J of Industrial Ecology - 2023 - Simon - Material Flows and Embodied Energy of Direct Air Capture A Cradle To Gate

DOI: 10.1111/jiec.
13357
METHODS ARTICLE
Material flows and embodied energy of direct air capture

A cradle-to-gate inventory of selected technologies
Balint Simon1,2
1
Chair of Operations Management, RWTH
Aachen University, Aachen, Germany Abstract
2
Institute for Energy and Environmental Direct air capture (DAC) is an essential nexus of CO2 chemistry and climate mitiga-
Research (ifeu GmbH), Heidelberg, Germany
tion. Life cycle assessment (LCA) is often used to validate the environmental potential
Correspondence of emerging technologies. Consequently, an increased number of ex ante LCAs is
Balint Simon, RWTH Aachen, Kackertstr. 7, expected in this field. However, a comprehensive description through parameterized
52072 Aachen, Germany.
Email: [email protected] modeling of life cycle inventories of distinct technological pathways, which is essential
for transparency, has recently been missing from the international literature. To fill this
Editor Managing Review: Alexis Laurent
gap, the present study analyzes three selected DAC technologies to create an inven-
Funding information tory. Amine-based adsorption and absorption, as well as alkali-based absorption, were
Ministry of Economics, Innovation,
modeled.
Digitalization, and Energy of the State of North
Rhine-Westphalia for the support through The energy consumption of the operation, cradle-to-gate embodied energy, and sen-
project SCI4climate.NRW, Grant/Award
sitivity analysis based on parameter variations were carried out. The “cradle-to-gate”
Number: EFO-001D; German Federal Ministry
of Education and Research through energy requirement of direct air capture (DAC) often lies in the range or above the
Kopernikus-P2X, Grant/Award Number:
formation energy of CO2 (8.94 GJ energy can be obtained by formation of 1 t CO2
03SFK2WO
from elementary C and O2 ). This indicates that theoretically more energy is required
for capture, as can be obtained during the formation of CO2 . Because energy has con-
tinuously growing economic and ecological value, this energy intensity of DAC implies
that DAC might have important role in CCU to add directly measurable economic value.
The parametrized model includes over 60 parameters, resulting in an array of possible
energy and material requirements. The use of this wide range of figures in life cycle
assessment (LCA) sheds light on real opportunities for DAC in future product systems.
The option of varying parameters enables the tailoring of the calculation to a particular
situation or design. In this way, the calculator offers a common base for LCA, fostering
an early stage analysis of DAC technologies.
KEYWORDS
CO2 adsorption, CO2 alkali absorption, CO2 amine absorption, direct air capture, industrial
ecology, parametrized life cycle inventory
1 IMPORTANCE OF AN EX ANTE ENVIRONMENTAL ASSESSMENT OF DIRECT AIR CAPTURE
Closing the life cycle of carbon is a promising and efficacious method for greenhouse gas (GHG) management (Bringezu, 2014), which is important
to stay below the global warming limit of 1.5◦ C (Tollefson, 2018). In addition, CO2 is a suitable feedstock for future fuels and chemicals (Goeppert
et al., 2014; Olah et al., 2011) even though fossil CO2 -based products pose a threat to emit their carbon content at the end of their “second life.”
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Anthropogenic CO2 originates from a point, and distributed sources exhibit an equal share of global emissions (Blanco et al., 2014). This highlights
the importance of distributed sources in climate mitigation, even if point sources have a higher CO2 concentration than dilute air, which enables
easier emission control (von der Assen et al., 2016).
Despite recent technological issues, DAC is an effective negative emission technology with a net consume of atmospheric CO2 (Daggash et al.,
2018; Lackner et al., 1999; Viebahn et al., 2019). However, this is true only at the “cradle-to-gate” life cycle stage. The overall carbon footprint is
subject to the subsequent use phase of the captured CO2 , whether it remains in the technosphere or is released again. Indeed, in specific cases, the
replacement of fossil energy sources with renewable resources decreases GHG emissions more efficiently than capturing emitted CO2 reported
by Jacobson (2019). However, DAC suits rather for the control of diffuse than fixed point sources of CO2 . On the other hand, deploying DAC for
fuel synthesis or CCS processes might bring climate benefits by using low-carbon energy sources (Daggash et al., 2018; Liu et al., 2020; Sagues
et al., 2019). A further benefit of air, in contrast to the limited carbon sources of biomass, is that it represents the largest climate-friendly carbon
reserve for the chemical and fuel industries (Goeppert et al., 2012; Olah et al., 2011; von der Assen et al., 2016). These attributes of DAC represent a
promising climate management tool, consequently, the number of environmental LCA is rapidly growing in the field of CO2 capture and subsequent
CO2 chemistry (Daggash et al., 2018; Deutz & Bardow, 2021; Deutz et al., 2018; Dieterich et al., 2020; Liu et al., 2020).
Life cycle inventory (LCI) is a vital part of an LCA that describes the physical input–output flows of a technology or production procedure. Accord-
ingly, a reliable and thorough LCA requires the complete understanding and a well-documented and complete LCI of the particular technology.
However, only several studies (from the past 2−3 years), by de Jonge et al. (2019), Deutz and Bardow (2021), and Sabatino et al. (2021), deal with
a comprehensive “cradle-to-gate/grave” analysis of DAC technology, furthermore, Terlouw et al. (2021) and Madhu et al. (2021) provide case spe-
cific data, as well. These studies report LCI with fixed values even though outcome might be significantly affected by changing ambient and work
parameters of capture. Despite the sparse understanding of these effects, a large number of studies have analyzed systems including DACs, such
as power to fuel (Deutz et al., 2018; Liu et al., 2020; Schreiber et al., 2020), power to methanol (Hoppe et al., 2017), systematic analysis of CCU/S
(carbon capture and use/sequestration) (Daggash et al., 2018), and future potential of decarbonization (Thonemann & Pizzol, 2019; Viebahn et al.,
2019).
Recent studies on CO2 utilization rely on reported figures of different available technical and techno-economic analyses of absorption (Baja-
mundi et al., 2019; Krekel et al., 2018) and adsorption of CO2 (Keith et al., 2018; Mazzotti et al., 2013), but none of them reported an LCI of DAC
in easily reproducible details. Hence, the large variety of deployed datasets and the lack of plain understanding of the process itself might lead to
insufficient transparency of recent LCAs. However, several parameters of capture technologies can be obtained using thermodynamic simulations
(e.g., Aspen Plus), which are associated with software-related costs and require the correct selection of the so-called property packages for the
simulation. Thus, future LCAs of DAC require a commonly available and scalable parametrized inventory, enabling more sophisticated sensitivity
and uncertainty analysis of the results. To overcome this issue, three different technologies were modeled in a parametrized LCI calculator based
