Screening of Pure ILs and DESs for CO2 Separation, N2O Separation, and H2S Separation Processes

Zhang, Yingying; Yang, Xuzhao; Han, Jingli; Tian, Junfeng; Zhang, Ting; Li, Yakun; Zhang, Jiangqiang; Shi, Yuxin; Zhang, Jingjing

doi:https://doi.org/10.1155/2023/8691957

International Journal of Chemical Engineering

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Abstract Introduction Results and Discussion Conclusions Data Availability Conflicts of Interest Acknowledgments Supplementary Materials References Copyright Related Articles

Research Article | Open Access

Volume 2023 | Article ID 8691957 | https://doi.org/10.1155/2023/8691957

Screening of Pure ILs and DESs for CO₂ Separation, N₂O Separation, and H₂S Separation Processes

Yingying Zhang,^1,2,3Xuzhao Yang ,^1,2,3Jingli Han,^1,3Junfeng Tian,¹Ting Zhang,¹Yakun Li,^1,2,3Jiangqiang Zhang,^1,2,3Yuxin Shi,¹and Jingjing Zhang¹

Academic Editor: Pedro Castano

Received21 Aug 2022

Revised27 Dec 2022

Accepted30 Dec 2022

Published18 Feb 2023

Abstract

Ionic liquids (ILs) are proposed as potential “green” solvents with remarkable properties. Deep eutectic solvents (DESs) are a new type of ILs with additional properties, such as higher biodegradability and a lower price. ILs and DESs are “green” absorbents for various gas separations, such as CO₂/N₂, CO₂/H₂/CO, H₂S/CH_4, and N₂O/N₂. Due to their large number, the screening of ILs is crucial. Although ILs with high absorption capacities were screened using gas solubility and selectivity, it is important to consider the energy and solvents used in the process. In this paper, the absorbent amount and the energy consumption were used for screening absorbents for various gas separation processes. The results reveal that physical IL [Bmim][DCA] and chemical IL [Eeim][Ac] are screened for CO₂/N₂ and CO₂/H₂/CO separation, physical IL [Omim][PF₆] for H₂S/CH₄ separation, and physical IL [P₆₆₆₁₄][eFAP] for NO/N₂ separation. The screened ILs offer some advantages over commercial absorbents in terms of lower energy consumption or amount.

1. Introduction

Every year, large amounts of gases are emitted into the atmosphere, with CO₂ being the primary greenhouse gas [1, 2], N₂O having a potential impact on global warming that is 310 times greater than that of CO₂ [3], and H₂S being one of the highest sulfur-containing compounds. Excess emissions of CO₂ and N₂O result in global warming and climate change, while H₂S emissions result in acid rain. Therefore, it is necessary to identify effective measures to mitigate the emission of CO₂, N₂O, and H₂S from different sources.

Carbon capture and storage (CCS) can be used to reduce CO₂ emissions. Meanwhile, biomass syngas from biomass gasification is used in transportation as biofuels. CO₂ separation is required for CCS and biomass syngas purification. The current CO₂ separation technologies have several shortcomings, such as high energy consumption [4], corrosion degradation, and/or large-scale operations, which affect removal efficiency.

The primary sources of anthropogenic N₂O emissions are nylon production, nitric acid production, and vehicle exhaust emissions. Many N₂O emission reduction technologies have been developed, such as thermal decomposition and catalytic decomposition. However, they may be constrained by the large energy consumption and increasing CO₂ emissions.

There are several technologies for H₂S separation, such as absorption, oxidation, and adsorption [5]. Absorption technology is extensively used for H₂S separation, whereas aqueous alkanolamine solutions are currently employed in industrial natural gas treatment and sweetening plants [6]. However, the application of H₂S absorption technology is impacted, similar to CO₂ separation, by intensive energy consumption and/or large-scale operations.

