Post-combustion Carbon Dioxide Capture Research Articles

Dissociation Constant of Di‐ and Tri‐Basic Solvents Based on Piperazine and Its Derivatives for Post‐Combustion CO2 Capture

AbstractAmine solvents remain popular in the industries for post combustion carbon dioxide (CO2) capture. Dissociation constant of basic amine solvents plays significant role to influence the CO2 absorption. It is thus important to study the dissociation of new amine solvents for assessing their viability for CO2 capture. In the present work, potentiometric titration method is employed to determine the dissociation constants of dibasic (e. g., Piperazine (PZ), 1‐methyl piperazine (1‐MPZ) and tribasic amines (1‐(2‐aminoethyl‐piperazine) (AEPZ) which could be promising for formulating blended solvent system towards enhancing the rate of CO2 absorption. The estimated dissociation constants for the PZ and 1‐MPZ while match well with reported results, the dissociation constants for AEPZ has been determined newly here within the temperature range 298—318 K. In addition, the structural geometric parameters and Natural Bond Order (NBO) calculations of the amine solvents are performed based on Density Functional Theory (DFT). The NBO calculations predict charge distribution on the nitrogen and other elements, and envisage its effect on the pKa values of the amines. Further, potential energy surface (PES) scanning calculations are performed for AEPZ to explain it's ring inversion which is responsible for obtaining a single pKa value in experimental studies.

Modeling gas–liquid equilibrium of carbon dioxide in mixtures of (1-butyl-3-methyl-imidazolium acetate + 1-(2-aminoethyl) piperazine + water) and (1-butyl-3-methyl-imidazolium acetate + bis (3-aminopropyl) amine + water) by electrolyte non-random two liquid (e-NRTL) model

Targeting the control in emissions of post-combustion carbon dioxide capture from large point sources, a simulation approach towards the estimation of important thermodynamic property parameters useful in designing of carbon capture and sequestration technologies is being proposed. In the current work, simulation is carried out for modeling the gas – liquid equilibrium of CO2 in two aqueous mixtures of ionic liquid 1-butyl-3-methyl imidazolium acetate ([bmim][Ac]) and amines viz. ([bmim][Ac] + 1-(2-aminoethyl) piperazine) (AEP) and ([bmim][Ac] + bis (3-aminopropyl) amine) (APA). The experimental CO2 solubilities were taken from our previously published work and is regressed with electrolyte–Non-Random Two Liquid (e-NRTL) model for the liquid phase while Redlich-Kwong (RK) equations of state (EOS) was used to model the gas phase. Various thermodynamic parameters of importance and concentration of species in the mixtures were regressed in the model using Aspen Plus 14.

Performance of industrially implemented turbulent contact absorbers – A comparative study

The current study aims to assess the performance and industrial feasibility of using three-phase fluidized bed absorption columns for post-combustion carbon dioxide (CO2) capture. The analysis is based on a mathematical model of a scaled-up fluidized bed absorption column that has been validated using pilot plant experimental data. The focus is on evaluating the energy efficiency of the fluidized bed column in comparison to packed bed technologies, which are currently widely used. The results of the analysis are evaluated in terms of three performance indicators (i.e., absorption efficiency, carbon capture rate, and energy performance index) and compared to packed bed columns. Simulation results indicate that the best column configuration is represented by a three-stage absorber and that the system performs optimally when particle diameter and density decrease with each section. Consequently, this leads to an increase in the total fluidized bed height and carbon capture rate by up to 25%. The energy performance index is maintained below 3.6, indicating an energy-efficient operation of the system. As such, the findings of this study suggest that the use of gas-solid-liquid three-phase fluidized bed absorption columns for post-combustion CO2 capture is a promising technology for the implementation of CCUS and for achieving of climate neutrality targets.

The relationship between oxidative degradation and ammonia emission of carbon capture amines based on their chemical structures