on the physical and thermodynamic properties of deployed materials and processes. The calculator generates information on material and energy
use under various capture conditions from the “cradle to gate” including the construction of the facility.
Section 2 (methodology) describes the three selected technologies such as (i) the adsorption process with an amine-based active material, (ii)
the amine-based absorption process, and (iii) absorption processes deploying alkali solution. The data sources and modeling parameters are also
included in this section. Section 3 (results) discusses the material flow and embodied energy that originates in capturing 1 ton of atmospheric CO2
by each technology assuming a plant capacity of 1 Mt/a (de Jonge et al., 2019; Deutz & Bardow, 2021; Keith et al., 2018). Embodied energy of
the capture is calculated on a “best-case, worst-case” basis to obtain the theoretical minimum and maximum energy required for CO2 capture
(see Section 3.4). The system boundary of embodied energy comprises all primary energy consumed in life cycle stages from the exploitation of
natural resources to the CO2 capture including “feedstock energy” which is physically embodied into the used fossil-based materials (polymer-
plastics, rubbers, etc.) and production energies (electricity, heat). The wide range of results supports the sophisticated analysis of DAC systems
from an industrial and ecological point of view. This section also deals with the similarities and differences between the available studies in this
field. Section 4 (summary) comprises the main findings and describes the value added for the LCA community.
2 TECHNOLOGICAL OPTIONS OF THE ANALYZED DAC
The Excel® -based tool in Supporting Information S1 provides detailed thermodynamic calculations and a parametrized (cross-linked) Excel® table
to obtain the energy and material consumption.
The calculation is based on freely variable parameters that can be adjusted to a particular situation or design, such as ambient temperature or
pressure, air humidity, capture capacity of the active material, pressure drop, different thermodynamic constants, or the efficiency of mechanical
parts (e.g., fluid pumps) (see Tables S3.4, S4.4, and S5.8 of Supporting Information S1). These variables define requirements, among others, the air
input, the adsorbed or absorbed amount of CO2 per hour, sorbent supplies (make-up and start-up demand), and the energy consumption of air
moving, heat exchangers, heating devices, or fluid pumps (see Tables S3.5, S4.5, and S5.9 of Supporting Information S1).
648 SIMON
FIGURE 1 Schematic representation of an adsorber unit
One amine-based adsorption and two absorption methods were selected because these two types of technologies constitute 72% of recent
research and patenting activities (Li et al., 2013). The following subsections describe the train of thought, how the energy and material requirements
of adsorption on modified amines (Wurzbacher, 2015), absorption in a special amine–water solution (Ohle, 2009, 2010), and alkaline solution were
calculated (Keith & Mahmoudkhani, 2012; Keith et al., 2015).
The calculation scheme and results were validated by comparison with the most recent publications reporting the energy consumption of adsorp-
tion (de Jonge et al., 2019; Deutz & Bardow, 2021; Bajamundi et al., 2019; Repond, 2017) and absorption (Keith et al., 2018; Sabatino et al., 2021)
(Table S1.1 of Supporting Information S1). The requirements of civil engineering are also calculated; however, the demands for material and mechan-
ical work of construction can vary over a wide range, as they hardly depend on the particular conditions of the construction site, such as the bearing
capacity of the soil (Day, 2010; Hemsley, 2000).
2.1 Adsorption
The current adsorption model is based on the temperature vacuum swing (TVS) adsorption method. Ambient air flows through a filter consisting
of an amine-based active material and porous support. Desorption occurs under vacuum and elevated temperatures (see Figure 1). Working con-
ditions and civil engineering demands are based on the general physical parameters and equations. Some values were taken from different reports
of ClimeWorks-DAC projects and were adjusted to the current situation, such as lifetime, module net capture capacity (Deutz & Bardow, 2021;
Lozanovski, 2019; Schreiber et al., 2020), pressure loss, capture efficacy, sorbent sorption capacity, sorbent decomposition rate or heat capacity of
sorbent support (see Table S3.1-3.8 of Supporting Information S1) (Gebald et al., 2011, 2013, 2015; Qi et al., 2020; Wurzbacher et al., 2016).
The requirements for civil engineering were reported by Schreiber et al. (2020), Lozanovski (2019), and Repond (2017). Deutz and Bardow (2021)
also considered the impacts of construction, although only the resulting CO2 equivalent GHG emissions have been reported without detailed LCI.
The DAC device was mounted on four columns several meters high from the soil. Supporting the large weight of adsorption machinery, a raft-type
foundation was selected based on the potential load of each pillar (Day, 2010; Hemsley, 2000).
2.2 Absorption in organic solution (washing column)
Absorption in amine-based solutions, similar to the adsorption by amines, provides the advantage of the low thermal intensity of desorption, in
contrast to the high thermal requirement of calcination processes (Baciocchi et al., 2006; Olah et al., 2011; Socolow et al., 2011; Yu et al., 2012).
GenosorbN (GS) (poly(methyldiglycol)amine) is an amine-containing low vapor pressure detergent; consequently, it might have low toxicity and
unlimited miscibility with water (Ohle, 2009). The modeled vertical counterflow washing system is based on Ohle (2009, 2010). The present study
is one of the firsts describing such absorption technology in detail.
The ambient air enters at the bottom of the absorber column (see Figure 2), flows through the packed bed, and leaves the absorber at the top
with a low CO2 concentration. The saturated sorbent is conveyed into the desorber column for recovery after a subsequently connected plate heat
exchanger. The temperature of the exhausted sorbent after leaving the plate heat exchanger was assumed to be 55−60◦ C. Desorption is carried
out at 70◦ C under vacuum at 200 mbar (Ohle, 2009). The diluted sorbent/water mixture is recovered in a thin-film evaporator to eliminate the
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FIGURE 2 Schematic flow chart of absorption operation (amine-based washing fluid, counterflow vertical column)
co-absorbed moisture by 0.5 kg/kg sorbent (Ohle, 2009). The recovery requires 3−8 kWhel /m3 water evaporated (Tleimat & Tleimat, 1995, 1996).
Evaporation occurs at 50◦ C which is in the range of the desorption decreasing its energy consumption.
A GS concentration of 50 wt.% is assumed to be used for CO2 capture purposes (see Table S4.4 of Supporting Information S1), as it leads to the
lowest moisture absorption from the air (Ohle, 2009). The calculation in Table S4.4 and S4.5 of Supporting Information S1 follows the conceptual
design of Ohle (2010). Different process steps were also adapted to the model, such as the design of sorption columns (Andersson et al., 2020;
Baciocchi et al., 2006; Mahmoudkhani et al., 2009; Mazzotti et al., 2013; Stripple & Zhang, 2018) and sorbent recovery with thin-film evaporation
(Tleimat & Tleimat, 1995, 1996). Several system elements have been scaled to the analyzed capture capacity based on data from laboratory and
