Reaction Chemistry & Engineering
·
2024
·Vol. 10
·期 1
·203-213
·
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.
研究领域:
化学工程
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Qinlan Luo,Yan Ouyang,Shumin Hong,Nan Wang,Yuanyuan Li,Hongxia Gao,Gyeong S. Hwang,Bohak Yoon,Teerawat Sema,Paitoon Tontiwachwuthikul,Peng Luo,Chintana Saiwan,Zhiwu Liang
To explore the regulatory factor of phase separation and the effect of solvent structure, the phase separation behavior, absorption/desorption performance, viscosity change, heat duty and ternary phase diagram of 3 monoethanolamine(MEA)-based phasic absorbents using 3 alcohols with various carbon chain lengths and isomers were determined by comprehensive experiments. The tunable phase separation behavior of MEA-based biphasic absorbents can be achieved by adjusting the mass concentration ratio of solvent and water, and the CO 2 loading of phase separation point was much more impacted by the effect of the carbon chain length than that of isomerism. The intermolecular interactions between species in solutions before and after CO 2 absorption were analyzed by the classical molecular dynamics simulations and independent gradient model analysis. Based on the experimental and computational results, the fundamental mechanism of phase separation was elucidated, which is related to the broken of hydrogen bonds between solvent with H 2 O or MEA, and the enhanced interaction among MEACOO − , MEAH + and H 2 O. This study highlights the effect of structure effect on developing advanced CO 2 biphasic absorbents, which may reduce the energy consumption of regeneration significantly.
研究领域:
化学工程
·
环境科学
·
计算化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Chao Liu,Guohua Jing,Zongqiang Zhu,Yinming Fan,Shengpeng Mo,Yanan Zhang,Dunqiu Wang,Bihong Lv,Mingming Fu,Xiaobin Zhou
Diamines or polyamines with two or more amino groups are suitable for formulating non-aqueous absorbents (NAAs) with high CO 2 loading capacity and low regeneration energy consumption. However, these two types of amines in NAAs are prone to produce insoluble gelatinous products after absorbing CO 2 , resulting in difficult operation of the CO 2 capture system. In this study, by using 2-amino-2-methyl-1-propanol (AMP) as an inhibitor, the insoluble gelatinous products of the aminoethylethanolamine (AEEA)-N-methyl-2-pyrrolidone (NMP) (A-A-N) and 3-(methylamino)propylamine (MAPA)-NMP (M-A-N) NAAs were successfully eliminated. The experimental results showed that the AMP-regulated NAAs possessed a high absorption rate, high CO 2 loading capacity, excellent desorption efficiency, and stable recyclability. The reaction mechanism of CO 2 absorption and the inhibitory mechanism of AMP on the formation of gelatinous products were comprehensively elucidated. Taking the A-A-N system as a representative, AEEA reacted with CO 2 to form zwitterionic protonated carbamate species (AEEACO 2 − (P) H + (S) ), which tended to self-aggregate via hydrogen-bond interaction, resulting in the formation of insoluble gelatinous products. With the introduction of AMP, the AMP-derived products could combine easily with AEEACO 2 − (P) H + (S) via strong electrostatic attraction to form ion pairs, preventing the AEEACO 2 − (P) H + (S) molecules from self-aggregating to form insoluble gelatinous products. The regeneration heat duty of the A-A-N system was 1.89 GJ∙ton −1 CO 2 , which was 49.9 % lower than that of the benchmark 30 wt% MEA. Overall, introducing AMP as a gelatinous product inhibitor was beneficial for the development of NNAs with high CO 2 absorption capacity and low-energy consumption.