Therefore, new gas separation processes for CO₂, N₂O, and H₂S must be developed to curb climate change and protect the environment. Ionic liquids exhibit remarkable properties for gas separation, such as high solubility for CO₂, N₂O, and H₂S. Although ILs have been used in studies related to gas separation [7–10], the large-scale commercial usage of ILs is limited by their high toxicity, poor biodegradability, and high cost. Deep eutectic solvents have low toxicity, biodegradability, and low cost and are proposed as promising CO₂ absorbents [11–14].

In our previous work, Gibbs free energy change (∆G) was employed to evaluate the performance of solvents [15, 16] for separating CO₂ from biogas and NH₃ from synthetic ammonia purge gas [17]. However, the effective absorbents for various gas streams with different conditions were not determined. In this study, thermodynamic analysis was utilized for gas separation using pure ILs and DESs. For CO₂ streams, effluent gases, kiln gas, and biomass syngas were chosen. For the H₂S stream, high-sulfur natural gas was chosen. For the N₂O stream, adipic acid off-gas was chosen. For various gas streams, several absorbents were screened as potential gas absorbents. Furthermore, the relationship between the performances, the properties, and the critical properties of gas streams was investigated. All of these are employed in the development of new gas separation technologies.

2. Gas Separation and Thermodynamic Model

2.1. Gas Streams

In this work, effluent gases were chosen as CO₂ streams due to their large emission amounts and low CO₂ concentration, whereas kiln gas was chosen due to its high CO₂ concentration. Biomass syngas is chosen as the CO₂ stream for CO₂/CO/H₂. The high-sulfur natural gas is used as the H₂S stream for H₂S/CH₄, and the adipic acid off-gas is used as the N₂O stream for N₂O/N₂. Table 1 lists the typical conditions of different gas streams.

2.2. Gas Separation Process

The gas separation process using liquid absorbents is shown in Figure 1. The absorbent quantity (m_abs, g abs·g X⁻¹) can be calculated using the following equation:where M_abs and M_x are the molecular weights of the absorbent and X gas, respectively, and g·mol⁻¹. x_a and x_s are the molar ratios of the X gas in the absorption tower and desorber, respectively.

The energy consumption required in the gas separation process can be calculated as shown inwhere n_x denotes the molecular weight of the X gas in moles. H_x denotes the Henry constant of X gas in the absorbents in bar units. P_a and P₁ denote the pressure of the absorption tower and the initial pressure, respectively, in bar units. C_{p, abs} represents the isobaric heat capacities of the absorbents in J·mol⁻¹·K⁻¹. T_a and T_s denote the temperatures of the absorption tower and desorber, respectively.

2.3. Theory

In thermodynamics, ∆G was used as the evaluation criteria to determine if the isothermal reversible process was spontaneous. As shown in Figure 2, the separation process is nonspontaneous, and the Gibbs free energy change for System 1 is above zero (∆G₁ > 0). Six reversible processes were designed, and the summation is represented as ∆G₂ for Surrounding 2. System 3 is composed of System 1 and Surrounding 2. Moreover, the addition of energy and absorbents causes ∆G₂ to be negative. In Figure 2, ∆G_comp represents the isothermal reversible compression process, ∆G_abs represents the reversible absorption process of X absorption, ∆G_T represents the reversible adiabatic expansion and reversible temperature increasing process of the solution, ∆G_des represents the reversible X gas desorption process, ∆G_exp represents the isothermal reversible expansion of the other gas, and ∆G_T’ represents the reversible adiabatic expansion and the reversible isothermal compression of the X gas. The optimal operating conditions are achieved when ∆G₃ is equal to 0, and the performance of different absorbents can be evaluated. Therefore, using the thermodynamic analysis as proposed in our previous work, the number of absorbents and the energy consumption are combined by Gibbs free energy change [12, 13].