similar large-scale technologies (Supporting Information S1, Piccinno et al., 2016; Simon et al., 2016), while the efficacy of CO2 capture per pass is
based on literature values (Baciocchi et al., 2006; Keith et al., 2018; Zeman, 2007).
The civil engineering demand is based on the assumption that the system consists of packed bed columns with diameters of 10−13 m. This
enables a low surface load per square meter. Thus, a simple slab foundation also meets the required bearing capacity (Schroeder, 2001). The whole
1 Mt/a plant requires at least 250 capture units (combination of above-described absorption–desorption columns), which is in accordance with
Mazzotti et al. (2013). Packaging properties were obtained from specific producer (MML, 2021), while the plate heat exchanger with an average
flow rate of 150 m3 /h was based also on the information of manufacturer (see Table S4.7 of Supporting Information S1, Onda, 2021).
2.3 Absorption in inorganic (alkali) solution
Carbon dioxide exhibits acidic characteristics. Hence, chemical absorption on an alkali-basis has proved to be a possible method for DAC (Baciocchi
et al., 2006; Keith et al., 2018; Mazzotti et al., 2013; Socolow et al., 2011; Stolaroff et al., 2008).
The recent model describes the CO2 capture by NaOH and Ti-based recovery reported and patented by Keith and Mahmoudkhani (Keith &
Mahmoudkhani, 2012; Keith et al., 2015). Even though KOH-based pathway was also suitable and analyzed by Keith et al. (2018) and de Jonge et al.
(2019), NaOH-based absorption was selected for the analysis because of the lower prices of NaOH (Chemanalyst, 2021a, 2021b) and lower heat
of reaction of titanate-based recovery loop (Mahmoudkhani & Keith, 2009). Thus, the present study is the first describing this system compilation
depicted in Figure 3.
Figure 4 depicts the three main parts of the model: the direct air contactor used to capture ambient CO2 (Holmes & Keith, 2012; Keith, 2009;
Keith & Mahmoudkhani, 2012; Keith et al., 2018), the crystallization of Na2 CO3 from a saturated solution for causticizing in a fluidized bed reactor
(FBR) (Dimoplan, 1978; Giesen et al., 2009; Keith & Mahmoudkhani, 2012; Mahmoudkhani & Keith, 2009), and the leaching recovery of NaOH using
sodium titanate (Keith & Mahmoudkhani, 2012; Nohlgren et al., 2000; Ruthven et al., 1993) .
The air flows through in a cross-flow air contactor, where NaOH reacts with atmospheric CO2 developing Na2 CO3 . The regeneration of the
NaOH solution and retrieval of CO2 by causticization accord to the Ti method which is a complex procedure as follows. Sodium carbonate decahy-
drate precipitates (see Table S5.12 of Supporting Information S1) after cooling the saturated sodium carbonate solution. This step is followed by
a resolution in warm water to eliminate crystal water from Na2 CO3 *10H2 O. After resolution, NaOH is leached by adding sodium pentatitanate
(see Equation 1). The formed sodium trititanate and sodium carbonate are crystallized in a subsequent process and conveyed to a FBR to retrieve
captured CO2 and sodium pentatitanate (see Equation 2 and Table S5.13-S5.14 of Supporting Information S1) (Keith & Mahmoudkhani, 2012; Keith
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FIGURE 3 Schematic representation of the NaOH-based DAC plant
F I G U R E 4 (a) Thermal, (b) electrical energy and (c) material demand of capturing 1 ton of CO2 (mean value, upper and lower 95%; min. and
max. values). Blue bars represent the adsorption, green is for absorption while grey bars stand for literature values. Calculated values are based on
1000 iterations, while literature values were taken from up to 18 reported values (Baciocchi et al., 2006; Brilman & Veneman, 2013; House et al.,
2011; Keith et al., 2006; Kulkarni & Sholl, 2012; Lackner, 2009; Lozanovski, 2019; Mahmoudkhani & Keith, 2009; Mahmoudkhani et al., 2009;
Schreiber et al., 2020; Socolow et al., 2011; Stolaroff et al., 2008; Wang et al., 2013; Zeman, 2007, 2014; Zhang et al., 2014, 2). Underlying data are
available in Table S6.1-6.3 of Supporting Information S1
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F I G U R E 5 Fluctuation of electricity consumption based on different parameter ranges (median, 95th percentile, and min–max values).
Underlying data are available in Table S7.1 of Supporting Information S1
et al., 2010; Mahmoudkhani & Keith, 2009).
3 (4Na2 O ∗ 5TiO2 ) + 7H2 O ↔ 5 (Na2 O ∗ 3TiO2 ) + 14NaOH (1)
7Na2 CO3 + 5 (Na2 O ∗ 3TiO2 ) ↔ 3 (4Na2 O ∗ 5TiO2 ) + 7CO2 (2)
Keith et al. (2018) and de Jonge et al. (2019) reported an inventory for the capture system; however, the secondary loop of salt recovery was
excluded from these datasets. While Liu et al. (2020) assess the carbon intensity of an alkali absorption-based DAC-to-fuel system, however, the
study lacks a detailed LCI and the analysis of civil engineering based on GHG values from EEIO LCA (environmentally extended input–output LCA).
The model of the air contactor in the current analysis is based on patents (Keith & Mahmoudkhani, 2012; Keith et al., 2015) and reports from the
last decade (Holmes & Keith, 2012; Holmes et al., 2013; Keith et al., 2010). Carbonate recovery is modeled by a system of crystallizers, fluid storage
tanks, and FBR taken from different reports and adapted to the current situation (Althaus et al., 2007; Frischknecht et al., 1996; Giesen et al., 2009;
Myöhänen et al., 2017; Turner, 2000).
2.4 Sensitivity analysis through parameter varations
The calculator was also tested through a sensitivity analysis to identify the technical bottlenecks. The following parameters were random-
ized (with “RAND” function) using 1000 iterations between two determined minimum and maximum values in Excel® (see Tables 3.4, 4.4,
5.8 of Supporting Information S1, and cf. Figures 5 and 6):
∙ The captured fraction (net capture efficiency of the plant—capture efficacy) was altered between 60% and −100% for each technology analyzed
(Baciocchi et al., 2006; Gebald et al., 2015; Mahmoudkhani et al., 2009; Mazzotti et al., 2013).
∙ The pressure drop in the capture section was changed between 100 and−500 kPa for adsorption (Gebald et al., 2015) and 65−120 kPa/m column
for amine absorption (Mazzotti et al., 2013). Because of the lack of information the pressure drop was fixed on 9.7 kPa/m depth for the NaOH
absortion (Mahmoudkhani et al., 2009).
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F I G U R E 6 Deviation of thermal energy requirement based on different parameter arrays (median, 95th percentile, and min–max values).
Underlying data are available in Table S7.2 of Supporting Information S1
∙ Ranges for sorption capacity were selected for 26−110 and 7.7–110 mg CO2 /g sorben per cycle for adsorption and amine absorption,
respectively (Gebald et al., 2011; Ohle, 2010).
∙ The efficiencies of the air fan and fluid pumps were selected as 45−65%, 80−90%, respectively (cf. de Jonge et al., 2019; Keith et al., 2018;
Sabatino et al., 2021).
∙ The efficiency of heat recovery from FBR was assumed fo 45−65%, the dry content of the input trititanate was changed in the range of 85−95%
while the heating efficiency of the reactor was selected for 85−95% (Dones et al., 2004; Keith & Mahmoudkhani, 2012).
The results of the randomization are then evaluated in aggregated form in Figure 4, and in Figures 5 and 6 they are disaggregated by the particular
parameters.
