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A special issue of Applied Sciences (ISSN 2076-3417). This special issue belongs to the section "Chemical and Molecular Sciences".

Deadline for manuscript submissions: closed (15 July 2018) | Viewed by 66455

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Prof. Dr. Angel Irabien

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Catedrático de Universidad/Chemical Engineering Professor/Head of Department, Departamento de Ingenierías Química y Biomolecular /Department of Chemical and Biomolecular Engineering, UNIVERSIDAD DE CANTABRIA/UNIVERSITY OF CANTABRIA, ETS de Ingenieros Industriales y de Telecomunicación, Avda. de los Castros, s/n. 39005 Santander, Spain
Interests: chemical engineering; siustainable chemistry and engineering; carbon capture and utilization

Dr. Clara Casado-Coterillo

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Department of Chemical and Biomolecular Engineering, University of Cantabria, Av. Los Castros s/n, 39005 Santander, Spain
Interests: synthesis; characterization; CO₂ capture and utilization; mixed matrix membranes; pervaporation; sustainable process intensification using membranes
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Special Issue Information

Dear Colleagues,

In the last few years, the greenhouse gas concentration in the atmosphere has increased. Carbon dioxide is considered one of the major contributors to greenhouse effects and climate change. In order to reduce CO₂ emissions, and the industry dependence on fossil fuels, it is necessary to develop technologies that combine capture and valorization processes to an adequate purity. Membrane technology has attracted extensive research and development as alternative clean CO₂ capture processes. Regarding the valorization of CO₂, electrochemical reduction of CO₂ has been studied recently at the laboratory scale as a potential means of converting CO₂ from flue gases to high added value chemicals and fuels. This Special Issue thus serves the need to promote exploratory research and development on CO₂ capture and utilization techniques, while addressing their challenges from a sustainable perspective.

Prof. Dr. Angel Irabien
Dr. Clara Casado-Coterillo
Guest Editors

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Keywords

CO₂ capture
CO₂ utilization
CO₂ storage

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Published Papers (10 papers)

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20 pages, 3060 KiB

Open AccessArticle

Optimization in the Absorption and Desorption of CO₂ Using Sodium Glycinate Solution

by Pao Chi Chen and Sheng-Zhong Lin

Appl. Sci. 2018, 8(11), 2041; https://doi.org/10.3390/app8112041 - 24 Oct 2018

Cited by 22 | Viewed by 3788

Abstract

This study used sodium glycinate as an absorbent to absorb CO₂ in the bubble column scrubber under constant pH and temperature environments to obtain the operating range, CO₂ loading, and mass transfer coefficient. For efficient experimentation, the Taguchi method is used for the experimental design. The process parameters are the pH, gas flow rate (Q_g), liquid temperature (T), and absorbent concentration (C_L). The effects of the parameters on the absorption efficiency, absorption rate, overall mass transfer coefficient, gas–liquid molar flow rate ratio, CO₂ loading, and absorption factor are to be explored. The optimum operating conditions and the order of parameter importance are obtained using the signal/noise (S/N) ratio analysis, and the optimum operating conditions are further verified. The verification of the optimum values was also carried out. The order of parameter importance is pH > C_L > Q_g > T. Evidence in the ¹³CNMR (Carbon 13 Nuclear Magnetic Resonance) spectra shows that the pH value has an effect on the solution composition, which affects both the absorption efficiency and mass transfer coefficient. There are 18 experiments for regeneration, where the operating temperature is 100–120 °C. The heat of regeneration was measured according to the thermodynamic data. The CO₂ loading, the overall mass transfer, and the heats of regeneration correlation are also discussed in this work. Finally, an operating policy for the CO₂ absorption process was confirmed. Full article

(This article belongs to the Special Issue Carbon Capture Utilization and Sequestration (CCUS))