∆G for different systems and processes can be calculated using the equations given in equations (3)–(10).where n is the number of moles in the gas stream, and y_i represents the molar fraction of component i in the stream.where and are the G values of the gaseous component i at (T, P) and (T_a, P_a), respectively, and they are calculated using the formula G = H − TS. The NIST standard reference database provides the values of H and S for the gas components.where H_x denotes Henry’s constant and K_x denotes the chemical reaction constant of X gas in absorbents.where Δ_fH_j, 298.15 K represents the standard enthalpy change in the formation of j in the absorbents at 298.15 K; S_j (298.15 K) represents the standard molar entropy of j at 298.15 K; and C_p,j represents the isobaric heat capacity of j in the absorbents.where y_x is the mole fraction of X gas in the gas stream, (T_a,y_xP_a) is the G value of the gaseous component i at (T_a, y_xP_a).where is the G value of the gaseous component i at (T_s, P_s).

3. The Properties of Absorbents

The properties of liquid absorbents, including Henry’s law constants of different gases in ILs/DESs, reaction equilibrium constants, the density of ILs/DESs at 298.15 K, and the heat capacity of the ILs/DESs, have been collected and listed in Table 2. In conventional ILs/DESs, the uncertainty in Henry’s law constants of CO₂, H₂S, and N₂O was estimated to be ±8 bar, ±0.4 bar, and ±0.07 bar, respectively. Henry’s law constants and reaction equilibrium constants were correlated for some physical ILs and the chemical ILs/DESs as per the CO₂ solubility data described in our previous work [11]. The uncertainties in the densities and the heat capacities of the conventional ILs/DESs were ±63 J·mol⁻¹·K⁻¹ and ±13 g·cm⁻³, respectively, based on the experimental data presented in Table 2. The names and molar weights of absorbents are listed in Appendix A (Supplementary data available here).

4. Results and Discussion

The desorption temperatures of absorbents in this study are identical to those in our previous work [12], which are 299.15–323.15 K for physical absorbents, 299.15–345.15 K, and 299.15–353.15 K for chemical DES and ILs, respectively. The absorption pressure is iterated until ∆G₃ = 0, and the optimal conditions, absorbent amount, and energy consumption are obtained.

4.1. Analysis of Gas Absorbents

4.1.1. Absorption Pressure

As shown in Figures 3 and 4, [BmPy][FAP] represents the minimum P_a, which is 16.16–87.77 bar, 8.75–45.65 bar, and 7.66–44.98 bar in 299.15–323.15 K for effluent gases, kiln gas, and biomass syngas, respectively. Among the four chemical absorbents that were analyzed, [Eeim][Ac] exhibits the lowest absorption pressures for the three CO₂ streams, with values of 70.60–137.96 bar, 36.00–74.44 bar, and 41.98–123.37 bar within 315.15–345.15 K, respectively. Among the ten physical absorbents that were analyzed for N₂O/N₂ separation, [Omim][PF₆] exhibits the lowest value of P_a in the temperature range of 299.15–323.15 K with pressure values in the range of 3.97–13.49 bar. [Bmim][FAP] exhibits the lowest P_a within 299.15–323.15 K with values of 4.40–22.25 bar among the eight physical ILs that were analyzed for H₂S/CH₄ separation.

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(b)

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As illustrated in Figure 3, the absorption pressures of different CO₂ absorbents in physical absorbents are greater than those of chemical ILs/DES for CO₂ streams. For the same IL [Bmim][BF₄], the absorption pressures for different gas streams are as follows: effluent gases ( = 0.12) > kiln gas = 0.25) > adipic acid off-gas ( = 0.45) > biomass syngas ( = 0.3) > biogas ( = 0.4) > high-sulfur natural gas ( = 0.32) > synthetic ammonia purge gas ( = 0.45). The key factors influencing the absorption pressure are gas concentration and gas solubility in absorbents. The absorption pressures increase with increasing gas concentrations in the gas stream and decreasing gas solubilities. Meanwhile, the absorption pressure shows an increasing trend as gas solubility decreases. Due to the low solubility of N₂O in [Bmim][BF₄], adipic acid off-gas exhibits a higher absorption pressure than biomass syngas. However, due to the high concentration of H₂S, high-sulfur natural gas shows a lower absorption pressure than biogas.

