Negative emissions refer to the reduction of CO2, not only in comparison to alternative approaches or technologies but also in terms of a device’s lifetime emissions falling to a level below net zero. Negative emissions can be achieved by using natural resources to exploit them, developing through the development of advanced technologies, and using hybrid approaches, as described below.
Natural NET refers to maintaining, restoring, and managing ecosystems to reduce CO2 in the atmosphere and increase CO2 absorption. Figure 1 shows a classification of NETs.
The first layer is classified as natural, technological, and hybrid NETs. Natural NET is distinguished into three categories: reforestation and improved forest management, wetland and coastal restoration, and soil carbon restoration. A recent study estimated that natural NET will reduce CO2 emissions by 14 GtCO2/y by 2030 (Griscom et al. 2017); however, natural NET faces resource constraints, such as land, water, and nutrients; it also has the disadvantage of reducing biodiversity and albedo (Smith et al. 2016). Ocean fertilization, for example, is a natural NET that involves introducing nutrients into the upper ocean to promote algal growth and CO2 uptake; however, the efficiency of ocean fertilization is low and may harm ecosystems.
Technological NETs are measures to reduce CO2 emissions from the atmosphere through various geoengineering schemes. These include indirect ocean capture, enhanced weathering, and ocean alkalinity modification (enhancement), which involves increasing the ocean’s ability to absorb atmospheric CO2 by adding alkalinity (House et al. 2007; Kheshgi 1995). The ocean plays an important role in CO2 reduction because it absorbed approximately 30% of total CO2 emissions after the Industrial Revolution (Webb et al. 2021). Previous research has investigated ocean alkalinity modification methods and their effectiveness (Köhler 2020; Renforth & Henderson 2017). According to the scenario analysis by Ilyina et al. (2013), although significantly adding alkalinity to large areas is required to avoid further ocean acidification, rapid increases in alkalinity over a broad ocean area may have an unexpected negative impact on the natural environment. Indirect ocean capture, which chemically treats seawater and returns decarbonized and alkalized seawater to the sea (de Lannoy et al. 2018; Eisaman et al. 2018), is another method to improve the ocean’s ability to absorb CO2. However, this method is still in the experimental stage.
Another NET that has recently piqued the interest of researchers is enhanced weathering, which has the potential to reduce CO2 in the atmosphere by improving the chemical weathering of rocks. Enhanced rock weathering has great potential in terms of performance and cost (Beerling et al. 2018, 2020), but its environmental impact is still unclear.
To reduce CO2, hybrid NETs combine natural and technological approaches, and bioenergy with carbon capture and storage (BECCS) is recognized as the most mature technology (de Lannoy et al. 2018). BECCS combines bioenergy applications and CCS; using energy derived from biomass combustion and capturing and storing CO2 emitted during combustion results in net CO2 removal (Bui et al. 2018). Although BECCS has the potential to play an important role in mitigating climate change (Duan et al. 2021), promotional challenges, such as efficiency and CO2 transportation, remain (Smith et al. 2016).
DAC systems (also known as postcombustion capture systems) remove CO2 directly from the atmosphere and are classified into three types: liquid solvent, solid sorbent, and membrane-based systems. Ishimoto et al. (2017) provided an overview of DAC estimation, proposing a wide range of cost estimates ranging from USD 100/tCO2 to USD 1000/tCO2.
The liquid-solvent DAC system includes an air contactor and a regeneration facility. In the air contactor, CO2 from the air reacts with potassium hydroxide solution (KOH) to produce water and potassium carbonate (K2CO3), as follows:
2KOH + CO →HO + KCO
The potassium carbonate solution is then dissolved in caustic soda, which reacts with calcium hydroxide (Ca[OH]2) to form a calcium carbonate (CaCO3) precipitate. Water is removed from the CaCO3 slurry by a clarificatory and filter press, and the precipitated CaCO3 is sent to a calcination furnace, where it is heated to about 900°C in an oxygen calcination furnace using natural gas to produce solid calcium oxide (CaO). Finally, CO2 gas can be compressed and stored indefinitely. Socolow et al. (2011) showed the cost of a liquid solvent DAC system at USD 641–819/tCO2. Meanwhile, Mazzotti et al. (2013) and Zeman (2014) estimate costs of USD 528–579/tCO2 and USD 309–580/tCO2 under optimized operation systems.