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12 pages, 2253 KiB

Open AccessArticle

Enhancement of CO₂ Removal Efficacy of Fluidized Bed Using Particle Mixing

by Ebrahim H. Al-Ghurabi, Abdelhamid Ajbar and Mohammad Asif

Appl. Sci. 2018, 8(9), 1467; https://doi.org/10.3390/app8091467 - 27 Aug 2018

Cited by 18 | Viewed by 4236

Abstract

The present study proposes a cost-effective assisted fluidization technique of particle mixing to improve the carbon capture effectiveness of a fluidized bed containing fine adsorbent powder. Using activated carbon as the adsorbent, we mixed external particle of Geldart group B classification in different fractions to examine the effectiveness of the proposed strategy of particle mixing. Four different particle-mixing cases were considered by varying the amount of added particle—0, 5, 10, and 30 wt %—on external particle-free basis. The inlet flow of the nitrogen was fixed, while two different flows of carbon dioxide were used. The adsorption experiment consisted of a three step procedure comprising purging using pure nitrogen, followed by adsorption with fixed inlet CO₂ concentration, and finally the desorption step. Inlet flows of both nitrogen and CO₂ were separately controlled using electronic mass flow controllers with the help of data acquisition system (DAQ). The CO₂ breakthrough was carefully monitored using the CO₂/O₂ analyzer, whose analog output was recorded using the DAQ. Best results were obtained with 10% external particles. This is in conformity with the results of our previous study of bed hydrodynamics, which pointed to clear improvement in the fluidization behavior with particle mixing. Full article

(This article belongs to the Special Issue Carbon Capture Utilization and Sequestration (CCUS))

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14 pages, 1322 KiB

Open AccessFeature PaperArticle

Acetic Acid as an Indirect Sink of CO₂ for the Synthesis of Polyhydroxyalkanoates (PHA): Comparison with PHA Production Processes Directly Using CO₂ as Feedstock

by Linsey Garcia-Gonzalez and Heleen De Wever

Appl. Sci. 2018, 8(9), 1416; https://doi.org/10.3390/app8091416 - 21 Aug 2018

Cited by 42 | Viewed by 6674

Abstract

White biotechnology is promising to transform CO₂ emissions into a valuable commodity chemical such as the biopolymer polyhydroxyalkanaotes (PHA). Our calculations indicated that the indirect conversion of acetic acid from CO₂ into PHA is an interesting alternative for the direct production of PHA from CO₂ in terms of CO₂ fixation, H₂ consumption, substrate cost, safety and process performance. An alternative cultivation method using acetic acid as an indirect sink of CO₂ was therefore developed and a proof-of-concept provided for the synthesis of both the homopolymer poly(3-hydroxybutyrate) (PHB) and the copolymer poly(3-hydroxybutyrate-co-3-hydroxyvalerate) (PHBV). The aim was to compare key performance parameters with those of existing cultivation methods for direct conversion of CO₂ to PHA. Fed-batch cultivations for PHA production were performed using a pH-stat fed-batch feeding strategy in combination with an additional Dissolved Oxygen (DO)-dependent feed. After 118 h of fermentation, 60 g/L cell dry matter (CDM) containing 72% of PHB was obtained, which are the highest result values reported so far. Fed-batch cultivations for PHBV production resulted in 65 g/L CDM and 48 g/L PHBV concentration with a 3HV fraction of 27 mol %. Further research should be oriented towards process optimisation, whole process integration and design, and techno-economic assessment. Full article

(This article belongs to the Special Issue Carbon Capture Utilization and Sequestration (CCUS))