2.5 The maximum obtainable energy assigned to CO2 emissions
The primary energy deployed in the construction and operation of capturing atmospheric CO2 is defined as embodied energy (cf. Section 1). Worst-
case and best-case scenarios were deduced from the most efficient and efficient energy- or material-conversion processes. Basic datasets for the
estimation of embodied energy of the process inputs, such as cement, steel, gravel, soil work, different plastics, and thermal and electrical energy
were taken from the Ecoinvent database (Version 3.5) (Wernet et al., 2016).
Furthermore, a reference value for embodied energy of CO2 capture was calculated to indicate the breakeven point from which the capture uses
more energy than the theoretically maximal gain from CO2 emission. Methane exhibits one of the highest lower heating value (LHV) among carbon-
containing fuels. Consequently, it can be used to calculate the above-mentioned limiting values. The conversion factor of methane to carbon dioxide
is ∼2.75 kg CO2 /kg CH4 . Thus, perfect oxidation of methane (50 MJ/kg LHV) to CO2 results in an energy development of 18,182 MJ per each kg
CO2 released from this particular burning process. This value also encompasses the formation of water. This means that if we emit 1 kg CO2 from
CH4 -burning process, theoretically 18.2 GJ thermal energy released. Using the enthalpy of formation from constituent elements (elementary C and
O2 ), the result is 8,942 MJ/t CO2 formed. This means that the emission of 1 kg CO2 from CH4 -burning thermodynamically results in the formation
of 8.94 GJ thermal energy. Accordingly, DAC technologies requiring more energy embodied in the “cradle to gate” life cycle than 8.94 GJ/t captured
CO2 are working on energetically inefficient point, because more energy is needed than emission of 1 kg CO2 can provide.
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2.6 The background data
Different sorbent active materials and support materials were also modeled to estimate the embodied energy of the capturing process.
Tables S2.1-S2.12 of Supporting Information S1 describe the calculation used to obtain the embodied energy in MJ/kg CO2 captured. Selected
sorbent and support combinations were taken from highly cited literature (Azarabadi & Lackner, 2019; Goeppert et al., 2014; Zhang et al., 2015).
The specific heat capacities of the sorbents (Cakstins, 2015; Chase, 1998; Ohle, 2010) and supports (Qi et al., 2020) were used to estimate the
minimal thermal energy demand for thermal sorbent recovery. Chemical reactions and energy requirements of material synthesis, such as NaOH
(Boustead, 2005) and silica (Ambaryan et al., 2020; Barthel et al., 1995; JRC, 2007), amines and silanes (Gaochao et al., 2014, 2015; Schwarz et al.,
2002), as well as, sorbent recovery processes (Hackett, 2018; Tedeschi & Wilson, 2010) are based on the literature. Embodied energy, namely the
whole energy demand from cradle to gate, was taken from the Ecoinvent database cut-off version 3.5 (Wernet et al., 2016).
Adsorption is assumed to have TRL 8−9 based on the fact that the Orca carbon capture facility was commenced on September 9 in Iceland with a
capture capacity of 4 kt/a (Reuters, 2021). The amine absorption is on TRL 5−6 because of the large laboratory scale carried out by Ohle (2010). The
NaOH absorption is assumed to be on TRL 7−8, because several parts are tested on a large scale, but the entire power-to-fuel process is waiting for
a near-future realization (CE, 2021). Furthermore, the most recent studies in this field have analyzed KOH-based recovery of carbonate (de Jonge
et al., 2019; Keith et al., 2018; Madhu et al., 2021), whereas the current study includes Ti-based recovery with a low TRL of 5−6 as it is well studied
and patented (Bonsu et al., 1996). Accordingly, the novel modeling of Ti-based recovery limits the direct comparison of outcomes to recent studies
using KOH-based recovery.
Low differences in TRL might partly affect the comparability of processes because a higher TRL presumes a higher level of knowledge, even
though the calculator is predominantly based on secondary data, because primary information is difficult to obtain. It should be noted that most of
the available unit processes in the LCA rely on secondary data. In addition, science-based engineering calculations enable us to obtain secondary LCI
data of good quality reflecting a close reality. The TRL-related issue was handled with sensitivity analysis (see parameter variations in Sections 2.4
and 3.3) using ranges of input values instead of single numbers (Moni et al., 2020).
3 ASSESSMENT OF ENERGY AND MATERIAL FLOWS
This section sheds light on significant material and energy flows of operation phase of DAC (Section 3.1). A parameter variation shows the possible
outcomes of energy requirement (Section 3.2) also broken down to each working parameters (Section 3.3) while cradle-to-gate embodied energy
was also analyzed (Section 3.4). The findings were compared with the recent knowledge from the literature in this field.
3.1 An overview of significant energy and material flows
The following section provides an insight into the material and energy flows in the use phase of the DAC (see Supporting Information S1). A 1 Mt/a
plant requires up to 1000 DAC units, as described in Supporting Information S1, which is composed of smaller modules, as depicted in Figure 2
(Deutz & Bardow, 2021; Schreiber et al., 2020)
Since LCA-based studies report only degradation-related material requirements, the capital amount remains hidden, which represents higher
volumes of the required material. Up to 11 kilotons (kt) of sorbent materials (50:50 active:support material) are required by a 1 Mt/a DAC-plant and
500 kg sorbent material decomposes (250 kg amine active material) every hour of the operation (for more information, see Supporting Informa-
tion S1, Table S3.3). A significant amount of water develops owing to the co-captured air moisture by up to 222 m3 /h (115 ton CO2 /h). Consequently,
a lower air humidity would lead to lower wastewater development. Although no information is available on its quality, we can assume, based on its
origin, that no environmentally relevant contamination is present.
In amine absorption, more than 127 m3 /h of washing fluid has to be moved in each washing unit on average. A 1 Mt/a plant requires up to 250
of such washing columns (Mazzotti et al., 2013) The saturated sorbent is pumped into a plate heat exchanger to utilize the “waste heat” of the
sorbent regenerated from the desorption column. The average electricity consumption is found to be lower than that at adsorption, whereas the
heat requirement is double of it.
The sorbent makeup of NaOH absorption is subtle because it is modeled to occur only by the hydroxide drifting effect into the air. Water house-
hold is calculated on the basis of vapor pressure of water in the system. This can lead to wastewater production or water makeup depending on
ambient temperature and relative air humidity (Socolow et al., 2011). Electricity demand is typically high due to the energy-intensive thermal swing
(cooling with heat pump requires up to 27% of the whole electric energy demand) for crystallization where up to 6000 m3 solution is chilled by
5−20◦ C (see Table S5.8.1 of Supporting Information S1; Keith & Mahmoudkhani, 2012; Socolow et al., 2011). Share of pumping work required is