DAC technology employs a solid sorbent system and a liquid solvent. Adsorption and desorption are the two processes for capturing CO2 (National Academies of Sciences, Engineering, and Medicine [NASEM] 2019). In the adsorption process, solid sorbents from gas mixtures capture CO2 via physisorption or chemisorption (McQueen et al. 2021). Physical adsorption by intramolecular forces between CO2 molecules and the surface of solid sorbents is referred to as physisorption, whereas chemisorption is a chemical reaction in which CO2 and specific sites on the sorbent form covalent bonds. Following adsorption, heating, and vacuuming can be used to desorb CO2 from the solid sorbent. According to NASEM (2019), the net removed cost of a solid sorbent DAC system is USD 124–407/tCO2.
The third DAC system under consideration employs membrane-based gas separation. There are many different types of membrane separation, each of which can separate different gases (i.e., N2/H2, natural gas sweetening, and CO2 capture), including free-standing, hollow fiber, and spiral wound membranes that separate CO2 from natural gas (Llosa Tanco et al. 2018). Membranes must have two qualities: permeance (i.e., the passage of gases through the membrane) and selectivity (i.e., the ability to filter the desired gas from a mixture of gases).
Membrane-based DAC systems have shown potential and have some advantages over solid sorbent and liquid solvent systems, such as a smaller footprint and simpler operation (Fujikawa et al. 2021). Zanco et al. (2021) evaluated the following postcombustion DAC systems: aqueous piperazine solution absorption, Zeolite 13X adsorption in conventional fixed beds, and polymeric multistage membrane separation. Their results indicate that the absorption system is the most cost-effective for the majority of plant sizes and recovery rates; however, the membrane-based system may also become cost-effective at smaller scales in the future.
Another study(Yun et al. 2021) compared postcombustion DAC processes based on absorption and membranes for the iron and steel industry. The simulation results showed that as the concentration of CO2 in the flue gas increases, the membrane-based DAC system becomes more cost-effective than the absorption-based system. To be cost-effective for post-combustion CO2 capture, polymeric membranes must have a CO2/N2 selectivity greater than 200 while maintaining a relatively high permeability (Al-Mamoori et al. 2017).
The nanomembrane technology is a free-standing membrane system. For example, Ariyoshi et al. (2021) developed a robust hyper-permeable nanomembrane out of polydimethylsiloxane and cellulose nanofibers (PDMS–CNF). With a 17-nm thick defect-free PDMS layer of 17-nm thickness, their robust PDMS–CNF nanomembrane achieves superior permeation of 50,000 gas permeation units.
Nano membrane-based DAC systems are more scalable and can be installed in various locations. Because of its scalability, membrane-based DAC technology is also useful for DAC-U systems. Based on the performance of state-of-the-art polymer separation membranes, Fujikawa et al. (2021) demonstrated that CO2 in the air (0.04%) could be concentrated to more than 40% through multistage membrane separation. This membrane-based CO2 capture approach, representing the concept of “ubiquitous CO2 capture,” can be implemented at various sizes and scales in any location. This technology approach could become a viable method of recycling CO2 and eventually lead to a circular CO2 society.
Life Cycle Assessment of the DAC-U System
Description of the DAC-U system
The DAC-U is a functional system that captures CO2 directly from the air, enriches it 1,000 times to approximately 40% by volume, and converts it into carbon fuel methane (CH4) for use at home. The DAC-U is made up of two parts: a capture unit and a conversion unit. The capture unit uses membrane separation technology. A thermal conversion method is used for the Sabatier reaction, a methanation process, as shown in Eq. 1.
CO2 methanation is carried out with the help of a Ru-based catalyst made of aluminum oxide, CaO, and ruthenium. Due to the exothermic nature of the methanation reaction, some heat is produced during the conversion process. This heat is conducive to sustaining the thermal conversion process.