temperature swing adsorption processes, the lower heat capacity of solids has been reported to reduce the sensible energy required for sorbent regeneration. [9] Many environmental concerns over liquid amines can be eliminated by the use of solid adsorbents. [5]

Disadvantages

Manufacturing costs are expected to be significantly greater than the cost of simple amines. Because flue gas contains trace impurities that degrade sorbents, solid sorbents may prove to be prohibitively expensive. Significant engineering challenges must be overcome. Sensible energy required for sorbent regeneration cannot be effectively recovered if solids are used, offsetting their significant heat capacity savings. Additionally, heat transfer through a solid bed is slow and inefficient, making it difficult and expensive to cool the sorbent during adsorption and heat it during desorption. Lastly, many promising solid adsorbents have been measured only under ideal conditions, which ignores the potentially significant effects H2O can have on working capacity and regeneration energy.

Physical adsorbents

Carbon dioxide adsorbs in appreciable quantities onto many porous materials through van der Waals interactions. Compared to N2, CO2 adsorbs more strongly because the molecule is more polarizabable and possesses a larger quadrupole moment. [9] However, stronger adsorptives including H2O often interfere with the physical adsorption mechanism. Thus, discovering porous materials that can selectively bind CO2 under flue gas conditions using only a physical adsorption mechanism is an active research area.

Zeolites

Zeolites, a class of porous aluminosilicate solids, are currently used in a wide variety of industrial and commercial applications including CO2 separation. The capacities and selectivities of many zeolites are among the highest for adsorbents that rely upon physisorption. For example, zeolite Ca-A (5A) has been reported to display both a high capacity and selectivity for CO2 over N2 under conditions relevant for carbon capture from coal flue gas, although it has not been tested in the presence of H2O. [15] Industrially, CO2 and H2O can be co-adsorbed on a zeolite, but high temperatures and a dry gas stream are required to regenerate the sorbent. [11]

Metal-organic frameworks

Metal-organic frameworks (MOFs) are promising adsorbents. [9] Sorbents displaying a diverse set of properties have been reported. MOFs with extremely large surface areas are generally not among the best for CO2 capture [9] compared to materials with at least one adsorption site that can polarize CO2. For example, MOFs with open metal coordination sites function as Lewis acids and strongly polarize CO2. [16] Owing to CO2's greater polarizability and quadrupole moment, CO2 is preferentially adsorbed over many flue gas components such as N2. However, flue gas contaminants such as H2O often interfere. MOFs with specific pore sizes, tuned specifically to preferentially adsorb CO2 have been reported. [17] 2015 studies using dolomite based solid sorbents and the MgO-based or CaO-based sorbent showed high capability and durability at elevated temperatures and pressures. [18]

Chemical adsorbents

Amine impregnated solids

Frequently, porous adsorbents with large surface areas, but only weak adsorption sites, lack sufficient capacity for CO2 under realistic conditions. To increase low pressure CO2 adsorption capacity, adding amine functional groups to highly porous materials has been reported to result in new adsorbents with higher capacities. This strategy has been analyzed for polymers, silicas, activated carbons and metal-organic frameworks. [1] Amine impregnated solids utilize the well-established acid-base chemistry of CO2 with amines, but dilute the amines by containing them within the pores of solids rather than as H2O solutions. Amine impregnated solids are reported to maintain their adsorption capacity and selectivity under humid test conditions better than alternatives. For example, a 2015 study of 15 solid adsorbent candidates for CO2 capture found that under multicomponent equilibrium adsorption conditions simulating humid flue gas, only adsorbents functionalized with alkylamines retained a significant capacity for CO2. [19]

Notable adsorbents

NameType0.15 bar Capacity (% weight)Reference
PEI-MIL-101Amine–MOF17.7 [20]
mmen-Mg2(dobpdc)Amine–MOF13.7 [21] [22]
dmen-Mg2(dobpdc)Amine–MOF13.3 [23]
dmpn–Mg2(dobpdc)Amine–MOF11.0 [24]
mmen-CuBTTriAmine–MOF9.5 [25]
NH2-MIL-53(Al)Amine–MOF3.1 [26]
en-CuBTTriAmine–MOF2.3 [27]
Mg-MOF-74MOF20.6 [16]
Ni-MOF-74MOF16.9 [28]
Co-MOF-74MOF14.2 [28]
HKUST-1MOF11.6 [29]
SIFSIX-3(Zn)MOF10.7 [17]
Zn(ox)(atz)2MOF8.3 [30]
Zn-MOF-74MOF7.6 [31]
CuTATB-60MOF5.8 [32]
bio-MOF-11MOF5.4 [33]
FeBTTMOF5.3 [34]
MOF-253-Cu(BF4)MOF4.0 [35]
ZIF-78MOF3.3 [36]
CuBTTriMOF2.9 [27]
SNU-50MOF2.9 [37]
USO-2-Ni-AMOF2.1 [26]
MIL-53(Al)MOF1.7 [26]
MIL-47MOF1.1 [28]
UMCM-150MOF1.8 [28]
MOF-253MOF1.0 [35]
ZIF-100MOF1.0 [38]
MTV-MOF-EHIMOF1.0 [39]
ZIF-8MOF0.6 [28]
IRMOF-3MOF0.6 [28]
MOF-177MOF0.6 [28]
UMCM-1MOF0.5 [28]
MOF-5MOF0.5 [28]
13XZeolite15.3 [40]
Ca-AZeolite18.5 [15]

