2016 Vol. 1, No. 3

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Editorial
CO2 capture: Challenges and opportunities
Liyuan Deng, Hanne Kvamsdal
2016, 1(3) doi: 10.1016/j.gee.2016.12.002
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Feature article
The European Carbon dioxide Capture and Storage Laboratory Infrastructure (ECCSEL)
Sverre Quale, Volker Rohling
2016, 1(3): 180-194. doi: 10.1016/j.gee.2016.11.007
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The transition to a non-emitting energy mix for power generation will take decades. This transition will need to be sustainable, e.g. economically affordable. Fossil fuels which are abundant have an important role to play in this respect, provided that Carbon Capture and Storage (CCS) is progressively implemented. CCS is the only way to reduce emissions from energy intensive industries. Thus, the need for upgraded and new CCS research facilities is widely recognised among stakeholders across Europe, as emphasised by the Zero Emissions Platform (ZEP) [1] and the European Energy Research Alliance on CCS (EERA-CCS) [2]. The European Carbon Dioxide Capture and Storage Laboratory Infrastructure, ECCSEL, provides funders, operators and researchers with significant benefits by offering access to world-class research facilities that, in many cases, are unlikely for a single nation to support in isolation. This implies creation of synergy and the avoidance of duplication as well as streamlining of funding for research facilities. ECCSEL offers open access to its advanced laboratories for talented scientists and visiting researchers to conduct cutting-edge research. In the planning of ECCSEL, gap analyses were performed and CCS technologies have been reviewed to underpin and envisage the future experimental setup; 1) Making use of readily available facilities, 2) Modifying existing facilities, and 3) Planning and building entirely new advanced facilities. The investments required for the first ten years (2015–2025) are expected to be in the range of €80–120 million. These investments show the current level of ambition, as proposed during the preparatory phase (2011–2014). Entering the implementation phase in 2015, 9 European countries signed Letter of Intent (LoI) to join a ECCSEL legal entity: France, United Kingdom, Netherlands, Italy, Spain, Poland, Greece, Norway and Switzerland (active observer). As the EU ERIC-regulation [3] would offer the most suitable legal framework for ECCSEL, the host country, Norway, will apply for establishing ERIC as the ECCSEL Research Infrastructure (RI) legal entity in 2017. Until the ECCSEL ERIC is approved by the European Commission (probably by summer 2017), an interim MoU agreement for the implementation phase of ECCSEL RI has been signed by 13 research institutions and universities representing the 9 countries. A consortium of these partners were granted 3 million EURO from Horizon 2020 to boost implementation of ECCSEL from September 2015 and two years onwards.
Research paper
Solubilities of CO2, CH4, H2, CO and N2 in choline chloride/urea
Yujiao Xie, Haifeng Dong, Suojiang Zhang, Xiaohua Lu, Xiaoyan Ji
2016, 1(3): 195-200. doi: 10.1016/j.gee.2016.09.001
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Solubilities of CO2, CH4, H2, CO and N2 in choline chloride/urea (ChCl/Urea) were investigated at temperatures ranging from 308.2 to 328.2 K and pressures ranging from 0.6 to 4.6 MPa. The results show that the solubilities of gases increase with increasing pressure and decreasing temperature. The solubility of CO2 is higher than that of CH4, H2, CO and N2, which indicates that ChCl/Urea may be used as a potential solvent for CO2 capture from the gas mixture. Solubility of CO2 in ChCl/Urea was fitted by Non-Random Two-Liquid and Redlich–Kwong (NRTL-RK) model, and solubility of CH4, H2, CO or N2 in ChCl/Urea was fitted by Henry's Law. The standard enthalpy, standard Gibbs energy and standard entropy of gases were calculated. Additionally, the CO2/CH4 selectivities in water, dry ChCl/Urea and aqueous ChCl/Urea were further discussed.
The effect of humidity on the CO2/N2 separation performance of copolymers based on hard polyimide segments and soft polyether chains: Experimental and modeling
Luca Olivieri, Alberto Tena, Maria Grazia De Angelis, Antonio Hernández Giménez, Angel E. Lozano, Giulio Cesare Sarti
2016, 1(3): 201-210. doi: 10.1016/j.gee.2016.09.002
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In this work, we studied two copolymers formed by segments of a rubbery polyether (PPO or PEO) and of a glassy polyimide (BPDA-ODA or BKDA-ODA) suitable for gas separation and CO2 capture. Firstly, we assessed the absorption of water vapor in the materials, as a function of relative humidity (R.H.), finding that the humidity uptake of the copolymers lies between that of the corresponding pure homopolymers values. Furthermore, we studied the effect of humidity on CO2 and N2 permeability, as well as on CO2/N2 selectivity, up to R.H. of 75%. The permeability decreases with increasing humidity, while the ideal selectivity remains approximately constant in the entire range of water activity investigated. The humidity-induced decrease of permeability in the copolymers is much smaller than the one observed in polyimides such as Matrimid® confirming the positive effect of the polyether phase on the membrane performance. Finally, we modeled the humidity-induced decrease of gas solubility, diffusivity and, consequently, permeability, using a suitable approach that considers the free volume theory for diffusion and LF model for solubility. Such model allows estimating the extent of competition that the gases undergo with water during sorption in the membranes, as a function of the relative humidity, as well as the expected reduction of free volume by means of water molecules occupation and consequent reduction of diffusivity.