Abstract This work investigates the effect of chemical structural positioning of different functional groups in 29 amines covering primary, secondary and tertiary alkanolamines as well as multi-alkylamines and cyclic amines on both amine degradation and ammonia (NH3) emissions during post-combustion amine-based carbon dioxide capture. The results helped to elucidate possible relationships between degradation and emissions as related to the chemical structure of the amine. The results showed that longer alkyl chain lengths in multi-alkylamines caused a more drastic decrease in both degradation and NH3 emissions followed by secondary alkanolamines. The decrease in those activities for primary and tertiary alkanolamines as well as cyclic amines was low and more so for NH3 emissions. In contrast, the increase in hydroxyl groups in secondary alkanolamines caused a drastic increase in degradation and NH3 emissions. On the other hand, having more hydroxyl groups in sterically hindered primary and tertiary alkanolamines caused a more drastic decrease in degradation and a smaller decrease in NH3 emissions due to the steric hindrance within their structure. An increase in the number of amino groups in an amine caused an increase in both degradation and NH3 emission rates because these provided the reactive sites for the formation of free radicals. This effect was not as large in alkyl-cyclic amines as in multi-alkylamines due to the ability of the former to resist oxidative degradation. Furthermore, branched alkyl groups between amino and hydroxyl groups more drastically increased both the degradation and NH3 emission activities than branched alkyl groups located at the nitrogen atom.

Performance of Water-Lean Solvent for Postcombustion Carbon Dioxide Capture in a Process-Intensified Absorber: Experimental, Modeling, and Optimization Using RSM and ML

Performance of Water-Lean Solvent for Postcombustion Carbon Dioxide Capture in a Process-Intensified Absorber: Experimental, Modeling, and Optimization Using RSM and ML

Synthesis of core-shell magnetic mesoporous silica nanoparticles to disperse amine functionalities for post-combustion carbon dioxide capture

BackgroundPost-combustion capture technology appears a suitable approach to reduce the emission of CO2 by power plants. The use of solid sorbents would permit to overcome the limitations of the well-established liquid amine-based absorption process. In particular, mesoporous silica materials have been proposed as suitable sorbents especially if functionalized with amines. MethodsThe properties of as-synthesized (by using dodecylamine as synthesis amine) and calcined hexagonal mesoporous silica (HMS), impregnated or not with tetraethylenepentamine (TEPA), were studied. Magnetite (Fe3O4) nanoparticles were specifically used to obtain HMS core-shell nanoparticles in order to investigate the effect of the magnetite core on CO2 uptake capability. CO2 uptake measurements were carried out on all HMS and core-shell particles. Furthermore, Transmission Electron Microscopy (TEM) images, Fourier Transform Infrared (FTIR) spectra and N2 adsorption/desorption measurements allowed analyzing some important properties of the sorbent particles, such as particle aggregation, incorporation and dispersion of amines, surface area, pore volume and pore size distribution. Significant FindingsThe best performance in terms of chemical CO2 uptake was obtained on core-shell material, calcined and impregnated with TEPA (about 89 mg/g), but also the as prepared core-shell sample impregnated with TEPA seems promising since the synthesis dodecylamine sites can be activated during the impregnation process.

Membrane Distillation-Crystallization for Sustainable Carbon Utilization and Storage.

Anthropogenic greenhouse gas emissions from power plants can be limited using postcombustion carbon dioxide capture by amine-based solvents. However, sustainable strategies for the simultaneous utilization and storage of carbon dioxide are limited. In this study, membrane distillation-crystallization is used to facilitate the controllable production of carbonate minerals directly from carbon dioxide-loaded amine solutions and waste materials such as fly ash residues and waste brines from desalination. To identify the most suitable conditions for carbon mineralization, we vary the membrane type, operating conditions, and system configuration. Feed solutions with 30 wt % monoethanolamine are loaded with 5-15% CO2 and heated to 40-50 °C before being dosed with 0.18 M Ca2+ and Mg2+. Membranes with lower surface energy and greater roughness are found to more rapidly promote mineralization due to up to 20% greater vapor flux. Lower operating temperature improves membrane wetting tolerance by 96.2% but simultaneously reduces crystal growth rate by 48.3%. Sweeping gas membrane distillation demonstrates a 71.6% reduction in the mineralization rate and a marginal improvement (37.5%) on membrane wetting tolerance. Mineral identity and growth characteristics are presented, and the analysis is extended to explore the potential improvements for carbon mineralization as well as the feasibility of future implementation.

Multiobjective optimization of membrane in hybrid cryogenic CO2 separation process for coal-fired power plants.

