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Journal of Materials Chemistry A · 2021 ·Vol. 9 ·期 21 ·12763-12771 · IF 12.732

MXene-supported stable adsorbents for superior CO2 capture

Fa-Qian Liu,Xin Liu,Lishui Sun,Rongxun Li,Chun-Xiao Yin,Bozhen Wu

Polyamine-based solid adsorbents are promising candidates for CO2 capture, but long-term stability under practical regeneration conditions (100% CO2 at 120 °C) remains the biggest hurdle. In this paper, we prepared MXene-supported adsorbents with excellent long-term stability by combining two strategies. First, 1,2-butylene oxide (BO) with an epoxy group was grafted onto polyethyleneimine (PEI) to suppress the formation of urea. Second, Ti3C2(OH)x MXene was used as the support of polyamines to improve the wear resistance and thermal conductivity. The prepared MXene-supported adsorbents exhibit a large working capacity (2.6 mmol g−1) and a very stable cycling stability because of the synergetic effect. The adsorbents also exhibit a very low regeneration heat of 1.90 MJ per kg (CO2) and a high mechanical stability against attrition (0.26% after 5 h time-on-stream). Thus, these MXene-supported adsorbents make the CO2 capture process promising.

研究领域: 材料科学 · 环境工程
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ENVIRONMENTAL SCIENCE & TECHNOLOGY · 2018 · IF 6.653

Advanced Monoethanolamine Absorption Using Sulfolane as a Phase Splitter for CO2 Capture

Lidong Wang,Yifeng Zhang,Rujie Wang,Qiangwei Li,Shihan Zhang,Meng Li,Jie Liu,Bo Chen

A novel phase splitter, namely, sulfolane, was proposed to advance the traditional monoethanolamine (MEA) absorption technology for CO2 capture by simultaneously promoting the absorption rate and lowering heat duty. The phase-splitting phenomenon was observed after the CO2 loading level had exceeded 0.73 mol CO2/L, thereby generating a CO2-rich MEA upper layer and a lower layer containing sulfolane. Sulfolane facilitated CO2 absorption because of its strong affinity with acid gases, which resulted in an absorption rate 2.7 times higher than that of the conventional MEA process. The process simulation using Aspen Plus indicated that the regeneration heat with the MEA/sulfolane mixture as a solvent substantially decreased to 2.67 GJ/t-CO2, which was 31% lower than that of the conventional MEA process (3.85 GJ/t-CO2). Moreover, the sensible heat and vaporization heat of MEA/sulfolane were markedly decreased by 62.4% and 47.9%, which could be ascribed to the decreased stripping volume and relatively high CO2 partial pressure caused by liquid–liquid phase separation. The proposed system is proved to be a promising candidate for the advancement of CO2 capture techniques with high CO2 absorption capacity, rapid absorption rate, and low-energy penalty.

CAS / MDL: 7789-20-0 123-91-1
研究领域: 化学工程 · 环境科学
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ACS Applied Materials & Interfaces · 2023 · IF 9.5

Wood-Inspired Ultrafast High-Performance Adsorbents for CO2 Capture

Bozhen Wu,Xuejiao Song,Dongchen Zheng,Qianyun Tan,Yong Yao,Fa-Qian Liu

Under favorable regeneration conditions (120 °C, 100% CO2), ultrafast adsorption kinetics and excellent long-term cycle stability are still the biggest obstacles for amine-based solid CO2 adsorbents. Inspired by natural wood, a biochar with a highly ordered pore structure and excellent thermal conductivity was prepared and used as a carrier of organic amines to prepare ideal CO2 adsorbents. The results showed that the prepared adsorbent has a very high adsorption working capacity (4.23 mmol CO2·g–1), and its performance remains stable even after 30 adsorption–desorption cycles in the harsh desorption environment (120 °C, 100% CO2). Due to the existence of the hierarchical structure, the adsorbent exhibited ultra-fast adsorption kinetics, and the reaction rate constant is 37 times higher than that of traditional silica. This adsorbent also showed a very low regeneration heat of 1.64 MJ·kg–1 (CO2), which is especially important for the practical application. Therefore, these biochar-based adsorbents derived from natural wood make the CO2 capture process promising.