significantly high compared to the calculated energy consumption of the overall process (up to 50% share; cf. Section 3.2).
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3.2 Effect of parameter variation on sorbent and energy flows in the use phase
Figure 4 represents the possible energy and sorbent consumption as a function of different variables (see Tables S3.4, S4.4, S5.8 of Supporting
Information S1, and section 2.4). The columns in Figure 4 merge the parameter variations described in Section 2.4 and are expressing only the use
phase energy requirement. The colored columns originate from the outcomes of their own calculations, whereas the values for grey columns are
based on other studies. The exergy for the thermal energy demand of adsorption and amine absorption was calculated using Equation (3) (Terzi,
2018).
( )
T0
e = Q̇ recovery ∗ 1− (3)
Trecovery
Where, Q̇ recovery and Trecovery stand for the heat and temperature required for CO2 desorption, while T0 represents the ambient temperature
(20◦ C). The exergy of the high-temperature sorbent recovery of NaOH absorption and all electricity consumption is the same as the particular
energy requirement (Sabatino et al., 2021).
The literature data of the thermal energy for the absorption and adsorption varied between 4.0–11 and 3.2–7.2 GJ/t CO2 , respectively, while
electricity demand ranges between 125−1200 and 200−1000 kWh/t CO2 , respectively (cf. Figure 4a,b). The calculated thermal energy requirement
moves in a broader range than the literature data, between 2.6 and 17 GJ/t CO2 , while the electricity consumption vary on a narrower range than
literature data (between 83 and 903 kWh/t CO2 ).
The calculated thermal energy requirement for adsorption is close to the values reported in the literature. Amine absorption shows a significantly
broader distribution and higher values than NaOH absorption, and the 95th percentile of both types ranges on the same scale as the literature val-
ues. The high peak of thermal energy requirement calculated for amine absorption can be explained by the specific heat capacity of the sorbent fluid
(measured to be 3.6 kJ/(mol*K) (Ohle, 2009)), resulting in considerable thermal energy demand in the desorption phase even at moderate temper-
atures (10.5 GJ/tCO2 at 70◦ C). However, the heat for amine desorption can be fed by low-quality energy, such as waste heat, the implementation
of such water/amine mixture-based sorbents with high specific heat capacity might be hindered by the availability of low-quality heat. The heat
requirement of NaOH absorption moves in a narrower range as for amine-based absorption. However, obtaining CO2 from carbonates occurs at a
high temperature of 850−900◦ C. This results in a substantial difference in exergy requirement compared to low-temperature desorption (exergy
of NaOH absorption is the same as the energy requirement while exergy of technologies demanding low-quality heat is lower than their apparent
energy consumption). The demand for high temperatures confines the NaOH absorption to the availability of natural gas or other deployable fuels.
The mean value of the calculated electricity consumption for adsorption overlaps with the literature, although wider marginal (95th percentile)
values have been found based on other reports (cf. Figure 4). This higher upper percentile suggests more conservative assumptions in the literature.
Sensitivity analysis explains in detail this deviation (Section 3.3). The calculated electricity consumption for the absorption processes shows a more
concentrated picture, as can be found in the literature. The higher values of NaOH absorption, compared to the amine counterpart, can be explained
by the system setting of thermally controlled crystallization, which requires significant cooling energy of large sorbent amounts to obtain solid
carbonates (heat pump requires 26% of the entire electricity consumption, cf. Table 1). The further energy-intensive procedure is the extensive
differences in the potential energy of the sorbent fluid in the case of 20 m tall washing columns.
Figure 4c depicts the differences in the active material requirements depending on the changing process parameters (cf. Table S3.4, S3.5, S4.4,
S4.5, S5.8, S5.9 of Supporting Information S1). The current literature provides a similar value of 3.75 kg of active material per ton of CO2 cap-
tured, and further effects of changing working conditions are neglected (Deutz & Bardow, 2021; Lozanovski, 2019; Repond, 2017; Schreiber et al.,
2020). The current adsorption model, however, results in values ranging on a wide scale (0.77–9.55 kg sorbent/t CO2 with a median of 2.44), in con-
trast to the low deviation of amine and NaOH absorption. Different parameters affect sorbent demand. For example, adsorption is modeled with
a higher decomposition rate of sorbent reported for ∼0.01% per cycle (Gebald et al., 2013), compared to the calculated considerably lower deteri-
oration of amine in fluid support up to ∼0.0008% per cycle (Davis & Rochelle, 2009; Heydari-Gorji & Sayari, 2012) and NaOH loss in air contactor
by ∼0.235 mg/m3 air throughput (Holmes et al., 2013). The sorption capacity of GenosorbN is calculated for 7.7 mg CO2 /g sorbent in each cycle,
while adsorption can capture 32.1 mg CO2 /g sorbent in the base case (Gebald et al., 2011; Ohle, 2009), which can lead to different sorbent con-
sumption. Eliminating this theoretical discrepancy of decomposition and sorption capacity by deploying the same factors for both technologies, the
amine absorption requires up to 150 kg sorbent make-up per ton CO2 on average. However, using a lower sorbent flow rate in the washing column,
according to the recommendations of packing producers down to 0.2 m3 /m2 *h instead of the originally implemented 8.5 m3 /m2 *h (Ohle, 2009), the
sorbent make-up decreases to the same level as of the adsorption (∼1.0–10 kg sorbent/t CO2 ).
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TA B L E 1 “Cradle-to-gate” life cycle embodied energy of each technology normalized to 1 ton of captured atmospheric CO2
3.3 Bottlenecks and pivots (sensitivity analysis)
Capture efficacy shows significant sensitivity, especially in the case of NaOH absorption (see Figures 5 and 6). The higher sensitivity of the
mentioned technology in the heat demand (Figure 6) can be explained by the thermally intensive desorption procedure.
Pressure drop represents a limiting factor, as a large volume of diluted air is required for capture. DAC typically works directly with unconditioned
ambient air containing solid particles such as dust, sand, or different organic components, leaves, or insects. Deposits of such solid contaminants
increase the pressure drop in the adsorption device by fouling the capillaries of the sorbent. This might result in a rapidly decreasing capture
efficiency and increasing sorbent demand. Thus, it causes larger deviations in electricity consumption (cf. Figure 5).
Likewise, the washing fluid in absorption might be contaminated by ambient air, leading to unwanted chemical–physical reactions, resulting in an
increasing make-up demand. Accordingly, deploying an air treatment regime is worth considering with regard to the trade-off between electricity
demand and efficient sorbent usage.
The pressure drop was also identified as a bottleneck in electricity consumption in a vertical flow absorption column. This depends on the gas
and fluid velocities defined by the packing material (Baciocchi et al., 2006; Mazzotti et al., 2013; Tan et al., 2012). This structural constraint can