研究领域:
化学工程
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Fen Liu,Jingcong Zhang,Wenxuan Bai,Jinxiang Chen,Zhiping Gu,Jiang Yu
To reduce the energy consumption of regeneration for HCl absorption, and to recover HCl to high-value products, a sustainable phase-change system was constructed with N-methyldiethanolamine (MDEA) and polyethylene glycol dimethyl ether (NHD) in this paper. The MDEA/NHD phase change absorbent for HCl absorption is optimized by the ternary phase diagram and phase behavior of MDEA/NHD/HCl system. The results demonstrate that the biphasic system can be constructed with the mass fraction of HCl less than 28% and NHD component in the range of 23.0% ∼ 95.3%. Because of the higher stability of protonated MDEA·HCl than that of NHD·HCl, HCl molecules are mainly enriched in MDEA phase containing the volume ratio of less than 1/3 and partition coefficient over 100 at the neutral point. Therefore, only MDEA phase needs to be recycled, which results in reducing the circulation of regeneration by approximately 68%. Moreover, concentrated HCl in anhydrous MDEA phase could further prevent the side reaction of OER and improve the Faradaic efficiency toward HER and CER to reach 98.5% and 90.5% at 55 °C, respectively. And the energy consumption of regeneration is reduced to 0.37 GJ/t(absorbed HCl) in MDEA/NHD biphasic absorbent compared with that of 2.3 GJ/tCO 2 by DMX™ phase change absorption for CO 2 . By enhancing the conductivity and decreasing the viscosity of MDEA phase, introducing water in MDEA/NHD/HCl solution within 5% could significantly promote the current density and maintain high Faradaic efficiency toward HER and CER as 89.0% and 86.8%, respectively. Therefore, it is a promising technology to be applied in industry.
研究领域:
化学工程
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
MACROMOLECULAR CHEMISTRY AND PHYSICS
·
2025
·
IF 2.7
Danni Zhu,Zhe Li,Yuqing Wang,Wuxiang Chen,Nanshan Wu,Miaoming Huang,Hao Liu,Suqin He,Wanlin Xu,Wentao Liu
Polyurethane (PU) is widely used in production and daily life due to its excellent mechanical properties and strong plasticity. Long-term ultraviolet (UV) irradiation will cause PU aging and shorten its service life. However, preparing UV-resistant PU, which is colorless, transparent, and non-migratory, remains a challenge. This work introduced the reactive benzotriazole UV absorber (R455) into the PU molecular chain to prepare colorless and transparent intrinsic UV-resistant samples (PCU) by polymerization, using polycarbonate diol as soft segment, dicyclohexylmethane diisocyanate as hard segment, and 1,6-hexanediol as chain extender. The results show that the light transmittance of the UV-resistant PCU sample is about 90% in the visible light range. Moreover, the UV-resistant PCU shows excellent mechanical properties with elongation at break respectively higher than 580% and tensile strength transcending 50 MPa. After UV irradiation for 192 h, the tensile strength as well as the elongation at break of the PCU sample without R455 of the original values are respectively reduced to simply 60.8% and 62.7%. Whereas the introduction of R455 gives the PCU sample excellent UV resistance, the PCU sample with 1.5% R455 is respectively about 99.0% and 92.8%. These samples can be used in various fields with both UV resistance and optical requirements.
研究领域:
材料科学
·
高分子科学
·
涂层技术
·
光学材料
·
机械工程
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Xiaobin Zhou,Dan Wang,Zhuo Wang,Zongqiang Zhu,Yinming Fan,Dunqiu Wang,Bihong Lv,Shengpeng Mo,Yanan Zhang,Yinian Zhu,Guohua Jing
Secondary amines are highly suitable candidates for constructing non-aqueous phase change absorbents (PCAs) that boast low viscosity and regeneration heat. However, the secondary amine-based PCAs often encounter the challenge of inadequate phase separation. This study proposed an innovative strategy of tailoring the polarity of absorption products to facilitate the controllable phase transition of the secondary amine-based PCA. Specifically, using aminoethylethanolamine (AEEA) as a regulator of product polarity to endow the 2-(ethylamino)ethanol (EAE)/pentamethyldiethylenetriamine (PMDETA)/dimethyl sulfoxide (DMSO) non-aqueous absorbent with tunable liquid–liquid phase transition behavior. The AEEA/EAE/PMDETA/DMSO (A/E/P/D) PCA realized a high CO 2 loading of 0.77 mol·mol −1 , with over 92% of the absorbed CO 2 being enriched in the CO 2 -rich phase, which exhibited a low viscosity of 13.83 mPa·s. The A/E/P/D PCA also possessed good reusability, maintaining a cyclic loading of 0.65 mol·mol −1 even after five absorption–desorption cycles. Analysis of the phase change mechanism indicated that AEEA reacted with CO 2 to form highly polar AEEA-derived products, which played a pivotal role in driving the phase transition of the A/E/P/D system. In brief, the AEEA-derived product easily combined with polar DMSO , creating a “polar sink” that continually attracted the medium-polar EAE-derived products. Consequently, these products clustered together to form the CO 2 -rich phase with less polar PMDETA being isolated to form the CO 2 -lean phase. Moreover, estimation of the regeneration heat demonstrated that the combined sensible heat and latent heat of A/E/P/D amounted to 0.32 GJ·ton −1 CO 2 , representing a significant reduction of 84% compared to 30 wt% MEA. This study provided a novel idea to manipulate the phase behavior of PCAs and offered a promising A/E/P/D PCA for energy-efficient CO 2 capture.