Post-combustion carbon dioxide (CO2) capture is considered a potential method to mitigate CO2 emissions from fossil fuels burned in power plants. In recent years, combining two different methods of post-combustion CO2 capture such as membrane and cryogenic distillation has been explored for availing the advantages of each method. This study focuses on the optimization of membranes for developing the membrane-cryogenic distillation process. For this purpose, a process flow sheet is developed, and simulation with model components such as compressor, heat exchanger, turbo expander, and distillation column is carried out using Aspen Plus. A membrane model is developed using in-house MATLAB code, and optimization is done to achieve higher concentration and recovery of CO2 using the MOJAYA algorithm. The membrane model is coupled to Aspen Plus through component object model (COM) technology. In this investigation, a hollow fiber membrane is considered. The optimized specifications of membrane modules are length, number of hollow fibers, feed pressure, and permeate pressure which are 0.3 m, 100,000, 5.76 bar, and 0.1 bar, respectively. This analysis results in the purity and recovery of the process of 99.8 and 90%, respectively, and an energy penalty of around 1.74 MJ/kg of CO2. A comparison of other processes available in the literature reveals that the current study renders maximum purity and recovery with a minimum energy penalty.

Perspectives on the green hybrid blend of diethanolamine-glycerol for post-combustion carbon dioxide capture via a Y-type micro-reactor

CO2 capture by aqueous primary and secondary alkanolamine solutions is a recognized technology in industrial CO2 separation processes. Yet, certain obstacles caused by high-energy consumption due to the amine regeneration demands, and the formation of thermally stable salts require to be overcome for the development of these solvents. In this paper, glycerol, as a beneficial by-product of biodiesel production, has been introduced as a second promising CO2 absorbent for aqueous diethanolamine solution in a Y-type micro-reactor with dimensions of 800 µm × 4 cm × 19 cm. The experiments of CO2 capture into the hybrid blend of DEA-Glycerol were investigated at ambient pressure and the operating temperature of 25–45 °C, volumetric gas flow rate of 100–300 ml/min, DEA concentrations of 1.5–2.5 M, and glycerol concentrations of 5–15%wt. Experimental results demonstrated that adding 10 wt% glycerol in the aqueous blend of 2.5 M DEA-Glycerol boosts the CO2 removal percentage, RP, up to 96.89%, and enhances the volumetric overall gas-phase mass transfer coefficient, KGaV, and volumetric mass transfer flux, NAaV, to 34.89 kmol/m3.h.kPa and 88.04 kmol/h.m3, respectively. Furthermore, based on the Box-Behnken statistical responses, under the constant concentration of 2 M of DEA, increasing the presence of glycerol from 5 to 10 wt% in the hybrid blend of DEA-Gly can intensify the CO2 RP, KGaV, and NAaV values by 2.12% and 8.66%, and 1.80%, respectively, illustrating the glycerol contribution on the CO2 capture process.

Integration of adsorption based post-combustion carbon dioxide capture for a natural gas-fired combined heat and power plant

This paper proposes a continuous CO2 capture system for natural gas combined heat and power (CHP) facility and explores the potential of low-temperature vacuum-swing adsorption (VSA) process for post-combustion CO2 capture (PCC) in the context of carbon capture and storage (CCS). Although VSA has strong potential for efficient CO2 capture in district-scale energy systems, previous case studies have largely focused on high-emission coal combustion sources, making VSA application challenging for these conditions. We address this issue by theoretically designing a ready-to-operate flue gas cleaning process with CCS for a medium-sized 4.3 MW natural gas CHP operating in the local industry. Our in-depth analysis examines the most critical parts such as dehydration, involving condenser and temperature-swing adsorption (TSA), and CO2 capture via VSA. The conceptual design and performance of VSA are approached by developing a mathematical model to estimate the technology size and performance. This work shows that utilising a small fraction of heat recovered from CHP-generated flue gas is sufficient to supply the necessary heat for auxiliary units, and that using natural cooling water for dehydration effectively reduces moisture (87 vol%) and energy demand for final dehydration via TSA. Furthermore, it demonstrates that 4-step VSA consisting of 15 columns using zeolite 13X can separate CO2 with a desired purity of 90.4%, meeting the requirements for CO2 storage and transportation onshore, at a 15.6% recovery rate. The cost of achieving high CO2 purity without pre-pressurising the CO2-rich flue gas, while maintaining cycle simplicity, is discussed. Overall, our paper provides a comprehensive approach to retrofitting distract-scale power plants with CO2-lean emissions, presenting a ready-to-operate flue gas cleaning technology based on real operating conditions and technical restrictions, which can contribute towards decarbonisation.