4.1.2. Amount of Absorbent

Figures 5 and 6 show the absorbent amounts. As the desorption temperature rises, the amount of absorbents decreases, especially at low desorption temperatures.

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The physical [Bmim][DCA] exhibits the lowest amount with values of 44.22–11.15 g·gCO₂⁻¹, 36.60–9.62 g·gCO₂⁻¹, and 32.26–6.84 g·gCO₂⁻¹ within the range of 300.15–323.15 K for effluent gases, kiln gas, and biomass syngas, respectively, in the 30 physical absorbents. The chemical Ch[Pro]/PEG200 (1 : 2) represents the minimum values of m_abs, which are 13.39–5.62 g·gCO₂⁻¹, 14.60–4.63 g·gCO₂⁻¹, and 9.35–1.44 g·gCO₂⁻¹ in 315.15–345.15 K, respectively. [P₆₆₆₁₄][FAP] and [Omim][PF₆] exhibited the lowest amount with values of 104.59–6.71 g·gN₂O⁻¹ and 4.72–14.74 g·gH₂S⁻¹ for adipic acid off-gas and high-sulfur natural gas, respectively, within the range of 300.15–323.15 K.

Due to differences in CO₂ solubility, the amounts of CO₂ absorbents follow the order of chemical absorbents < physical absorbents. Generally, the solubility of CO₂ in chemical absorbents is greater than that in physical absorbents. For different CO₂ streams with the same absorbents, the quantity has the following order: high-sulfur natural gas ( = 0.32) > synthetic ammonia purge gas ( = 0.45) > effluent gases ( = 0.12) > kiln gas ( = 0.25) > biomass syngas ( = 0.3) > biogas ( = 0.4) > adipic acid off-gas ( = 0.45). The major reason for the significant amount of absorbents is the high gas solubility in high-sulfur natural gas and synthetic ammonia purge gas.

4.1.3. Energy Consumption

In Figures 7 and 8, the energy consumption is displayed. The energy consumption increases with an increase in the desorption temperature. The physical [Hmpy][NTf₂] displays the lowest Q_tot for the CO₂ separation process in the 30 physical absorbents, with values of 1.94–2.87 GJ·ton CO₂⁻¹, 1.02–1.49 GJ·ton CO₂⁻¹ and 0.89–1.21 GJ·ton CO₂⁻¹ for effluent gases, kiln gas, and biomass syngas, respectively, within the range of 299.15–323.15 K. The chemical [Eeim][Ac] exhibits the lowest energy consumption in the four chemical absorbents, with values of 2.48–3.70 GJ·ton CO₂⁻¹, 1.40–2.27 GJ·ton CO₂⁻¹, and 1.24–1.92 GJ·ton CO₂⁻¹ respectively, within 303.15–345.15 K. The physical IL [Omim][PF₆] exhibits the lowest energy consumption for the separation of H₂S from high-sulfur natural gas in the 10 physical ILs, with values of 1.05–1.44 GJ·ton H₂S⁻¹ within 299.15–323.15 K for high-sulfur natural gas. [P₆₆₆₁₄][FAP] shows the lowest energy consumption for N₂O separation in the 8 physical ILs, with values of 0.65–0.95 GJ·ton H₂S⁻¹ within 299.15–323.15 K for adipic acid off-gas.

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Due to the high heat of chemical absorbents, the energy consumption of chemical absorbents is larger than that of physical absorbents. The CO₂ concentrations have an impact on the energy consumption for various CO₂ streams. The energy consumption sequence is as follows: effluent gases ( = 0.12) > synthetic ammonia purge gas ( = 0.45) > kiln gas ( = 0.25) > biomass syngas ( = 0.3) > high-sulfur natural gas ( = 0.32) > biogas ( = 0.4) > adipic acid off-gas ( = 0.45). The energy consumption for separating CO₂ from effluent gases (CO₂/N₂) is the largest due to the low CO₂ molar ratio, and the energy consumption for separating N₂O from adipic acid off-gas is the lowest due to the highest N₂O solubility and a high amount of absorbents.