Integration of multi-stage membrane carbon capture processes to coal-fired power plants using highly permeable polymers
Maria-Chiara Ferrari, Davide Bocciardo, Stefano Brandani
2016, 1(3): 211-221. doi: 10.1016/j.gee.2016.10.001
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Membrane separation systems could be a feasible option as post combustion carbon capture technologies in coal-fired power plants. Recent advancement on membrane materials based on microporous super glassy polymers could improve significantly the capture process but the properties of the materials have to guide the design of the separation stage. In this study an advanced hybrid two-stage membrane process employing one of the most permeable polymer known (PIM-1) is retrofitted to a coal fired power plant and the process is analysed in terms of energy requirement and cost performance. The results are based on the use of an in-house detailed membrane module model implemented in UniSim Design®, the Honeywell process flowsheet simulator. The study indicates the need for advanced configuration in order for highly permeable membranes to be competitive with more mature technologies in terms of capture cost. The effect of ageing and impurities on the material is also investigated in order to predict the decline in process performance over time and suggest a timeproof design.
Techno-economical evaluation of membrane based biogas upgrading system: A comparison between polymeric membrane and carbon membrane technology
Shamim Haider, Arne Lindbråthen, May-Britt Hägg
2016, 1(3): 222-234. doi: 10.1016/j.gee.2016.10.003
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A shift to renewable energy sources will reduce emissions of greenhouse gases and secure future energy supplies. In this context, utilization of biogas will play a prominent role. Focus of this work is upgrading of biogas to fuel quality by membrane separation using a carbon hollow fibre (CHF) membrane and compare with a commercially available polymeric membrane (polyimide) through economical assessment. CHF membrane modules were prepared for pilot plant testing and performance measured using CO2, O2, N2. The CHF membrane was modified through oxidation, chemical vapour deposition (CVD) and reduction process thus tailoring pores for separation and increased performance. The post oxidized and reduced carbon hollow fibres (PORCHFs) significantly exceeded CHF performance showing higher CO2 permeance (0.021 m3(STP)/m2 h bar) and CO2/CH4 selectivity of 246 (5 bar feed vs 50 mbar permeate pressure). The highest performance recorded through experiments (CHF and PORCHF) was used as simulation basis. A membrane simulation model was used and interfaced to 8.6 V Aspen HYSYS. A 300 Nm3/h mixture of CO2/CH4 containing 30–50% CO2 at feed pressures 6, 8 and 10 bar, was simulated and process designed to recover 99.5% CH4 with 97.5% purity. Net present value (NPV) was calculated for base case and optimal pressure (50 bar for CHF and PORCHF). The results indicated that recycle ratio (recycle/feed) ranged from 0.2 to 10, specific energy from 0.15 to 0.8 () and specific membrane area from 45 to 4700 (). The high recycle ratio can create problems during start-up, as it would take long to adjust volumetric flow ratio towards 10. The best membrane separation system employs a three-stage system with polyimide at 10 bar, and a two-stage membrane system with PORCHF membranes at 50 bar with recycle. Considering biomethane price of 0.78 $/Nm 3 and a lifetime of 15 years, the techno-economic analysis showed that payback time for the best cascade is 1.6 months.
High-permeance crosslinked PTMSP thin-film composite membranes as supports for CO2 selective layer formation
Stepan D. Bazhenov, Ilya L. Borisov, Danila S. Bakhtin, Anastasia N. Rybakova, Valery S. Khotimskiy, Sergey P. Molchanov, Vladimir V. Volkov
2016, 1(3): 235-245. doi: 10.1016/j.gee.2016.10.002
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In the development of the composite gas separation membranes for post-combustion CO2 capture, little attention is focused on the optimization of the membrane supports, which satisfy the conditions of this technology. The primary requirements to the membrane supports are concerned with their high CO2 permeance. In this work, the membrane supports with desired characteristics were developed as high-permeance gas separation thin film composite (TFC) membranes with the thin defect-free layer from the crosslinked highly permeable polymer, poly[1-(trimethylsilyl)-1-propyne] (PTMSP). This layer is insoluble in chloroform and can be used as a gutter layer for the further deposition of the СО2-selective materials from the organic solvents. Crosslinking of PTMSP was performed using polyethyleneimine (PEI) and poly (ethyleneglycol) diglycidyl ether (PEGDGE) as crosslinking agents. Optimal concentrations of PEI in PTMSP and PEGDGE in methanol were selected in order to diminish the undesirable effect on the final membrane gas transport characteristics. The conditions of the kiss-coating technique for the deposition of the thin defect-free PTMSP-based layer, namely, composition of the casting solution and the speed of movement of the porous commercial microfiltration-grade support, were optimized. The procedure of post-treatment with alcohols and alcohol solutions was shown to be crucial for the improvement of gas permeance of the membranes with the crosslinked PTMSP layer having thickness ranging within 1–2.5 μm. The claimed membranes showed the following characteristics: CO2 permeance is equal to 50–54 m3(STP)/(m2 h bar) (18,500–20,000 GPU), ideal CO2/N2 selectivity is 3.6–3.7, and their selective layers are insoluble in chloroform. Thus, the developed high-permeance TFC membranes are considered as a promising supports for further modification by enhanced CO2 selective layer formation.