Emerging technologies in post-combustion carbon dioxide capture & removal

While climate change has been recognized as a major issue in our century, posing existential threats at the planetary scale and affecting people’s lives worldwide, relatively little in a practical sense has been accomplished to date in terms of concrete action to mitigate this burning issue. Carbon Capture Utilization and Sequestration (CCUS) and its expansion to Carbon Dioxide Removal (CDR) and Negative Emissions Technologies (NET) have been widely accepted as important and necessary pathways to mitigate anthropogenic emissions of carbon dioxide (CO2). Post-combustion CO2 emissions are a major contributor to anthropogenic CO2 emissions and currently constitute greater than 30% of total global CO2 emissions. This paper reviews the existing post-combustion CCUS technologies in terms of their current stage of development, their commercialization potential by 2035, and options for their improvement. Consideration will be given to the fundamental principles upon which the reviewed technologies are based and the information available in the public domain by each technology provider. Of the reviewed technologies, two amine-based absorption technologies (MHI, Shell) have reached technology readiness level (TRL) 9 and are now at the commercialization stage. Several demonstration-based technologies at TRL > 6 are rapidly developing and they feature solvent, adsorption-based, membrane, and cryogenic carbon capture and hence are the focus of this review. Emphasis will be given to deployed and existing projects, as well as the type, size, and duration of the various development efforts for the technologies reviewed. Several research and development stage carbon capture technologies (TRL < 6) are promising and are expected to reach the demonstration stage by 2035, however, for reasons of succinctness and focus they will not be reviewed here. The authors have applied a commercial yet pragmatic lens in their review and commentary of the various technologies in development to gauge their potential commercial success based upon both existing commercialization stage of the technologies being reviewed, as well as their cost reduction potential. Finally, this review reflects the author’s opinions which are not necessarily shared by the technology owners/developers.

Post-Combustion Capture of Carbon Dioxide by Natural and Synthetic Organic Polymers

The elevation of carbon dioxide (CO2) levels in the atmosphere is responsible for global warming which in turn causes abrupt climate change and consequently poses a threat to living organisms in the coming years. To reduce CO2 content in the atmosphere CO2 capture and separation is highly necessary. Among various methods of CO2 capture post-combustion capture is very much useful because of its operational simplicity and applicability in many industries and power sectors, such as coal-fired power plants. Polymers with high surface area, high volume and narrow pores are ideal solid sorbents for adsorption-driven post-combustion CO2 capture. Natural polymers, such as polysaccharides are cheap, abundant, and can be modified by various methods to produce porous materials and thus can be effectively utilized for CO2 capture while the surface area and the pore size of synthetic porous organic polymers can be tuned precisely for high CO2 capturing capacity. A significant amount of research activities has already been established in this field, especially in the last ten years and are still in progress. In this review, we have introduced the latest developments to the readers about synthetic techniques, post-synthetic modifications and CO2 capture capacities of various biopolymer-based materials and synthetic porous organic polymers (POPs) published in the last five years (2018–2022). This review will be beneficial to the researchers to design smart polymer-based materials to overcome the existing challenges in carbon capture and storage/sequestration.

Thermodynamic analysis of a post-combustion carbon dioxide capture process in a pilot plant equipped with a heat integrated stripper

This paper presents a thermodynamic analysis of a carbon dioxide absorption process from flue gases, focusing on the Heat Integrated Stripper (HIS) as a promising modification to the conventional process. The primary objective is to compare the performance of the HIS-modified process with that of the standard process. Experimental research was conducted on a mobile pilot plant using aqueous solutions of MEA 30% for treating 200 m3/h of the flue gas.An advanced data validation and reconciliation method was used to reconcile measurements in the mass balancing of the carbon dioxide absorption process. The results demonstrate that heat integration has a positive impact on the temperature profile of the stripper, leading to an increase in carbon dioxide capture without requiring additional heat consumption. Specifically, the reboiler heat duty in the process was reduced from 3.22 to 3.00 MJ/kgCO2, indicating the effectiveness of the HIS-modified process in reducing energy consumption. The use of the advanced data validation and reconciliation method also increases the reliability of the obtained results, which can be beneficial for process modeling and design. These findings contribute to the development of more efficient carbon capture technologies.