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21 pages, 4580 KiB

Open AccessArticle

Nonlinearity Analysis and Multi-Model Modeling of an MEA-Based Post-Combustion CO₂ Capture Process for Advanced Control Design

by Xiufan Liang, Yiguo Li, Xiao Wu, Jiong Shen and Kwang Y. Lee

Appl. Sci. 2018, 8(7), 1053; https://doi.org/10.3390/app8071053 - 28 Jun 2018

Cited by 5 | Viewed by 4040

Abstract

The monoethanolamine (MEA)-based post-combustion CO₂ capture plant must operate flexibly under the variation of the power plant load and the desired CO₂ capture rate. However, in the presence of process nonlinearity, conventional linear control strategy cannot achieve the best performance under a wide operation range. Considering this problem, this paper systematically studies the multi-model modeling of the MEA-based CO₂ capture process for the purpose of (1) implementing well-developed linear control techniques to the design of an advanced controller and (2) achieving a wide-range flexible operation of the CO₂ capture process. The local linear models of the CO₂ capture process are firstly established at given operating points using the method of subspace identification. Then the nonlinearity distribution at different loads of an upstream power plant and different CO₂ capture rates is investigated via the gap metric. Finally, based on the nonlinearity investigation results, the suitable linear models are selected and combined together to form the multi-model system. The proposed model is validated using the measurement data, which is generated from a post-combustion CO₂ capture model developed in the go-carbon capture and storage (gCCS) simulation platform. As the proposed multi-linear model has a simple mathematical expression and high prediction accuracy, it can be directly employed as the control model of a practical advanced control strategy to achieve a wide operating range control of the CO₂ capture process. Full article

(This article belongs to the Special Issue Carbon Capture Utilization and Sequestration (CCUS))

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15 pages, 1675 KiB

Open AccessArticle

CO₂ Capture by Alkaline Solution for Carbonate Production: A Comparison between a Packed Column and a Membrane Contactor

by Israel Ruiz Salmón, Nicolas Cambier and Patricia Luis

Appl. Sci. 2018, 8(6), 996; https://doi.org/10.3390/app8060996 - 19 Jun 2018

Cited by 43 | Viewed by 10158

Abstract

A comparison between a traditional packed column and a novel membrane contactor used for CO₂ absorption with carbonate production is addressed in this paper. Membrane technology is generally characterized by a lower energy consumption, it offers an independent control of gas and liquid streams, a known interfacial area and avoids solvent dragging. Those advantages make it a potential substitute of conventional absorption towers. The effect of the concentration and the flow rates of both the flue gas (10–15% of CO₂) and the alkaline sorbent (NaOH, NaOH/Na₂CO₃) on the variation of the species present in the system, the mass transfer coefficient, and the CO₂ removal efficiency was evaluated. Under the studied operation conditions, the membrane contactor showed very competitive results with the conventional absorption column, even though the highest mass transfer coefficient was found in the latter technology. In addition, the membrane contactor offers an intensification factor higher than five due to its compactness and modular character. Full article

(This article belongs to the Special Issue Carbon Capture Utilization and Sequestration (CCUS))

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12 pages, 2020 KiB

Open AccessFeature PaperArticle

Formic Acid Manufacture: Carbon Dioxide Utilization Alternatives

by Marta Rumayor, Antonio Dominguez-Ramos and Angel Irabien

Appl. Sci. 2018, 8(6), 914; https://doi.org/10.3390/app8060914 - 2 Jun 2018

Cited by 90 | Viewed by 11638

Abstract

Carbon dioxide (CO₂) utilization alternatives for manufacturing formic acid (FA) such as electrochemical reduction (ER) or homogeneous catalysis of CO₂ and H₂ could be efficient options for developing more environmentally-friendly production alternatives to FA fossil-dependant production. However, these alternatives are currently found at different technological readiness levels (TRLs), and some remaining technical challenges need to be overcome to achieve at least carbon-even FA compared to the commercial process, especially ER of CO₂, which is still farther from its industrial application. The main technical limitations inherited by FA production by ER are the low FA concentration achieved and the high overpotentials required, which involve high consumptions of energy (ER cell) and steam (distillation). In this study, a comparison in terms of carbon footprints (CF) using the Life Cycle Assessment (LCA) tool was done to evaluate the potential technological challenges assuring the environmental competitiveness of the FA production by ER of CO₂. The CF of the FA conventional production were used as a benchmark, as well as the CF of a simulated plant based on homogeneous catalysts of CO₂ and H₂ (found closer to be commercial). Renewable energy utilization as PV solar for the reaction is essential to achieve a carbon-even product; however, the CF benefits are still negligible due to the enormous contribution of the steam produced by natural gas (purification stage). Some ER reactor configurations, plus a recirculation mode, could achieve an even CF versus commercial process. It was demonstrated that the ER alternatives could lead to lower natural resources consumption (mainly, natural gas and heavy fuel oil) compared to the commercial process, which is a noticeable advantage in environmental sustainability terms. Full article