研究领域: 材料科学 · 环境科学 · 化学工程
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ENVIRONMENTAL SCIENCE & TECHNOLOGY · 2018 · IF 6.653

Kinetics, Thermodynamics, and Mechanism of a Novel Biphasic Solvent for CO2 Capture from Flue Gas

Shihan Zhang,Yao Shen,Peijing Shao,Jianmeng Chen,Lidong Wang

The main issue related to the deployment of the amine-based absorption process for CO2 capture from flue gas is its intensive energy penalty. Therefore, this study screened a novel biphasic solvent, comprising a primary amine e.g., triethylenetetramine (TETA) and a tertiary amine e.g., N,N-dimethylcyclohexylamine (DMCA), to reduce the energy consumption. The TETA-DMCA blend exhibited high cyclic capacity of CO2 absorption, favorable phase separation behavior, and low regeneration heat. Kinetic analysis showed that the gas- and liquid-side mass transfer resistances were comparable in the lean solution of TETA-DMCA at 40 °C, whereas the liquid-side mass transfer resistance became dominant in the rich solution. The rate of CO2 absorption into TETA-DMCA (4 M, 1:3) solution was comparable to 5 M benchmark monoethanolamine (MEA) solution. Based on a preliminary estimation, the regeneration heat with TETA-DMCA could be reduced by approximately 40% compared with that of MEA. 13C NMR analysis revealed that the CO2 absorption into TETA-DMCA was initiated by the reaction between CO2 and TETA via the zwitterion mechanism, and DMCA served as a CO2 sinker to regenerate TETA, resulting in the transfer of DMCA from the upper to lower phase. The proposed TETA-DMCA solvent may be a suitable candidate for CO2 capture.

研究领域: 化学工程 · 环境科学
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ENERGY · 2018 · IF 4.968

A study of structure-activity relationships of aqueous diamine solutions with low heat of regeneration for post-combustion CO2 capture

Zeyang Wu,Sen Liu,Hongxia Gao,Qiqi Yin,Zhiwu Liang

The structure-activity relationship of eleven diamines and MEA was investigated in order to provide guidance for the selection of the potential CO 2 capture absorbent. The effects of methyl, ethyl, hydroxyl groups, and distance between N groups in molecular structures were evaluated experimentally by using the rapid fast screening method and computed by Gaussian 09. Experimental results revealed that the proper number of methyl groups and ethyl groups on N atom could improve the absorption rate as well as the cyclic CO 2 capacity, and the addition of a hydroxyl group actually achieved a lower energy requirement (i.e. cyclic CO 2 capacity) for solvent regeneration with the decreasing stability of carbamate. In addition, the diamine with a hydroxyl group is more favorable for good stability in regeneration process, which addresses the problem of solvent loss in the application of diamines. Chain length extension from C 2 to C 3 can result in the poorer stability of the carbamate and lower energy requirement for amine regeneration. Thus, the lowest energy consumption (i.e. CO 2 cyclic capacity) was then achieved by aqueous 2-((2-aminoethyl)amino)ethanol (AEEA) solution, presenting it can be considered as an alternative or a potential absorbent for post-combustion CO 2 capture. Furthermore, the relative free energies of the tested diamines were computed by the Gaussian software for validating the stability of the carbamate formation , the order of which is in accordance with the order of the cyclic CO 2 capacity for all tested amines, indicating the experimental conclusion can be reliable.

研究领域: 化学工程 · 环境科学
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JOURNAL OF THERMAL ANALYSIS AND CALORIMETRY · 2019 ·Vol. 137 ·期 4 ·1225-1232 · IF 2.471

Form-stable phase change materials based on castor oil and palmitic acid for renewable thermal energy storage