研究领域:
化学工程
·
环境科学
·
量子化学
✓ 已验证
产品关联
DOI
高影响因子
CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2016
·
IF 1.207
Jie Wang,Wenqi Zhong
Experiments on simultaneous absorption of SO 2 and NO X from sintering flue gas via a composite absorbent NaClO 2 /NaClO were carried out. The effects of various operating parameters such as NaClO 2 concentration ( m s ), NaClO concentration ( m p ), molar ratio of NaClO 2 /NaClO ( M ), solution temperature ( T R ), initial solution pH, gas flow ( V g ) and inlet concentration of SO 2 ( C S ) and NO ( C N ) on the removal efficiencies of SO 2 and NO were discussed. The optimal experimental conditions were determined to be initial solution pH = 6, T R = 55 °C and M = 1.3 under which the average efficiencies of desulfurization and denitrification could reach 99.7% and 90.8%, respectively. Moreover, according to the analysis of reaction products, it was found that adding NaClO to NaClO 2 aqueous solution is favorable for the generation of ClO 2 and Cl 2 which have significant effect on desulfurization and denitrification. Finally, engineering experiments were performed and obtained good results demonstrating that this method is practicable and promising.
研究领域:
环境工程
·
化学工程
·
能源技术
·
污染控制
·
工业生态学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Shuai Wang,Guangyi Cui,Yue Gu,Zhixuan Ma,Jing Wang,Shufeng Shen
Water-lean liquid–liquid biphasic absorbents have recently received increasing attention due to the potential advantages for capturing low CO 2 concentration flue gas with high efficiency in capture rate and energetic aspects. However, performance assessment has rarely been performed in a lab-scale continuous and integrated capture plant. In this work, a water-lean biphasic system containing 2-(methylamino) ethanol (M), diglyme (D) and water (H) was proposed for about 5 vol% CO 2 exhaust gas treatment based on the batch absorption–desorption capture tests. Integrated phase changing capture process using the developed absorbent formulation 40 M−50D−10H (WLS-10C) was demonstrated in a lab-scale CO 2 capture plant over 200 hrs testing. Energetic and capture performance as well as operational stability were evaluated and compared with aqueous 30 mass % MEA under the same targeted capture rate (about 90 %). The stable phase change behavior after CO 2 absorption was observed in the phase separator, and the CO 2 rich phase can be effectively regenerated at 393 K, forming a monophasic solution in the feed tank with the CO 2 lean phase from the separator for solvent reuse. This biphasic WLS-10C can reduce the energy consumption by about 45–55 % compared with aqueous MEA at about 90 % capture rate, demonstrating a pronounced energy-saving effect. Moreover, volumetric mass transfer coefficient and viscosity were also discussed. These findings provide valuable insights into the further pilot demonstration of the proposed biphasic absorbent.