(This article belongs to the Special Issue Carbon Capture Utilization and Sequestration (CCUS))

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12 pages, 721 KiB

Open AccessArticle

Water Resistant Composite Membranes for Carbon Dioxide Separation from Methane

by Colin A. Scholes

Appl. Sci. 2018, 8(5), 829; https://doi.org/10.3390/app8050829 - 21 May 2018

Cited by 8 | Viewed by 4408

Abstract

Membranes that are resistant to water vapor permeation have potential in natural gas sweetening by reducing the need for pretreatment. The perfluorinated polymer Teflon AF1600 has proven resistance to water vapor, which is adapted here in the form of composite membranes consisting of a Teflon AF1600 protective layer on membranes of the polyimide 4,4′-(hexafluoroisopropylidene) diphthalic anhydride 2,3,5,6-tetramethyl-1,4-phenylenediamine (6FDA-TMPDA) as well as Polymer of Intrinsic Micro-porosity (PIM-1). The permeability of CO₂ and CH₄ through the composite membranes was shown to be a function of the respective permeabilities of the individual polymer layers, with the Teflon AF1600 layer providing the majority of the resistance to mass transfer. Upon exposure to water, the composite membranes had reduced water permeation of 7–13% compared to pure membranes of 6FDA-TMPDA and PIM-1, because of the water resistance of the Teflon AF1600 layer. It was observed that water permeated as clusters through the composite structure. Under CO₂-CH₄ mixed gas conditions, 6FDA-TMPDA layer permselectivity performance was reduced and became comparable to Teflon AF1600, while the PIM-1 layer retained much of its high permselectivity performance. Importantly, at water activities below 0.2 the PIM-1 composite membrane achieved higher permeability for CO₂ compared to water. Full article

(This article belongs to the Special Issue Carbon Capture Utilization and Sequestration (CCUS))

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14 pages, 4473 KiB

Open AccessArticle

Capability of the Direct Dimethyl Ether Synthesis Process for the Conversion of Carbon Dioxide

by Ainara Ateka, Javier Ereña, Miguel Sánchez-Contador, Paula Perez-Uriarte, Javier Bilbao and Andrés T. Aguayo

Appl. Sci. 2018, 8(5), 677; https://doi.org/10.3390/app8050677 - 26 Apr 2018

Cited by 24 | Viewed by 5360

Abstract

The direct synthesis of dimethyl ether (DME) is an ideal process to achieve the environmental objective of CO₂ conversion together with the economic objective of DME production. The effect of the reaction conditions (temperature, pressure, space time) and feed composition (ternary mixtures of H₂ + CO + CO₂ with different CO₂/CO and H₂/CO_x molar ratios) on the reaction indices (CO_x conversion, product yield and selectivity, CO₂ conversion) has been studied by means of experiments carried out in a fixed-bed reactor, with a CuO-ZnO-MnO/SAPO-18 catalyst, in order to establish suitable ranges of operating conditions for enhancing the individual objectives of CO₂ conversion and DME yield. The optimums of these two objectives are achieved in opposite conditions, and for striking a good balance between both objectives, the following conditions are suitable: 275–300 °C; 20–30 bar; 2.5–5 g_cat h (mol_C)⁻¹ and a H₂/CO_x molar ratio in the feed of 3. CO₂/CO molar ratio in the feed is of great importance. Ratios below 1/3 are suitable for enhancing DME production, whereas CO₂/CO ratios above 1 improve the conversion of CO₂. This conversion of CO₂ in the overall process of DME synthesis is favored by the reverse water gas shift equation, since CO is more active than CO₂ in the methanol synthesis reaction. Full article

