Journal of Cleaner Production
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2026
·
IF 10.7
Min Zhou,Ningbo Yu,Dongyang Li,Minghao Wang,Hongxia Gao,Zhiwu Liang
Intrinsic CO 2 kinetics of cyclic amines are quantified in water-lean ethers. • Zwitterion mechanism is validated as dominant in aprotic ether-water mixtures. • Ether solvents impede CO 2 absorption by disrupting the dynamic H-bond network. • MD shows an ether-induced solvent cage effect restricting CO 2 access to amines. • Rigid C-substituted amines with high nucleophilicity suit ether-based systems. Piperazine-derived cyclic amines represent promising solutions for efficient CO 2 capture. However, fundamental understanding of their structure-activity relationships remains limited. This work combined experimental and computational approaches to elucidate the influences of cyclic structures and functional groups of piperazine-derived cyclic amines (PZ, 2MPZ, AEP, 1MPZ and 2HPZ) on their CO 2 capture performance and the structure-activity relationship in both pure water and water-lean environments. Key findings reveal that substituents reduce nitrogen electron density and impose steric hindrance, impeding CO 2 access to active sites. Stopped-flow measurements of the intrinsic kinetics of cyclic amines in aqueous and ether-water solvents revealed a reactivity trend: PZ > 2MPZ > AEP > 1MPZ > 2HPZ. The zwitterion mechanism demonstrates relatively good accuracy (AARD: 1.30%-2.66%) than base-catalyzed hydration (AARD: 2.62%-9.46%). DFT validates the zwitterion pathway, while MD simulations indicate that pure water solution maintains dynamic hydrogen-bond networks without outer-layer clustering. Ether addition disrupts hydrogen bonding and diminishes electron density at reactive sites, reducing absorption rates. These findings elucidate the underlying structure-activity relationships and solvation effects, providing a fundamental molecular-level understanding of the kinetic behaviors in water-lean amine systems. Download: Download high-res image (578KB) Download: Download full-size image
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CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Xi Tang,Bin Xu,Xiaoyi Gao,Xiaoshan Li,Ge Gao,Wen Chen,Fan Wu,Cong Luo,Liqi Zhang
A multi-criteria rapid preliminary screening method for absorbents has been proposed. • Quasi-cycle capacity, absorption heat, and boiling point indicators were highly important for amine absorbents. • TEDA-DMEN exhibited a large quasi-cycle capacity, a low CO 2 absorption heat, and a low cost. The core of the CO 2 capture technology based on chemical absorption lies in the optimization of the performance of the absorbent. However, the current methods and indicators used to evaluate the performance of absorbents are limited, particularly those that incorporate energy consumption. This paper proposes a multi-criteria rapid preliminary screening method for absorbents, covering seven key indicators of the amine absorbent for CO 2 capture, to characterize CO 2 reaction performance, energy consumption performance, physical properties, and economic performance. The Analytic Hierarchy Process (AHP)-entropy weight Technique for Order Preference by Similarity to Ideal Solution (TOPSIS) method was used to rapidly screen 18 amine absorbents in three categories. The results showed that the evaluation method was primarily suitable for aqueous amines and could also be extended to other types of absorbents. In addition, the combined subjective and objective weighting results indicated that the quasi-cycle capacity, absorption heat, and boiling point indicators were highly important for amine absorbents. The comprehensive index (CI) demonstrated that among the three amine categories, AEEA, PS, and TEDA-DMEN were the best absorbents for CO 2 capture, respectively. In particular, TEDA-DMEN exhibited a large quasi-cycle capacity (0.560 mol/mol), as well as low CO 2 absorption heat (66.87 kJ/mol), sensible heat (37.61 kJ/mol), and cost (0.104 $/g). This paper provides a theoretical basis and methodological support for developing high-efficiency, low-energy, and low-cost absorbents for CO 2 capture.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Ge Gao,Xiaoyi Gao,Bin Xu,Wufeng Jiang,Zhenghong Zhao,Fan Wu,Xiaoshan Li,Cong Luo,Liqi Zhang
The CO 2 phase change absorbents(CPCAs) formed by introducing phase-splitting agents have attracted increasing attention because of their great energy-saving potential. However, the volatilization problem of the phase-splitting agents and the high viscosity of the solution affect the application of CPCAs. In this work, a novel CPCAs based on 2-Methylpiperazine (2MPRZ)/H 2 O was established by introducing triethylene glycol monobutyl ether (TGBE) with a high boiling point as a phase-splitting agent, and the 2MPRZ/H 2 O/TGBE system exhibited low volatility and low viscosity. The CO 2 capture performance of the novel CPCAs with different ratios was investigated in this work. The best CO 2 absorption rate was achieved by 2.5 M 2MPRZ/H 2 O/TGBE. The viscosity of this system before and after the CO 2 absorption process was merely 7.68 mPa·s and 11.64 mPa·s, respectively, and no volatilization of the phase-splitting agent was observed simultaneously. A convenient and rapid titration method was employed to determine the distribution of the 2MPRZ products in the two phases, which showed that 98 % of the 2MPRZ products were located in the CO 2 -rich phase. In addition, the CO 2 -rich phase captured 99 % of the total CO 2 , indicating that this system has superior phase-splitting behaviors. The regeneration energy consumption of this biphasic absorbent was 2.59 GJ/t CO 2 , which was 32.6 % lower than that of traditional MEA. Furthermore, the salting-out effect was proved to be the cause of the phase-splitting behavior by 13 C NMR analysis.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2018
·
IF 3.141
Rui Zhang,Wusan Jiang,Zhiwu Liang,Xiao Luo,Qi Yang
The CO2 reaction rate in aqueous 2-methylpiperazine (2MPZ) solution was investigated in terms of the pseudo-first-order rate constant (k0) by using a stopped-flow apparatus with amine concentration ranges of 0.05–0.125 mol/L and the measuring temperature ranges of 293.15–313.15 K. The results show that the CO2 reaction rate in the 2MPZ solution increased as the temperature and the amine concentration increases. The results also demonstrate that the 2MPZ has a faster reaction rate in terms of k0 than 3-dimethylaminopropylamine, 3-diethylaminopropylamine, and monoethanolamine (MEA) but slower than that of PZ at the same amine concentration. The equilibrium solubility as an important absorption parameter for CO2 capture also were measured at 298.15, 313.15, and 333.15 K with CO2 partial pressures of 5–100 kPa, respectively, in 2 M 2MPZ solution. The results show that the CO2 equilibrium solubility of 2MPZ increased as the CO2 partial pressure increased but decreased as the temperature increased. The heat of CO2 absorption in 2 M 2MPZ solution was estimated by using the Gibbs–Helmholtz equation, and the value (−70.9 kJ/mol) is similar to that of PZ but lower than that of MEA. Besides the conclusions stated above, the results of the 13C NMR quantitative investigation suggest that 2MPZ can produce less carbamate and more bicarbonate than PZ at the same CO2 loading.