Wu Bo,Zhao Yuanyang,Liu Qinfeng,Zhou Changlin,Zhang Xi,Lei Jingxin

Utilization of renewable biomass to prepare phase change material (PCM) that can reversibly store renewable thermal energy is of great interest. Castor oil with functional hydroxyl groups is especially attractive for the preparation of polymeric materials. In this work, a novel castor oil-based polyurethane-acrylate oligomer (COPUA) was firstly synthesized through a two-step condensation reaction. Followed by in situ polymerization of COPUA in the presence of palmitic acid (PA), a novel biomass-based form-stable PCM was prepared, in which renewable PA serves as phase change functional ingredient and castor oil-based crosslinking network acts as encapsulation material. Tailoring the mass ratio of PA and COPUA provides the ultimate encapsulation ratio (70%) of PA in form-stable PCM. The chemical structure, crystalline property, thermal property of form-stable PCM were characterized using Fourier transform infrared spectroscopy, wide-angle X-ray diffraction, differential scanning calorimetry and thermogravimetric. Those results demonstrate that the prepared form-stable PCM possesses that good thermal storage capacity with the phase change enthalpy reaches 141.2 J g −1 . Accelerated thermal cycling test was also performed to illustrate the thermal reliability of form-stable PCM.

CAS / MDL: 4098-71-9
研究领域: 材料科学 · 能源工程
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SEPARATION AND PURIFICATION TECHNOLOGY · 2023 · IF 8.6

Diamine-appended metal-organic framework for carbon capture from wet flue gas: Characteristics and mechanism

J.Y. Yong,R.Y. Xie,Q. Huang,X.J. Zhang,B. Li,P.F. Xie,C.F. Wu,L. Jiang

Due to the superior CO 2 adsorption capacity and selectivity, amine-functional solid adsorbents have received increasing attention. Nevertheless, amine-functionalized polyporous materials have a large performance deviation when considering carbon removal capacity under wet flue gas. Therefore, a variety of metal–organic frameworks (MOFs) with amine functionality are synthesized in this work by appending diamine with a propylene linker to Mg 2 (dobpdc) (dobpdc 4- = 4,4′-dioxido-3,3′-biphenyldicarboxylate) and screened under the simulated flue gas environment with a high water content (7 v%). The results indicate that ndmpn-grafted Mg 2 (dobpdc) (ndmpn = N,N-dimethyl-1,3-propanediamine) has a high CO 2 adsorption capacity of 1.72 mmol/g at 60 °C with an extremely low regeneration heat (2.26 GJ/ton CO 2 at the desorption temperature of 145 °C). Adsorption property of ndmpn-Mg 2 (dobpdc) at high humidity is even more excellent than that of another well-reported diaminopropene-appended MOF, dmpn-Mg 2 (dobpdc) (dmpn = 2,2-dimethyl-1,3-propanediamine). Herein, van der Waals (vdW)-corrected density functional theory (DFT) calculations are used to quantitatively analyze binding strengths and water effects on it between diamine-appended Mg 2 (dobpdc) and CO 2 . It is revealed that the addition of water makes ammonium carbamate chains produced in ndmpn-Mg 2 (dobpdc) more stable. These chemisorption structures under humid conditions have also been disclosed by using 15 N solid-state nuclear magnetic resonance (NMR) spectroscopy experiments and DFT calculation. To conclude, we unveil the binary adsorption characteristics and mechanism of ndmpn-Mg 2 (dobpdc). It enables a thorough understanding of this compound and highlights its potential as a promising adsorbent under humid conditions for post-combustion applications.

CAS / MDL: 302-01-2
研究领域: 材料科学 · 环境科学
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JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY · 2023 ·Vol. 99 ·期 1 ·183-194 · IF 3.4

An investigation on the effects of organic additives on CO2 capture performance of Na2CO3 solution