Related Research Articles

<span class="mw-page-title-main">Adsorption</span> Phenomenon of surface adhesion

Adsorption is the adhesion of atoms, ions or molecules from a gas, liquid or dissolved solid to a surface. This process creates a film of the adsorbate * on the surface of the adsorbent(solvent). This process differs from absorption, in which a fluid is dissolved by or permeates a liquid or solid. Adsorption is a surface phenomenon and does not penetrate through the surface to the bulk of the adsorbent, while absorption involves the whole volume of the material, although adsorption does often precede absorption. The term sorption encompasses both processes, while desorption is the reverse of it.

<span class="mw-page-title-main">Activated carbon</span> Form of carbon processed to have small, low-volume pores that increase the surface area

Activated carbon, also called activated charcoal, is a form of carbon commonly used to filter contaminants from water and air, among many other uses. It is processed (activated) to have small, low-volume pores that increase the surface area available for adsorption or chemical reactions. Activation is analogous to making popcorn from dried corn kernels: popcorn is light, fluffy, and its kernels have a high surface-area-to-volume ratio. Activated is sometimes replaced by active.

<span class="mw-page-title-main">Heterogeneous catalysis</span> Type of catalysis involving reactants & catalysts in different phases of matter

In chemistry, heterogeneous catalysis is catalysis where the phase of catalysts differs from that of the reactants or products. The process contrasts with homogeneous catalysis where the reactants, products and catalyst exist in the same phase. Phase distinguishes between not only solid, liquid, and gas components, but also immiscible mixtures, or anywhere an interface is present.

<span class="mw-page-title-main">Membrane gas separation</span> Technology for splitting specific gases out of mixtures

Gas mixtures can be effectively separated by synthetic membranes made from polymers such as polyamide or cellulose acetate, or from ceramic materials.

<span class="mw-page-title-main">Molecular sieve</span> Filter material with homogeneously sized pores in the nanometer range

A molecular sieve is a material with pores of uniform size. These pore diameters are similar in size to small molecules, and thus large molecules cannot enter or be adsorbed, while smaller molecules can. As a mixture of molecules migrate through the stationary bed of porous, semi-solid substance referred to as a sieve, the components of highest molecular weight leave the bed first, followed by successively smaller molecules. Some molecular sieves are used in size-exclusion chromatography, a separation technique that sorts molecules based on their size. Other molecular sieves are used as desiccants.

Amine gas treating, also known as amine scrubbing, gas sweetening and acid gas removal, refers to a group of processes that use aqueous solutions of various alkylamines (commonly referred to simply as amines) to remove hydrogen sulfide (H2S) and carbon dioxide (CO2) from gases. It is a common unit process used in refineries, and is also used in petrochemical plants, natural gas processing plants and other industries.

<span class="mw-page-title-main">Activated alumina</span>

Activated alumina is manufactured from aluminium hydroxide by dehydroxylating it in a way that produces a highly porous material; this material can have a surface area significantly over 200 m²/g. The compound is used as a desiccant (to keep things dry by adsorbing water from the air) and as a filter of fluoride, arsenic and selenium in drinking water. It is made of aluminium oxide (alumina; Al2O3). It has a very high surface-area-to-weight ratio, due to the many "tunnel like" pores that it has. Activated alumina in its phase composition can be represented only by metastable forms (gamma-Al2O3 etc.). Corundum (alpha-Al2O3), the only stable form of aluminum oxide, does not have such a chemically active surface and is not used as a sorbent.

<span class="mw-page-title-main">Flue gas</span> Gas exiting to the atmosphere via a flue

Flue gas is the gas exiting to the atmosphere via a flue, which is a pipe or channel for conveying exhaust gases from a fireplace, oven, furnace, boiler or steam generator. Quite often, the flue gas refers to the combustion exhaust gas produced at power plants. Its composition depends on what is being burned, but it will usually consist of mostly nitrogen derived from the combustion of air, carbon dioxide, and water vapor as well as excess oxygen. It further contains a small percentage of a number of pollutants, such as particulate matter, carbon monoxide, nitrogen oxides, and sulfur oxides.