be tackled by a diagonal contactor where the air streams horizontally (Holmes & Keith, 2012; Holmes et al., 2013). Accordingly, the diagonal flow
656 SIMON
design might significantly mitigate the air-fan-related energy requirements (see Figure 5, the lower sensitivity of NaOH absorption in the pressure
drop).
Such “diagonal constructs” enable to build a higher stacked tower as absorption columns. The gross height of the absorption facility represents a
trade-off between the fluid pumping work and land occupation, as a lower-built facility requires less pumping work but uses a larger land surface. It
is worth considering whether land occupation becomes a sensitive factor in planning (cf. sensitivity of pumping efficiency in Figure 5).
A further sensitive parameter is the air fan efficiency affecting adsorption more remarkably as absorption (cf. share of fan in embodied energy,
Table 1). Careful selection of industrial heat pumps for the NaOH-absorption system is crucial because of the large share in the overall energy
consumption (cf. Table 1).
The efficiency of heating devices in absorption processes is crucial. Thus, a well-designed insulation system is highly important for achieving
moderate heat requirements. Nevertheless, the efficiency of heat exchange between desorption and the saturated sorbent was found to be vital for
moderate heat management in amine absorption (see Figure 6).
In conclusion, the sensitivity analysis sheds light on the fact, how, and which operational parameters are crucial for managing the direct energy
requirement of the capture process (Young et al., 2021). For example, a properly selected sorbent structure with a low pressure drop can consid-
erably decrease electricity consumption, while the efficiency of gas and fluid movement also plays a vital role. The sorption capacity of sorbents is
crucial for the moderate specific heat requirement of desorption, whereas the heat efficiency of thermal devices and especially the efficiency of the
heat exchanger of amine absorption are important to tackle high heat requirements.
3.4 Life cycle embodied energy
Table 1 shows the embodied energy of each technology divided into the best and worst cases. The values are broken down to the environmental cost
of civil engineering and the impacts of the operation (“running cost”). Each value is of the same order of magnitude; however, adsorption is calculated
to demand 1.5–2 times more energy for foundations than the counterpart technologies. This can be explained by the higher need for a DAC unit
for a 1 Mt/a plant, furthermore, amine absorption requires less foundation owing to the slightly lower load factor of the wide absorption columns.
Assuming that the material requirement of machinery is a demanding task (cf. Table S3.6, S4.7-4.8, S5.16, S5.18-5.19 of Supporting Information S1).
Lozanovski (2019) and Schreiber et al. (2020) report the numbers for machinery consumption of an adsorption DAC unit, Deutz and Bardow
(2021) also analyze a similar system. However, contrary to the previous two, Deutz and Bardow (2021) deploy an alternative lifetime without
describing the exact inventory of construction. Thus, obtaining machinery LCI for the current calculation tool was encumbered because of this
minuscule discrepancy in the underlying literature. The information on adsorption was more elaborated; accordingly, Table 1 describes significantly
higher embodied energy for adsorption machinery than for absorption. Without considering aluminum and copper, for which no information is
available for the absorption, the figures of adsorption would decrease nearly to the same range as the counterpart technologies.
However, the construction of the plant is an important life cycle stage, less significant from the embodied energy point of view, as DAC is typically
an energy-intensive process. Consequently, impacts of operation, due to the purchased energy, considerably outweigh the “capital costs.”
The sorbent demand in Figure 4c is also manifested in the embodied energy. These values exhibit uncertainty, as described in Section 3.2. Namely,
the higher decomposition rate of amine absorption might lead to a remarkably higher embodied energy. Air fans are the most important machinery
parts, especially for adsorption, where air movement is the main consumer of electricity, accounting for up to 95% of the embodied energy. Fluid
pump becomes an important part of absorption technologies, as the column height determines the potential energy to overcome by fluid pumping.
For example, the sorbent fluid has to be pumped up to 20 m high in the case of NaOH absorption.
Sorbent recovery accounts for 9.5% of the total electricity input of amine absorption, encompassing the evaporation of surplus absorbed
moisture; accordingly, managing the uptake of water by the washing fluid plays an important role in electricity consumption. Similarly, in NaOH
absorption, the recovery loop requires up to 40% of the entire embodied energy, that is, cooling the saturated solution before crystallization and
generating nearly pure oxygen for oxy-combustion in the FBR.
3.5 Operability of DAC calculator
Schreiber et al. (2020) considered anionic resin for modeling sorbent materials based on Ecoinvent 3.5. It results in 3.18 kg CO2e /kg resin (Wernet
et al., 2016), while the same figure for the calculated aminosilane ranges between 4.76 and 13.59 kg CO2e /kg sorbent (depending on material
degradation rate and sorbent capture capacity). The required energy is set to 500 kWh and 5.4 GJ for electricity and thermal energy, respectively
(Schreiber et al., 2020). However, this value can change between 80−800 kWh and 3.0–9.0 GJ due to varying operation parameters. This wide
difference might considerably affect the result, making the power-to-fuel production environmentally less attractive as it projected.
Liu et al. (2020) found that 139 g CO2e /kWhe is required for synthetic fuel production to outperform the GHG intensity of conventional diesel
fuel. However, the electricity consumption of alkali-based absorption can deviate by ± 35–40%. The so-calculated wide array of GHG emissions
SIMON 657
from electricity can drastically impact the carbon footprint of DAC-based fuels. Accordingly, in some cases, the range of 102−139 g CO2e /kWhe is
required to provide environmental benefits against fossil-based diesel.
As shown in Figures 5 and 6, electrical energy is the main energy source in the absorption/adsorption phase, while thermal energy is deployed
for desorption and causticization, but to a larger extent. Thus, access to different sources of thermal energy limits the overall process. For example,
future diverse political decisions, such as phasing out fossil coal-fired thermal power plants from the national energy mix can lead to a lack of low-
value heat to meet DAC capacities. It might rebound in deploying high-quality energy sources (electricity or natural gas) (Schreiber et al., 2020).
However, using power-to-heat based on renewable electricity is a viable option for desorption, whether it is direct heating or heat pumps (IRENA,
2019; Sternberg & Bardow, 2015). Furthermore, converting solar energy directly to heat using solar collectors can also fuel the desorption process
(Bhatia, 2014).
Although renewables offer a low-carbon energy source for DACs, their availability is constrained by time and space. Different load leveling and