研究领域:
化学工程
·
环境科学
✓ 已验证
DOI
高影响因子
Scientific Reports
·
2024
·Vol. 14
·期 1
·1-16
·
IF 3.8
Wang Qian,Gong Dehong,Zhang Zhongxiao,Zhu Jiangdong,Luo Qingling
The high energy consumption of Carbon Capture Utilization and Storage(CCUS) promotes the research of integrated absorption and mineralization technology. A novel DEEA/AEP biphasic absorbent is used to absorb \(\hbox {CO}_{2}\) . After phase separation, only one phase enriched with the absorption product is sent into the mineralization system, then reacts with \(\hbox {Ca(OH)}_{2}\) to produce \(\hbox {CaCO}_{3}\) at normal temperature and pressure. The effects of temperature, Ca/C and dispersion of the system were investigated, and cyclic utilization experiment was also conducted. The process was characterized and analyzed by Thermal gravimetric analysis (TGA), X-ray diffraction (XRD), and nuclear magnetic resonance ( 13 C NMR). The results showed that at 50 \(^{\circ }\) C, Ca/C = 1, the extent of mineralization of \(\hbox {CO}_{2}\) -enriched phase mineralization was 95.73% after ultrasonic treatment for 30 min. During 6 cycles, the volume percentage of \(\hbox {CO}_{2}\) -enriched phase could be maintained at 52–55%, and the \(\hbox {CO}_{2}\) load was 11.92mol/L. The results above indicate that the \(\hbox {CO}_{2}\) -enriched phase mineralization technology after absorption by biphasic absorbent can effectively capture \(\hbox {CO}_{2}\) , realize recycling, and reduce CCUS energy consumption.
研究领域:
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Nanoscale
·
2024
·
IF 5.8
Shuxin Sui,Fengjiao Zhao,Tianfu Zhang,Zhen Chen,Hongming Yin
Superabsorbers have been widely used in industrial and daily chemical products. Polymerized sodium acrylate (PAA-Na) is the most popular superabsorber used in diapers. Here we report the enhanced photodegradation of PAA-Na via carbon dots (CDs) in aqueous solutions. For a system comprising PAA-Na and CDs, CDs act as photosensitizers which improve the photodegradation efficiency by ∼5.6% compared with PAA-Na alone. Moreover, for PAA-Na+TiO2+CDs system, CDs also play the role of transfer stations of excited electrons which facilitate electron transfer from TiO2 nanoparticles (NPs) to PAA-Na and further boost the photodegradation efficiency of PAA-Na by ∼9.8%. Based on the spectral results, electrons can hardly transfer from TiO2 NPs to PAA-Na directly even with a bigger driving force compared with CDs; however, CDs can provide effective electron transfer channels within CDs-TiO2 NPs and CDs-PAA-Na which finally build an efficient pathway for electron transfer from TiO2 NPs to PAA-Na. This study reveals the great potential applications of CDs in photodegradation fields as photosensitizers or mediators to promote electron transfer efficiency.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
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.
研究领域:
化学工程
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
ENERGY
·
2024
·
IF 9
Fanli Meng,Kun Fu,Xueli Wang,Bonan Ye,Pan Zhang,Lemeng Wang,Dong Fu
Previous work has shown that non-aqueous absorbent composed of dimethyl sulfoxide (DMSO) and 2-ethylhexylan-1-amine (EHA) is superior to commercial monoethanolamine (MEA) in both absorption of CO 2 and desorption. However, the price of DMSO is too high, which leads to the high cost of reagents. It is worthwhile to choose a cheap solvent instead of DMSO, which can also achieve satisfactory absorption and desorption performance. Around this goal, we selected diethylene glycol diethyl ether (DEGDEE) to form a non-aqueous absorbent with EHA and investigated the absorption and desorption performance. The desorption efficiency of 70 wt% EHA +30 wt% DEGDEE was 99 % at 373 K. The desorption efficiency was 89.4 %, and the desorption energy consumption was only 45.1 % of MEA when the water content was 10 wt%. DEGDEE can achieve similar or even better performance than DMSO, while the cost of DEGDEE (12000–31000 RMB/ton, technical grade purity 99 %) is lower than DMSO (40000–48000 RMB/ton, technical grade purity 99 %). In addition, it also has a good recycling capacity. These advantages will certainly endow this newly developed absorbent with great application prospects in the field of CO 2 capture.
研究领域:
化学工程
·
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）