A highly effective and low-cost sepiolite-based solid amine adsorbent for CO2 capture in post-combustion

Post-combustion carbon dioxide capture using inexpensive and highly efficient materials is a powerful tool for lowering industrial CO2 emissions. Herein, by impregnating acid-modified sepiolite with pentaethylenehexamine (PEHA), a series of adsorbents were delivered. For the comprehensive study of the adsorbents, the textural properties, saturation adsorption experiment, breakthrough adsorption experiment, kinetic models, reaction mechanism, economic evaluation, cyclic and thermal stability were measured. The results exhibited that the optimal H-P-0.9 adsorbent demonstrated a adsorption capacity of 2.47 mmol/g at 50 °C with good regeneration. Considering application to capture CO2 in flue gas, breakthrough adsorption experiments were studied, a higher adsorption capacity of 2.94 mmol/g at 50 °C (with 5% H2O) appeared in contrast to other sepiolite sorbents. The main factors of CO2 capture process were chemisorption and physisorption by Avrami model. Furthermore, appropriate moisture promoted the CO2 capture performance of the adsorbent. In addition, the result of in-situ DRIFTs revealed the capture process follows the anion cation mechanism, CO2 was finally converted to carbamate. The economic evaluation showed that the adsorbent capture 1 t CO2 at a low price of 2.0 × 105 $. These results proved that the sepiolite-based adsorbent may be a potential material for CO2 capture with low price and excellent adsorption capacity.

Energy Analysis of Low Carbon Hydrogen from Methane and End Use Implications

Today an abundance of natural gas offers an option for hydrogen generation from methane with carbon management that avoids greenhouse gas (GHG) emissions. The resulting low carbon hydrogen (LCH) may be an ecologically attractive and cost-effective compliment to hydrogen generation from electrolysis. This study highlights process comparisons based on energy efficiency for power generation and transportation. Cost-effective options for both end uses are emerging. While cost-effective for decarbonizing low-capacity factor natural gas power generation, using LCH does not offer a major energy efficiency advantage over postcombustion carbon dioxide (CO2) capture from existing high-capacity factor natural gas power plants. In contrast, LCH does offer a more energy-efficient substitute for liquid transportation fuel. While transportation electrification is more energy efficient than the use of LCH, there are strong reasons why it is likely that the transition away from the current liquid-fuel-dominated transportation sector will favor both electric and hydrogen fuel cell vehicles.

Thermo-economic optimization of a new solar-driven system for efficient production of methanol and liquefied natural gas using the liquefaction process of coke oven gas and post-combustion carbon dioxide capture

The suitable use of hydrogen-containing industrial by-products such as coke oven gas (COG) leads to a reduction of environmental pollution and energy waste. This paper develops a novel integrated structure for the simultaneous production of portable and relatively clean liquid fuels from COG and power plant exhaust gases. The subsystems include a CO2 capture unit to separate carbon dioxide from exhaust gases, natural gas purification and liquefaction process to produce liquefied natural gas (LNG), and a methanol production cycle. Photovoltaic panels with a geographical location in Iran are used to provide the required power. This process provides 1.287 kg/s of methanol and 1.678 kg/s of LNG as the main product and 46 kg/s of hot water as an industrial utility. The integrated structure's total energy and exergy efficiencies are 65.36% and 68.72%, respectively. The largest share of exergy degradation belongs to the photovoltaic panels (81.33%), heat exchangers (5.66%), and distillation towers (3.152%). The results of the economic assessment show that the payback period and the prime cost of product are 4.29 years and 0.3967 US$/kg methanol. The sensitivity analysis outcomes demonstrate that the efficiency of the whole process and the prime cost of the product increase to 69.05% and 0.4005 US$/kg methanol when the hydrogen content of the coke oven gas decreases from 65 to 54 mol%. Moreover, the flow rate decrease of COG from 991.6 to 901.6 kmol/h, reduces the prime cost of the product and the irreversibility of the whole system to 0.3855 US $/kg methanol and 55382 kW. Thermo-economic optimization of the hybrid system based on the non-dominated sorting genetic algorithm is implemented with TOPSIS and LINMAP being the decision-making methods. From the optimization results, the optimum values for the efficiency of the whole hybrid system and the prime cost of the methanol are calculated to be 65.83% and 0.3611 US$/kg methanol.

(3-Aminopropyl) triethoxysilane-functionalized silica nanocapsule adsorbent: Synthesis and analysis of physicochemical characteristics

3-aminopropyltriethoxysilane (APTES)-functionalized silica nanocapsule (A-SiNC) was prepared from a one-step synthesis process for the application of post-combustion carbon dioxide (CO2) capture. A-SiNC was synthesized from the microemulsion method by using cetyl trimethylammonium bromide (CTAB) as a cationic surfactant, toluene as co-solvent, APTES as an amine group, and tetraethyl orthosilicate (TEOS) as silica base. The synthesis and functionalization were carried out in a variation of APTES using Fourier-transform infrared spectroscopy (FTIR), thermogravimetric analysis (TGA), nitrogen adsorption-desorption measurements (BET), and transmission electron microscopy (TEM). The results showed that silica nanocapsules (SiNC) potential to react until a temperature of 166 ​°C, which indicates a stable thermal decomposition property. The surface area and surface morphology were influenced by the presence of an amino group as APTES loaded SiNC provides a different mechanism compared to blank SiNC. The close-packed structure was seen and proven in A-SiNC based on the observation from TEM.