peak shaving methods (e.g., battery storage) might enable the use of more renewables at a low price and low cumulative energy demand (Baumann
et al., 2013; Daggash et al., 2018; Zimmermann et al., 2013). Hence, the realization of a large-scale DAC project might require international coop-
eration by placing DAC and other components close to renewable sources (cf. Power-to-X exports from North Africa to Europe, Boulakhbar et al.,
2020).
Considering the above-discussed capacity constraints and energy availability for DAC purposes, further systematic analyses will answer the
question of how DAC can appropriately be tailored and embedded in a particular system to obtain low environmental burdens. The known param-
eter sensitivity provides essential information for further planning. Optionally, if the present study was expanded into a broader material flow
analysis of special cases, the pedigree matrix extended data analysis could significantly support the uncertainty evaluation of each estimated
parameter. Accordingly, the present sensitivity analysis can be completed using the coefficients of variation (Laner et al., 2016).
The present parameterized model shows that the embodied energy of the DAC is above the calculated formation energy of CO2 (8.94–18.2
GJ/tCO2 ). However, by selecting an appropriate sorbent material and operational parameters, the energy demand for adsorption can be decreased
below this value (Young et al., 2021). Table 1 indicates that thermal energy represents the bottleneck of embodied energy, with the highest demand
for primary energy sources, thus significantly contributing to embodied energy. This raises the demand for thorough analysis and planning of the
DAC in the design phase to find its energetically affordable implementation (according to the sustainable and responsible use of renewables).
Indeed, several studies have shown that DAC is an essential part of the climate-mitigation puzzle. The first inter-model comparison revealed that
direct air capture and storage (DACS) might help reduce climate-mitigation-related costs despite the extensive energy requirement (Realmonte
et al., 2019).Another study stated that global restoration of cultivated lands by 15% would sequester up to 299 Gt of atmospheric CO2 (Strassburg
et al., 2020). This type of sequestration in the solid state is probably a more sustainable and responsible way of CCS than direct geological storage.
However, geological CCS gives us time to find the answer to the question of “what to do with CO2 ” because biological sequestration requires a long
time period to become effective. Indeed, the IEA (2020) shows that the share of DAC in capture technologies will run up to 4%, while approximately
8% of captured CO2 will be conveyed to market value creation, such as CO2 -(petro)chemistry. This suggests that DAC is more suitable for short-
and mid-term carbon management, capturing CO2 from dissipated sources, or creating market value via CCU, such as power to fuel. DACS is also
a viable option to bridge the time gap between short- and long-term carbon management (Daggash et al., 2018; van der Giesen et al., 2017). These
tactical choices may overwrite the question of DAC’s high embedded energy demand.
The high energy consumption might be tackled by using passive air contacting and harnessing the wind to move air through the sorbent layer
(Lackner, 2014). The combination with humidity-swing adsorption (HSA) can completely eliminate any additional heat requirement (van der Giesen
et al., 2017). Even though, the so-called “artificial trees” with HSA might require significantly less electricity by up to 210 kWhe /t CO2 , the capture
efficacy might extensively decrease due to idle time of windless periods. This might increase the investments cost to meet required capacity.
4 SUMMARY
As CO2 chemistry and DAC appear more frequently in the context of a low-carbon future (Goeppert et al., 2012; Olah et al., 2011), the number
of science-based environmental assessments has increased to analyze the validity of future technologies. To meet this demand, the current study
provides a transparent calculation method of LCI for selected DAC technologies and enlightens the parameters representing a bottleneck or even
playing a pivotal role in energy and material consumption. The calculation tables in Supporting Information S1 represent a data generation tool for
the LCA of product systems encompassing atmospheric carbon capture. There is also an option to develop and extend the tables.
The calculator delivers values in the same order of magnitude as the latest research and measured data of this field (see Table S1.1 of Supporting
Information S1 and Bajamundi et al., 2019; de Jonge et al., 2019; Deutz & Bardow, 2021; Keith et al., 2018; Repond, 2017) This close correlation
presumes the correctness of the calculation paths. In addition, the calculator provides a detailed parameter analysis, which is not available in the
most recent literature. It supports the calculation of an appropriate range of environmental impacts, enabling a more sophisticated evaluation of
the analyzed system and careful future planning.
658 SIMON
Summarizing the results, the thermal energy requirement contributes extensively to the overall energy consumption of the DAC, followed by
the electricity of forced air movement, as a large volume of air is required to treat for each ton of CO2 captured. Fluid pumps are more significant
for fluid-based sorption. This makes the height of the absorption column an important factor, enabling significant energy saving by an appropriate
design. However, lower-built air contactors with less pumping work requirements result in larger land occupation (cf. Section 3.3).
Construction demand exhibits negligible figures in the overall life cycle, even though the type and measures of the foundation depend on the
on-site conditions. Thus, this calculation is highly uncertain without knowing the particular circumstances.
An important finding is that embodied energy analysis shows large energy demand in most cases. Namely, capturing one unit of atmospheric
CO2 often requires more energy, as it thermodynamically can be obtained by the formation of the same amount of CO2 . This can become a
bottleneck in the case of rising energy prices. Implementing sorbents with high sorption capacity, developing technologies with low thermal
energy demand, and thoroughly selected operational parameters represent a suitable direction for an energetically optimized DAC (Young et al.,
2021).
The current DAC model delivers valid results without using complex software-based simulations. It represents a general basis for future inte-
grated assessment models and LCA studies in the field of DAC and CO2 chemistry supporting more transparent results. The model can be elaborated
to include more details of material losses or a new design for sorbent recovery in absorption systems.
ACKNOWLEDGMENTS
Special thanks to the Ministry of Economics, Innovation, Digitalization, and Energy of the State of North Rhine-Westphalia for the support through
project SCI4climate.NRW (EFO-001D). This study was partly supported by the German Federal Ministry of Education and Research through
Kopernikus-P2X (03SFK2WO). Special thanks to Prof. Dr. rer. pol. Grit Walther for her continuous support during the review procedure.
CONFLICT OF INTEREST
The authors declare no conflict of interest.
DATA AVAILABILITY STATEMENT

