ChemSusChem
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2017
·Vol. 10
·期 17
·3368-3377
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IF 7.226
Yuhui Li,Mohammad Chand Ali,Qiwei Yang,Zhiguo Zhang,Zongbi Bao,Baogen Su,Huabin Xing,Qilong Ren
Graphical Quick on the uptake : A flexible hydrogen-bonded supramolecular network in hybrid deep eutectic solvents (DESs) enables strong physical solvation of NH 3 to achieve high and reversible NH 3 uptake. The unique hybrid DESs showed superior desorption–regeneration performance as well as superb NH 3 /CO 2 selectivity. Serious environmental concerns have led to a great demand for efficient uptake of NH 3 by solvents. However, traditional aqueous absorbents have many shortcomings and efforts to use ionic liquids have met with limited success. A hybrid deep eutectic solvents (DESs) designed with a flexible hydrogen-bonded supramolecular network exhibits both exceptional NH 3 uptake capacity and superior desorption–regeneration performance, along with superb NH 3 /CO 2 selectivity and environmental merit. Elucidated by molecular dynamic simulations and spectroscopic analysis, the abundant hydrogen-bonding sites in the hybrid DESs bind every atom of the NH 3 molecule and enable strong physical reversible solvation, whereas the multiple interactions among the hybrid components create a flexible hydrogen-bonded supramolecular network and allow for solvent-unbreaking absorption to ensure the full participation of the solvent and process stability. A mass solubility of NH 3 up to 0.13 g g −1 was achieved at 313 K and 101 kPa by the hybrid DES choline chloride/resorcinol/glycerol (1:3:5), which is higher than all reported ionic liquids and ordinary DESs. Moreover, the performance remained the same after ten absorption–desorption cycles and the DESs could be easily regenerated.
研究领域:
化学工程
·
环境科学
✓ 已验证
DOI
高影响因子
ENERGY & FUELS
·
2019
·
IF 3.021
Haiming Zhang,Bin Jiang,Na Yang,Na Zhang,Luhong Zhang,Zhaohe Huang,Xiaoming Xiao,Xiaowei Tantai
Ionic liquid (IL) aqueous solutions (aq) have emerged as promising candidates for SO2 absorption. In this work, a new series of diamino polycarboxylate protic ionic liquids (DPPILs) aq with low viscosities and high stabilities were developed and used for SO2 capture. All of the prepared absorbents could efficiently absorb low-concentration SO2 in simulated flue gas. Among them, DPPILs aq based on citric acid (CA) presented the most excellent SO2 desorption performance; nearly all absorbed SO2 could be easily desorbed under mild conditions. Particularly, N,N-dimethylethylenediamine citrate [DMEDA][CA] showed the highest available absorption capacity toward 0.2 vol % SO2 (up to 0.51 molSO2/molILs and 0.058 gSO2/gabs in 50 wt % aq at 20 °C), which also presented satisfactory SO2/CO2 selectivity, reusability, and SO2 removal efficiency. Fourier transform infrared and nuclear magnetic resonance spectroscopic analyses revealed that the protonation of [DMEDA]+ and [CA]− promoted SO2 absorption. Overall, the studied DPPILs aq with excellent physical properties, SO2 absorption–desorption performance, and stability may have a great perspective in industrial SO2 removal.
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
Journal of the Taiwan Institute of Chemical Engineers
·
2014
·
IF 2.637
Shidong Tian,Yucui Hou,Weize Wu,Shuhang Ren,Jianguo Qian
In this work, three kinds of ammonium salts containing chloride ion [DETA]· n Cl ( n = 1, 2, 3) were synthesized via the reactions between diethylenetriamine (DETA) and hydrochloric acid . And ethylene glycol (EG) was chosen as a solvent to dissolve [DETA]· n Cl to prepare liquid hybrid absorbents for the capture of CO 2 . Effects of amount of chloride ion, absorption temperature, CO 2 partial pressure and [DETA]·Cl concentration on the absorption of CO 2 were systematically studied. It has been found that [DETA]·Cl (1) + EG (2) (mole ratio of EG to [DETA]·Cl R = 4.0) shows a high absorption capacity of CO 2 . The mole ratio of CO 2 to [DETA]·Cl could reach 0.765 (0.0868 g CO 2 /g absorbent) at 50 °C under atmospheric pressure. Importantly, the viscosity of [DETA]·Cl (1) + EG (2) ( R = 4.0) is quite low (105.3 mPa s) even when it is saturated with CO 2 at 50 °C. Finally, [DETA]·Cl (1) + EG (2) ( R = 4.0) could be reused to absorb CO 2 for five times without obvious loss of absorption capacity. The result indicates that [DETA]·Cl (1) + EG (2) is a promising reversible absorbent for the capture of CO 2 .