Zhen Wang,Zhitao Han,Gang Liu,Zelu Zhou,Xi Wu,Song Zhou,Xinxiang Pan

BACKGROUND The large-scale practical application of CO 2 capture using carbonate solutions is mainly limited by their low CO 2 absorption rate. In view of this, it is feasible to improve CO 2 capture performance of carbonate solution by adding additives. In this paper, low-cost sodium carbonate (Na 2 CO 3 ) solution was selected as the main CO 2 absorbent, and the effects of different organic additives on CO 2 capture performance of Na 2 CO 3 solutions were systematically investigated. RESULTS The results showed that 0.04 mol/L tetrabutylammonium bromide (TBAB) could achieve a better enhancement effect on CO 2 capture performance of Na 2 CO 3 solution. After addition of TBAB, the maximum CO 2 absorption rate of Na 2 CO 3 solution was improved to 2.52 × 10 −3 mol/min, which increased by 105%. And the maximum CO 2 desorption rate could also be improved by 45%. TBAB/Na 2 CO 3 system not only realized a high CO 2 absorption capacity of 0.769 mol/mol, but also maintained 82% of the initial CO 2 absorption capacity after three cyclic tests. The regeneration heat duty of TBAB/Na 2 CO 3 solution was calculated to be 1136.6 kJ/mol, which was significantly lower than that of single Na 2 CO 3 solution and conventional MEA aqueous solution. The promotion mechanism of TBAB in Na 2 CO 3 solution was explored using Fourier transform infrared spectra (FTIR) and 13 C nuclear magnetic resonance (NMR) analysis. CONCLUSION The introduction of TBAB additive could significantly improve CO 2 capture performance of Na 2 CO 3 solution and reduce regeneration heat duty, making it a possible option in the field of post-combustion CO 2 capture. © 2023 Society of Chemical Industry (SCI).

研究领域: 化学工程 · 环境科学
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ENERGY · 2025 · IF 9.4

Energy consumption analysis and parameter optimization of CO2 desorption in a structured packaged column

Kefei Li,Yue Wu,Yiming Bai,Hai Yan,Yiming Wang,Yuzhe Guan,Liang Li,Guicheng Liu

Reducing the energy consumption of CO 2 regeneration is crucial for enhancing the economic feasibility of CO 2 capture processes. While most studies have focused on developing novel absorbents, the influence of operating parameters on gas-liquid mass transfer behavior and their subsequent impact on energy consumption has received limited attention. This study experimentally investigates the regeneration heat duty (Q reg ) for CO 2 desorption from a 1-(Dimethylamino)-2-propanol (1DMA2P)/2-Methylaminoethanol (MAE) aqueous blend in a lab-scale stripper equipped with high-efficiency Sulzer DX structured packing. The effects of key operating parameters, including rich CO 2 loading, lean CO 2 loading, solution flow rate, amine concentration, and synergistic parameters (Δ α  ×  L and C  ×  L ), on Q reg were systematically analyzed. The experimental results showed that all these factors greatly influenced Q reg . For example, the Q reg decreases as the lean CO 2 loading (α lean ) , rich CO 2 loading (α rich ) , and 1DMA2P/MAE concentration (C) increase, indicating that the Q reg can be reduced by optimizing these operating parameters. Additionally, compared with MEA, 1DMA2P/MAE reduces energy consumption by 51.5 % and decreases the stripper height by 35 %. This study underscores the critical role of operating parameters in reducing CO 2 regeneration energy consumption. The findings provide valuable insights into optimizing stripper performance and demonstrate the advantages of the 1DMA2P/MAE blend as an energy-efficient alternative to MEA-based solvents in industrial CO 2 capture applications.

CAS / MDL: 109-83-1
研究领域: 化学工程 · 环境工程 · 能源技术 · 过程优化
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ACS Sustainable Chemistry & Engineering · 2020 · IF 7.632

An Efficient Solid–Liquid Biphasic Solvent for CO2 Capture: Crystalline Powder Product and Low Heat Duty