<span class="mw-page-title-main">Pressure swing adsorption</span> Method of gases separation using selective adsorption under pressure

Pressure swing adsorption (PSA) is a technique used to separate some gas species from a mixture of gases under pressure according to the species' molecular characteristics and affinity for an adsorbent material. It operates at near-ambient temperature and significantly differs from the cryogenic distillation commonly used to separate gases. Selective adsorbent materials are used as trapping material, preferentially adsorbing the target gas species at high pressure. The process then swings to low pressure to desorb the adsorbed gas.

<span class="mw-page-title-main">Carbon capture and storage</span> Process of capturing CO2 from industrial emissions and storing it

Carbon capture and storage (CCS) is a process in which a relatively pure stream of carbon dioxide (CO2) from industrial sources is separated, treated and transported to a long-term storage location. For example, the carbon dioxide stream that is to be captured can result from burning fossil fuels or biomass. Usually the CO2 is captured from large point sources, such as a chemical plant or biomass plant, and then stored in an underground geological formation. The aim is to reduce greenhouse gas emissions and thus mitigate climate change.

Douglas Patrick Harrison is a Professor Emeritus of Chemical Engineering from Louisiana State University's Gordon A. and Mary Cain Department of Chemical Engineering, where he taught undergraduate and graduate classes and served as dissertations advisor to Ph.D. and M.S. students. He held the Department Chair position, occupied the Marguerite Voorhies Professor endowed chair, and managed several research projects since his retirement in 2005.

<span class="mw-page-title-main">Metal–organic framework</span> Class of chemical substance

Metal–organic frameworks (MOFs) are a class of compounds consisting of metal ions or clusters coordinated to organic ligands to form one-, two-, or three-dimensional structures. The organic ligands included are sometimes referred to as "struts" or "linkers", one example being 1,4-benzenedicarboxylic acid (BDC).

A carbon dioxide scrubber is a piece of equipment that absorbs carbon dioxide (CO2). It is used to treat exhaust gases from industrial plants or from exhaled air in life support systems such as rebreathers or in spacecraft, submersible craft or airtight chambers. Carbon dioxide scrubbers are also used in controlled atmosphere (CA) storage. They have also been researched for carbon capture and storage as a means of combating climate change.

<span class="mw-page-title-main">Polyethylenimine</span> Chemical compound

Polyethylenimine (PEI) or polyaziridine is a polymer with repeating units composed of the amine group and two carbon aliphatic CH2CH2 spacers. Linear polyethyleneimines contain all secondary amines, in contrast to branched PEIs which contain primary, secondary and tertiary amino groups. Totally branched, dendrimeric forms were also reported. PEI is produced on an industrial scale and finds many applications usually derived from its polycationic character.

The electrochemical regeneration of activated carbon based adsorbents involves the removal of molecules adsorbed onto the surface of the adsorbent with the use of an electric current in an electrochemical cell restoring the carbon's adsorptive capacity. Electrochemical regeneration represents an alternative to thermal regeneration commonly used in waste water treatment applications. Common adsorbents include powdered activated carbon (PAC), granular activated carbon (GAC) and activated carbon fibre.

Calcium looping (CaL), or the regenerative calcium cycle (RCC), is a second-generation carbon capture technology. It is the most developed form of carbonate looping, where a metal (M) is reversibly reacted between its carbonate form (MCO3) and its oxide form (MO) to separate carbon dioxide from other gases coming from either power generation or an industrial plant. In the calcium looping process, the two species are calcium carbonate (CaCO3) and calcium oxide (CaO). The captured carbon dioxide can then be transported to a storage site, used in enhanced oil recovery or used as a chemical feedstock. Calcium oxide is often referred to as the sorbent.

<span class="mw-page-title-main">Hydrogen spillover</span>

In heterogeneous catalysis, hydrogen molecules can be adsorbed and dissociated by the metal catalyst. Hydrogen spillover is the migration of hydrogen atoms from the metal catalyst onto the nonmetal support or adsorbate. Spillover, generally, is the transport of a species adsorbed or formed on a surface onto another surface. Hydrogen spillover can be characterized by three major steps, the first being where molecular hydrogen is split via dissociative chemisorption into its constitutive atoms on a transition metal catalyst surface, followed by migration from the catalyst to the substrate, culminating in their diffusion throughout the substrate surfaces and/or in the bulk materials.

The use of ionic liquids in carbon capture is a potential application of ionic liquids as absorbents for use in carbon capture and sequestration. Ionic liquids, which are salts that exist as liquids near room temperature, are polar, nonvolatile materials that have been considered for many applications. The urgency of climate change has spurred research into their use in energy-related applications such as carbon capture and storage.

Sorption enhanced water gas shift (SEWGS) is a technology that combines a pre-combustion carbon capture process with the water gas shift reaction (WGS) in order to produce a hydrogen rich stream from the syngas fed to the SEWGS reactor.

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