研究领域:
化学工程
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2018
·
IF 6.735
Dongshun Deng,Bao Gao,Chao Zhang,Xiuzhi Duan,Yanhong Cui,Jingheng Ning
Ammonia (NH 3 ) is not only a harmful gas to environmental problem, but also a fundamental raw material in chemical industry. The effective separation and recovery of NH 3 from exhaust gas at low cost still remains a challenge for a long time. In this study, a new strategy to construct protic deep eutectic solvents (DESs) by paring NH 4 SCN as hydrogen-bond acceptor with various hydrogen-bond donors [glycerol (G), ethylene glycol (EG), urea (U), acetamide (AT), and caprolactam (CL)] was proposed for efficient and reversible absorption of NH 3 . Results showed that all the DESs possessed exceptional NH 3 absorption capacity and high NH 3 /CO 2 selectivity. At 303 K and 0.10 MPa, the absorption capacity of NH 3 in NH 4 SCN-glycerol (2:3) is as high as 0.223 g NH 3 per g DES, which is much higher than all reported functional ILs and DESs up to date. The NH 3 saturated DES was easily regenerated and recycled 25 times with persistent absorption performance. The influences of DES composition, temperature, NH 3 partial pressure on NH 3 absorption performance were also explored in detail. The absorption mechanism was analyzed using NMR spectroscopy and quantum calculation. These protic NH 4 SCN-based DESs presented as promising absorbents for NH 3 because of their high absorption capacity and good reversibility.
研究领域:
环境化学
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分离科学
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绿色溶剂
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气体吸收
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化学工程
✓ 已验证
DOI
高影响因子
ENERGY & FUELS
·
2018
·
IF 3.024
Kai Zhang,Yucui Hou,Yiming Wang,Kun Wang,Shuhang Ren,Weize Wu
Extremely low-volatility functional deep eutectic solvents (DESs), based on ethylene glycol (EG) and diethylene glycol (DG) as hydrogen-bond donor and the ammonium salts obtained from triethylenetetramine (TETA) and HCl at different mole ratios as hydrogen-bond acceptor, were designed and used to capture CO2. All of the designed DESs can efficiently capture CO2 even at low partial pressures. CO2 absorption capacity of [TETA]Cl-EG DES with n[TETA]Cl/nEG 1:3 is high up to 17.5 wt % (1.456 mol CO2/mol [TETA]Cl) at 40 °C and 1 atm. CO2 absorption capacity decreases with increasing temperature and decreasing CO2 partial pressure. Regeneration experiments show that CO2 absorption capacities in [TETA]Cl-EG DES and [TETA]Cl-DG DES do not vary after five absorption/desorption cycles. It is found that EG or DG can increase the absorption capacity via activating −NH– or −NH2 on [TETA]Cl and enhance the basicity of DESs. In addition, CO2 absorption mechanism in [TETA]Cl-EG DES based on the change of its viscosity during absorption and FTIR analysis indicates that there is a chemical interaction between CO2 and [TETA]Cl, and the stoichiometry for the reversible absorption is 1.5 molecules of CO2 per [TETA]Cl-EG DES molecule.
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
JOURNAL OF MOLECULAR LIQUIDS
·
2024
·
IF 5.3
Huifang Guo,Jia Liu,Yunlong Shi,Xiaohong Xie
In this study, bio-based pyrrolidone (2-Pyr) and low-toxicity tetraethylammonium chloride (TEAC) were selected to prepare inexpensive, low-viscosity deep eutectic solvents (DESs), which is in line with the concept of green and sustainable chemistry and is suitable for industrial production. The highest absorption capacity of TEAC:2-Pyr (1:4) was determined to be 1.03 g SO2 /g DES at 20 °C. Eight absorption–desorption cycling tests were performed, and it was found that the absorption performance of DESs for SO 2 slightly varied. It was also proved that DESs have a certain degree of water resistance and high SO 2 selectivity. Fourier transform infrared spectroscopy and computational chemical analysis showed that the DESs composed of TEAC:2-Pyr formed intermolecular hydrogen bonds, the O atoms in Cl − and 2-Pyr played a role in the absorption of SO 2 , and hydrogen bonds were broken by the addition of SO 2 .
研究领域:
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2020
·
IF 5.774
Pengfei Li,Dawei Shang,Wenhui Tu,Shaojuan Zeng,Yi Nie,Lu Bai,Haifeng Dong,Xiangping Zhang
Ammonia (NH 3 ) is one of the main reasons for the formation of aerosols. NH 3 pollution mainly comes from a large amount of emissions in industrial production. Ionic liquids (ILs), as a green solvent, can efficiently separate and recover NH 3 from industrial NH 3 -containing tail gas. In this work, novel protic ionic liquids (PILs) with hydrogen bond donating ability were designed and synthesized by incorporating six-membered N -heterocyclic compounds including pyridinium and piperidinium as cations. Three pyridinium-based PILs with single protic H showed higher NH 3 capacity with the maximum of 3.078 mol NH 3 /mol IL at 313.1 K and 0.10 MPa than the piperidinium-based PILs with double interaction sites. However, there was obvious reduction in NH 3 capacity for pyridinium-based PILs during absorption and absorption-desorption cycles. The reason is that the acidic protic H of cations of pyridinium-based PILs is easily stripped in supersaturated alkaline environment due to the smaller p K a of pyridine derivatives than that of NH 3 , forming the NH 4 + and volatile neutral pyridine derivatives. This work will provide useful guidance to the design of novel ILs used for efficient and reversible absorption of NH 3 .
研究领域:
环境科学
·
化学工程
✓ 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）