(This article belongs to the Special Issue Carbon Capture Utilization and Sequestration (CCUS))

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20 pages, 31470 KiB

Open AccessArticle

Preliminary Design and Model Assessment of a Supercritical CO₂ Compressor

by Zhiyuan Liu, Weiwei Luo, Qingjun Zhao, Wei Zhao and Jianzhong Xu

Appl. Sci. 2018, 8(4), 595; https://doi.org/10.3390/app8040595 - 10 Apr 2018

Cited by 29 | Viewed by 7373

Abstract

The compressor is a key component in the supercritical carbon dioxide (SCO₂) Brayton cycle. In this paper, the authors designed a series of supercritical CO₂ compressors with different parameters. These compressors are designed for 100 MWe, 10 MWe and 1 MWe scale power systems, respectively. For the 100 MWe SCO₂ Brayton cycle, an axial compressor has been designed by the Smith chart to test whether an axial compressor is suitable for the SCO₂ Brayton cycle. Using a specific speed and a specific diameter, the remaining two compressors were designed as centrifugal compressors with different pressure ratios to examine whether models used for air in the past are applicable to SCO₂. All compressors were generated and analyzed with internal MATLAB programs coupled with the NIST REFPROP database. Finally, the design results are all checked by numerical simulations due to the lack of reliable experimental data. Research has found that in order to meet the de Haller stall criterion, axial compressors require a considerable number of stages, which introduces many additional problems. Thus, a centrifugal compressor is more suitable for the SCO₂ Brayton cycle, even for a 100 MWe scale system. For the performance prediction model of a centrifugal compressor, the stall predictions are compared with steady numerical calculation, which indicates that past stall criteria may also be suitable for SCO₂ compressors, but more validations are needed. However, the accuracy of original loss models is found to be inadequate, particularly for lower flow and higher pressure ratio cases. Deviations may be attributed to the underestimation of clearance loss according to the result of steady simulation. A modified model is adopted which can improve the precision to a certain extent, but more general and reasonable loss models are needed to improve design accuracy in the future. Full article

(This article belongs to the Special Issue Carbon Capture Utilization and Sequestration (CCUS))

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Review

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22 pages, 9499 KiB

Open AccessReview

Role of Amine Type in CO₂ Separation Performance within Amine Functionalized Silica/Organosilica Membranes: A Review

by Liang Yu, Masakoto Kanezashi, Hiroki Nagasawa and Toshinori Tsuru

Appl. Sci. 2018, 8(7), 1032; https://doi.org/10.3390/app8071032 - 24 Jun 2018

Cited by 49 | Viewed by 7611

Abstract

Various types of amine-functionalized silica/organosilica membranes have been developed due to their potentially superior CO₂ separation performance. This article reviews the progress made in this field and special attention is paid to elucidating the role of amine type in CO₂ separation performance within amine-functionalized silica/organosilica membranes. This review includes a systematic comparison of various organosilica membranes with either unhindered or sterically hindered amines developed in our previous studies. Herein, we thoroughly discuss the structural characterizations and CO₂ adsorption/desorption properties of amine-functionalized xerogel powders and CO₂ transport/separation performance across the relevant membranes. Future directions for the design and development of high-performance CO₂ separation membranes are suggested, and particular attention is paid to the future of activation energies for gas permeation. Full article

(This article belongs to the Special Issue Carbon Capture Utilization and Sequestration (CCUS))

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