Thermodynamic modelling of unloaded and loaded N,N-diethylethanolamine solutions
Monica Garcia, Hanna K. Knuutila, Sai Gu
2016, 1(3): 246-257. doi: 10.1016/j.gee.2016.11.003
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Chemical absorption is a crucial step for several chemical processes such as ammonia production, coal gasification, methane reforming, ethylene oxide manufacturing and treatment of associated gas streams [1]. It is considered one of the main processes to eliminate CO2 emissions from power plants by post-combustion. Use of new solvents are of high interest in chemical absorption for carbon capture. For the design of the absorption and desorption columns it is essential to know the vapour–liquid equilibrium (VLE), heat of absorption and densities. N,N-diethylethanolamine (DEEA) appeared as one of the amines with the lowest amount of energy needed for its regeneration [2], which would directly decrease the operation costs. DEEA has a high CO2 loading of 1 mol/mol of amine compared to the traditional MEA solvent (0.5 mol/mol amine) and is obtained from renewable sources [1]. The main weakness is its low absorption rate and consequently the use of promoters is desirable. In this work, a thermodynamic model based on the electrolyte non-random two-liquid theory (eNRTL) was created and fitted to correlate and predict the partial and total pressures of the unloaded and loaded aqueous DEEA solutions. New interaction parameters were obtained for the binary and tertiary system. This model represents the vapour pressures of the pure components, DEEA and H2O, with AARD of 1.9% and 1.73% respectively. Furthermore, the fitted model predicts the total pressure above the binary system, H 2O-DEEA, with AARD of 0.05%. The excess of enthalpy and densities are predicted with AARD of 5.63% and 1.38% respectively. The tertiary system, H2O-DEEA-CO2, is fitted for 2 M and 5 M DEEA solutions with loading between 0.042 and 0.9 mol CO2/mol amine up to 80 °C. Results of CO2 partial pressures and total pressures are reproduced, with AARD of 19.45% and 16.18% respectively. Densities are predicted with an AARD of 1.52%.
Simultaneous measurement of CO2 sorption and swelling of phosphate-based ionic liquid
Junfeng Wang, Camille Petit, Xiangping Zhang, Ah-Hyung Alissa Park
2016, 1(3): 258-265. doi: 10.1016/j.gee.2016.11.004
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The development of alternative CO2 capture solvents such as ionic liquids (ILs) and nanoparticle organic hybrid materials (NOHMs) have provided interesting options for CO2 capture. In this study, CO2 interactions with 1,3-dimethylimidazolium dimethylphosphate ([MMIM]DMP), 1-ethyl-3-methylimidazolium dimethylphosphate ([EMIM]DMP) and 1-ethyl-3-methylimidazolium diethylphosphate ([EMIM]DEP) that contain inorganic ester groups based on phosphate, were investigated using ATR FT-IR spectroscopy. CO2-induced swelling, CO2 diffusivity and CO2 capture capacity were simultaneously measured to identify CO2 capture mechanisms, kinetics and diffusion behaviors as a function of the alkyl chain length of the cation. Henry's law constants of CO2 were found to be in the range of 4–11 MPa, which is in agreement with those reported in other studies.
Modelling of a tubular membrane contactor for pre-combustion CO2 capture using ionic liquids: Influence of the membrane configuration, absorbent properties and operation parameters
Zhongde Dai, Muhammad Usman, Magne Hillestad, Liyuan Deng
2016, 1(3): 266-275. doi: 10.1016/j.gee.2016.11.006
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A membrane contactor using ionic liquids (ILs) as solvent for pre-combustion capture CO2 at elevated temperature (303–393 K) and pressure (20 bar) has been studied using mathematic model in the present work. A comprehensive two-dimensional (2D) mass-transfer model was developed based on finite element method. The effects of liquid properties, membrane configurations, as well as operation parameters on the CO2 removal efficiency were systematically studied. The simulation results show that CO2 can be effectively removed in this process. In addition, it is found that the liquid phase mass transfer dominated the overall mass transfer. Membranes with high porosity and small thickness could apparently reduce the membrane resistance and thus increase the separation efficiency. On the other hand, the membrane diameter and membrane length have a relatively small influence on separation performance within the operation range.

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