The data used in this study were obtained from multiple and diverse sources. The sources are cited in the appropriate places in the main text, and a
description of the availability of the various sources can be seen in Supporting Information S2.
ORCID
Balint Simon https://orcid.org/0000-0002-7828-0386
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SUPPORTING INFORMATION
Additional supporting information can be found online in the Supporting Information section at the end of this article.
How to cite this article: Simon, B. (2023). Material flows and embodied energy of direct air capture: A cradle-to-gate inventory of selected
technologies. Journal of Industrial Ecology, 27, 646–661. https://doi.org/10.1111/jiec.13357

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DOI: 10.1111/jiec.

Material flows and embodied energy of direct air capture

1 IMPORTANCE OF AN EX ANTE ENVIRONMENTAL ASSESSMENT OF DIRECT AIR CAPTURE

2 TECHNOLOGICAL OPTIONS OF THE ANALYZED DAC

FIGURE 1 Schematic representation of an adsorber unit

2.2 Absorption in organic solution (washing column)

2.3 Absorption in inorganic (alkali) solution

FIGURE 3 Schematic representation of the NaOH-based DAC plant

et al., 2010; Mahmoudkhani & Keith, 2009).

3 (4Na2 O ∗ 5TiO2 ) + 7H2 O ↔ 5 (Na2 O ∗ 3TiO2 ) + 14NaOH (1)

7Na2 CO3 + 5 (Na2 O ∗ 3TiO2 ) ↔ 3 (4Na2 O ∗ 5TiO2 ) + 7CO2 (2)

2.4 Sensitivity analysis through parameter varations

2.5 The maximum obtainable energy assigned to CO2 emissions

2.6 The background data

3 ASSESSMENT OF ENERGY AND MATERIAL FLOWS

3.1 An overview of significant energy and material flows

3.3 Bottlenecks and pivots (sensitivity analysis)

3.4 Life cycle embodied energy

3.5 Operability of DAC calculator

DATA AVAILABILITY STATEMENT

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