User-assisted methodology targeted for building structure interpretable QSPR models for boosting CO2 capture with ionic liquids

Task-specific ionic liquid (IL) is an emerging class of compounds that may be environmentally friendly. Properly selected, these compounds may be green alternative to amine solutions and can replace them in post-combustion carbon dioxide (CO2) capture processes on an industrial scale. However, owing to the vast diversity of ions and their possible combinations, laboratory research is time consuming and expensive. Therefore, computational methods are preferred for assessing their potential applications. In this study, three quantitative structure–property relationship models based on six distinct descriptors were created to predict Henry’s law constant (HLC) of CO2 in 62 ILs. The statistical parameters of multiple linear regression, logistic regression, and partial least squares models were satisfactory. In all cases, the coefficients of determination (R2) exceeded 0,90, and both external and internal validation proved them to be reliable and predictive with Q2 and Rpred2 values exceeding 0,90 and 0,87, respectively. Three of the descriptors were attributed to cations, and three were attributed to anions. In contrast to many other models, the descriptors were chosen in a manner that ensured their interpretability. Each of the six descriptors was analyzed for its influence on HLC. On this basis, guidelines for designing the structure of ionic liquids with increased CO2 absorption capacity were developed.

Optimal computer-aided molecular design of ionic liquid mixtures for post-combustion carbon dioxide capture

This work addresses the post-combustion carbon dioxide capture capabilities of optimally designed mixtures of ionic liquids, as well as pure ionic liquids. We postulate that ionic liquid mixtures can display better absorption rates and processing features when compared with pure ionic liquids. The computer-aided molecular design of the ionic liquids mixture was posed as a mixed-integer nonlinear programming problem to determine both the chemical structure and the amount of each ionic liquid in the mixture. Also, multiobjective optimization was performed to determine optimal operating conditions, specifically pressure and ionic liquids mixture feed stream, for an absorption separation process with various optimal mixtures. Results show that the anion [Tf2N] with the chain -(CH)2(CH2)5(CH3)3 was present both in the pure ionic liquid case and in the mixtures of these compounds. Results also indicate that, even though the amount of carbon dioxide absorbed by pure ionic liquid is slightly higher than the absorbed by ionic liquids mixture, there are important operational and environmental advantages of using such type of mixtures since they have milder physical properties than the pure ionic liquid.

Fabrication of a superhydrophobic mixed matrix PVDF-SiO2-HDTMS hollow fiber membrane for membrane contact carbon dioxide absorption

In order to obtain high performance polyvinylidene fluoride (PVDF) hollow fiber membrane for post combustion carbon dioxide (CO2) capture from flue gas by membrane contact absorption technology, a novel mixed matrix membrane fabrication process was proposed in this study. The mixed matrix PVDF-SiO2 (silicon dioxide)-HDTMS (hexadecyltrimethoxysilane) hollow fiber membranes fabricated via this process exhibit super-hydrophobicity on the outer surface and high mechanical strength. Among the membranes, the PVDF-SiO2(1.5)-HDTMS membrane exhibited the highest CO2 absorption performance, which was due to its excellent properties. It had water and diethanolamine (DEA, 1 mol/L) contact angles of 159.3° and 157.5°, respectively. Tensile strength, elongation at break, and LEPW (liquid entry pressure of water) of it were 3.2 × 106 Pa, 35.0%, and 9.0 × 105 Pa, respectively. The CO2 absorption flux of PVDF-SiO2(1.5)-HDTMS membrane attained 2.39 × 10−3 mol‧m−2‧s−1, which was 7.2% and 141.4% higher than that of the PVDF-HDTMS-1.5 and PVDF membranes, respectively. Moreover, CO2 absorption flux of the PVDF-SiO2(1.5)-HDTMS membrane decreased only 3% after twenty days of continuous operation. Highlighted by the outstanding performance in membrane contact CO2 absorption, the PVDF-SiO2(1.5)-HDTMS membrane shows great potential in the application of membrane contact absorption for post-combustion CO2 capture.