4.2. Screening Absorbents

The screening criteria for absorbents include both absorbent amounts (m_abs) and energy consumption (Q_tot). The physical [Bmim][DCA] was screened between 299.15–323.15 K with low amounts of the absorbent (<190 g·gCO₂⁻¹ for effluent gases, <150 g·gCO₂⁻¹ for kiln gas, <140 g·gCO₂⁻¹ for biomass syngas) and low energy consumption (<2 GJ·tonCO₂⁻¹ for effluent gases, <1 GJ·tonCO₂⁻¹ for kiln gas, <0.9 GJ·tonCO₂⁻¹ for biomass syngas). The chemical [Eeim][Ac] was screened with a lower amount of ILs (<43 g·gCO₂⁻¹ for effluent gases at 303.15–345.15 K, <142 g·gCO₂⁻¹ for kiln gas at 299.15–345.15 K, <68 g·gCO₂⁻¹ for biomass syngas at 300.15–345.15 K). A lower amount of ILs (<293 g·gH₂S⁻¹) was used to screen [Omim][PF₆] for high-sulfur natural gas at 299.15–323.15 K. A lower amounts of ILs (<108 g·gN₂O⁻¹) was used to screen [P₆₆₆₁₄][FAP] for adipic acid off-gas at 299.15–323.15 K. The uncertainties of Henry’s law constant, heat capacity, and density were taken into consideration while estimating the uncertainties in the iterated results. The uncertainties in the absorption pressure, the required amount of ILs, and the energy expended for CO₂ separation were estimated to be ±3.97 bar, ±2.47 g·gCO₂⁻¹, and ±0.09 GJ·tonCO₂⁻¹, respectively. The uncertainties in the absorption pressure, the required amount of ILs, and the energy expended for H₂S separation were estimated to be ±0.41 bar, ±0.37 g·gH₂S⁻¹, and ±0.003 GJ·tonH₂S⁻¹, respectively. The uncertainties in the absorption pressure, the required amount of ILs, and the energy used for N₂O separation were estimated to be ±0.12 bar, ±0.17 g·gN₂O⁻¹, and ±0.04 GJ·tonN₂O⁻¹, respectively. Table 3 lists the screened absorbents and their values of T_s, P_a, m_abs, and Q_tot.

4.3. Comparison with Commercial Absorbents

The superiority of the screened absorbents is demonstrated by comparisons with commercial absorbents. For CO₂ separation, the chemical [Eeim][Ac] in this study is compared with 30% MEA and 30% MDEA. [Bmim][DCA] is compared with DEPG for CO₂ separation. Furthermore, for H₂S separation, [Omim][PF₆] is compared with water. The findings of P_a, m_abs, and Q_tot of commercial absorbents for gas separation from effluent gases, kiln gas and biomass syngas, biogas, high-sulfur natural gas, and adipic acid off-gas are displayed in Table 4 with the set desorption temperature.

The results of m_abs and Q_tot for [Bmim][DCA] and DEPG are displayed in Figures 9 and 10. Figure 11 displays the predicted results of m_abs and Q_tot for chemical [Eeim][Ac] at 338.15 K, 30 wt% MEA at 393.15 K, and 30 wt% MDEA at 393.15 K.