Zhibiao Chen,Guohua Jing,Bihong Lv,Zuoming Zhou

A nonaqueous, phase-change absorbent of 2-amino-2-methyl-1-propanol (AMP)/piperazine (PZ) and environmentally friendly solvent dipropylene glycol dimethyl ether (DME) fixes a number of issues suffered by a solid–liquid biphasic solvent, such as high viscosity of the saturated solution and difficult separation and regeneration of the viscous solid. The solid phase occupies 43% of the total volume while attributes about 94% of the total loading (0.87 mol mol–1) of the solution. Beside the formation of AMP-carbamate and PZ-carbamate according to zwitterions mechanism, the coupling products of AMP/PZ-carbamate are also found in the crystal, which helps to reduce the desorption temperature during the regeneration. Because of low solubility, self-aggregation, and high lattice energy in DME, the CO2 products precipitate and form a white crystalline powder in the lower phase of the solution. Meanwhile, the solid precipitation helps the bulk solution to keep a lower partial pressure and higher diffusivity of CO2, conforming a perfect performance of CO2 capture into the biphasic solvent. The regeneration heat duty of the solvent (1.61 GJ t–1 CO2) was approximately 57% less than that of the benchmark monoethanolamine (MEA) because of its perfect performance on CO2 capture, such as high absorption loading, high regeneration efficiency, and low amount of rich phase required for regeneration. The novel absorbent has a great potential for green and sustainable CO2 capture.

研究领域: 化学工程 · 环境科学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2025 · IF 9

Diluent Tailored quaternary deep eutectic solvents for energy efficient carbon capture

Jubao Gao,Yixuan Liu,Xueyi Song,Shujuan Wang,Yongqiang Ren,Shisen Xu

Deep eutectic solvents (DESs) are recognized as promising environmentally friendly absorbents for carbon capture. While a considerable body of research has been dedicated to the development of ternary DESs, the energy performance of these systems, especially under low-dilution conditions, remains a relatively under-explored area. In this study, we developed a novel quaternary DES system by introducing water and ethylene glycol as diluents into the ternary DES [ChCl][MEA]-5% M. The impact of diluent incorporation was systematically evaluated through (1) simulated flue gas CO 2 capture experiments, (2) NMR and FTIR spectral analyses, and (3) CO 2 desorption experiments with regeneration heat evaluations. Energy efficiency assessments were subsequently conducted to quantify the overall performance enhancement. Key findings revealed that the formulated quaternary DES achieved a substantial viscosity reduction while maintaining 90.1 % of the baseline absorption capacity. The regeneration heat of [ChCl][MEA]-5%M−20 %H 2 O and [ChCl][MEA]-5%M−20 %EG was found to be reduced by 46.87 % and 46.62 %, respectively, in comparison with that of 30 wt% MEA. Remarkably, the diluted system exhibited 74.4 % lower heat exchanger capital cost and sensible heat loss compared to conventional ternary DESs, with normalized capacity of 4.07 mol CO 2 /kg. These results demonstrate that water/ethylene glycol-modified quaternary DESs present a technologically superior and economically viable alternative for industrial carbon capture applications, effectively balancing absorption efficiency, energy demand, and operational stability.

研究领域: 化学工程 · 环境科学 · 能源技术 · 材料科学
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ENVIRONMENTAL SCIENCE & TECHNOLOGY · 2021 · IF 9.028

A Novel Dual-Stage Phase Separation Process for CO2 Absorption into a Biphasic Solvent with Low Energy Penalty

Xiaowei Zhou,Yao Shen,Fan Liu,Jiexu Ye,Xinya Wang,Jingkai Zhao,Shihan Zhang,Lidong Wang,Sujing Li,Jianmeng Chen

An amine-based biphasic solvent is promising to cut down the energy penalty of CO2 capture. However, the high viscosity of the CO2-enriched solvent retards its industrial application. This work proposed a novel dual-stage phase separation process using a triethylenetetramine and 2-(diethylamino)ethanol blend as a biphasic solvent, which separates a certain proportion of CO2-enriched phase during CO2 absorption to reduce its viscosity. Experimental results showed that the proposed dual-stage phase separation process improved the phase separation behavior and effectively enhanced the absorption rate by 49% at 50 °C, when 50 vol % CO2-enriched phase was separated at 0.3 mol mol–1. Kinetic analysis showed that the absorption rate was mainly controlled by liquid-side mass transfer. The regeneration heat of the dual-stage phase separation process cut down the energy penalty by 33% compared with the monoethanolamine-based process. Compared with the conventional biphasic solvent-based process, the heat duty was further declined by 8%. The 1H nuclear magnetic resonance analysis showed that the dual-stage phase separation process could effectively control the generation of absorption products and intensify the interphase migration of tertiary amines.

研究领域: 化学工程 · 环境科学 · 能源技术
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