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APPLIED ENERGY
·
2018
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IF 7.9
Fei Liu,Mengxiang Fang,Wenfeng Dong,Tao Wang,Zhixiang Xia,Qinhui Wang,Zhongyang Luo
Using biphasic solvents for carbon dioxide (CO 2 ) capture is regarded as a promising technology to drastically reduce the regeneration energy. However, this technology hasn’t been put into commercial application due to lack of the biphasic solvents with high stabilities and low costs. To overcome this challenge, we developed a novel type of biphasic solvent based on alkanolamine-alkanolamine blends, i.e., aqueous blends of 2-(diethylamino)-ethanol (DEEA, 50 wt%) and monoethanolamine (MEA, 25 wt%) or 2-((2-aminoethyl) amino) ethanol (AEEA, 25 wt%). The aqueous DEEA-AEEA solvent demonstrated a cyclic capacity as high as 0.64 mol CO 2 /mol which is significantly higher than those of 30 wt% MEA and other reported biphasic solvents. In addition, a phase split time as short as a few minutes is obtained. The phase split dynamics were analyzed to investigate the effects of CO 2 loading, temperature, gas flow rate and height-to-diameter ratio. Quantitative 13 C NMR analysis was then performed to reveal the reaction and phase split mechanism of CO 2 absorption in the DEEA-AEEA solvent. It indicated that the reaction of AEEA with CO 2 dominated at the beginning of CO 2 absorption and the products are formed as carbamates. Then, DEEA began reacting with CO 2 to yield bicarbonate and carbonate. The phase split mechanism indicated that the reaction products of carbamates and HCO 3 − /CO 3 2− migrated to the lower phase while DEEA and unreacted AEEA migrated to the upper phase. Finally, the cyclic tests were repeated and the energy consumption was evaluated. The regeneration energy of the biphasic solvent, without process optimizations, is 2.58 GJ/tCO 2 , which is 32% lower than that of the traditional 30 wt% MEA solvent.
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Reaction Chemistry & Engineering
·
2024
·Vol. 10
·期 1
·203-213
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IF 3.4
Ning Ma,Liu Yang,Zhenchang Fang,Kaijia Jiang,Xinling Li,Zhen Huang
Deficiencies such as high viscosity, volatility, and rich phase precipitation limited the engineering application of non-aqueous absorbents. A series of high boiling point solvent screening experiments were conducted to develop an absorption saturated solution with a homogeneous phase at low viscosity (14.71 mPa s) in this study. Further addition of polyamines increased the absorption capacity by 42% (3.55 mol CO2 per kg). The 13C NMR results indicated that in the DETA/MEA/NMF blended amine system, MEA was involved in the deprotonation process of DETA zwitterions as proton acceptors. Quantum chemical calculations were utilized to compare the energies of each possible single-step reaction, providing insights into the reaction pathways of the blended amine system. The rate constant of the MEA/CO2 reaction was found to be 1.98 times that of the DETA/CO2 reaction, indicating lower reaction activity, consistent with NMR results. In addition, the results of the analysis of weak interactions revealed that the hydrogen bonds were key factors affecting the viscosity change and precipitation in non-aqueous absorbents, providing a new method for designing novel low-viscosity non-aqueous absorbents. The combination of theoretical analysis and experimental results underscores the potential of the blended amine non-aqueous absorbent as a feasible alternative for the industrial applications of CO2 capture.
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CHIRALITY
·
2025
·Vol. 37
·期 7
·e70040
·
IF 3
Qinhua Liu,Xuan Kuang
Chiral recognition of amino acids is crucial in pharmaceutical and clinical fields due to the enantiomer-dependent bioactivity of chiral compounds. Here, we report an electrochemiluminescent (ECL) sensor utilizing a chiral covalent organic framework (CC-MP CCTF) for the selective discrimination of phenylalanine (Phe) enantiomers. Critical experimental parameters, including buffer pH (optimized to 7.38), tripropylamine (TPrA) concentration (9.99 mM), and CC-MP CCTF dilution ratio (1.6×), were optimized to maximize sensitivity. The sensor achieved a linear detection range (0.2–1.0 mM) for both D- and L-Phe with a limit of detection (LOD) of 0.1 mM. Remarkably, it exhibited exceptional enantioselectivity, showing a 1.96-fold higher ECL response to D-Phe than L-Phe, which originates from the chiral confinement effect of the CC-MP CCTF. This study proposes a cost-effective and rapid strategy for chiral amino acid recognition, demonstrating potential applications in bioanalysis and quality control processes.
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