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Based on the comparisons of the performances of physical absorbents for CO₂ separation shown in Figures 9 and 10, both energy consumption and the amount required for DEPG are lower than those of [Bmim][DCA] when P_a is 12.5 bar and 25 bar, respectively. This suggests that the performance of the screened ILs is not superior to that of commercial physical absorbents for DEPG. Based on the comparison of the performances of chemical absorbents for CO₂ streams in Figure 11, [Eeim][Ac] displays a larger absorbent amount and lower energy consumption than those of 30 wt% MDEA and 30 wt% MEA. Assuming that the cost of [Eeim][Ac] is high, the screening of chemical ILs for CO₂ separation must be further researched. However, the volatility of [Eeim][Ac] can be ignored.

From the comparison of the performances of physical absorbents for the H₂S stream in Figure 12, [Omim][BF₄] exhibited higher energy consumption and a lower amount of absorbents. The comparison of [Omim][BF₄] and DEPG shows that the performance of physical IL is not superior to that of DEPG. The screened ILs have the advantage of low energy consumption and nonvolatility, although they have a higher amount than chemical CO₂ absorbents (30 wt% MDEA and 30 wt% MEA). The physical H₂S absorbent consumes less energy than water.

The cost of conventional ILs is significantly higher than that of commercial CO₂ absorbents when operational costs and solvent costs are considered. For instance, the estimated costs of water, DEPG, MEA, and MDEA were estimated to be 0.3 × 10⁻³ US$·kg⁻¹ [134], 3.5 US$·kg⁻¹ [135], 1.25–2.25 US$·kg⁻¹ [136, 137], and 20 US$·kg⁻¹ [138], respectively, while the cost of the used commercial ILs was estimated as 6–13.5 US$·kg⁻¹ [136]. Both the price and the amount needed of conventional ILs are higher than those of commercial gas absorbents; therefore, the advantages of ILs are located at nonvolatility, low energy use for chemical absorbents, and nondegradability. It is needed to develop process simulation with consideration of solvent degradation to compare conventional ILs and commercial gas absorbents. Furthermore, with technological advancement, the cost of ILs will drop, and the cost difference between conventional ILs and commercial absorbents will reduce.

5. Conclusions

In this study, green absorbents were analyzed based on ∆G to screen the absorbents for CO₂ separation from effluent gases, kiln gas, and biomass syngas; H₂S separation from high-sulfur natural gas (H₂S/CH₄); and N₂O separation from adipic acid off-gas (N₂O/N₂).

[Bmim][DCA] and [Eeim][Ac] were screened for CO₂ separation using m_abs and Q_tot as criteria. [Omim][PF₆] and [P₆₆₆₁₄][FAP] were screened for H₂S separation and N₂O separation, respectively. According to comparisons between the screened absorbents and the DEPG, the physical IL has a higher energy consumption and higher m_abs than the DEPG. When compared with 30 wt% MDEA and 30 wt% MEA, the chemical IL has a lower Q_tot and is involatile. Lower energy consumption and a higher amount of H₂S separation were observed when screened [Omim][BF₄] was compared to H₂O.

Due to the differences in gas concentration in gas streams and gas solubility in absorbents, the amount of absorbents has the following order: high-sulfur natural gas > synthetic ammonia purge gas > effluent gases > kiln gas > biomass syngas > biogas > adipic acid off-gas. The order of energy consumption is as follows: effluent gases > synthetic ammonia purge gas > kiln gas > biomass syngas > high-sulfur natural gas > biogas > adipic acid off-gas.

Data Availability

The data used to support the findings of this study are from previously reported studies and datasets, which are cited in the article. The enthalpy and entropy of gas components are available and can be found at NIST Standard Reference Data (https://webbook.nist.gov/chemistry/fluid/).

Conflicts of Interest

The authors declare that they have no conflicts of interest.

Acknowledgments

This work was supported by the Scientific and Technological Key Project in Henan Province (grant no. 22A530004), Ph.D. Research Startup Foundation of the Zhengzhou University of Light Industry (grant nos. 2017BSJJ029 and 2020BSJJ018), and the National College Students’ Innovation and Entrepreneurship Training Program (grant no. 202210462074).

Supplementary Materials

Appendix A: supplementary data associated with this article. (Supplementary Materials)

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