NEW JOURNAL OF CHEMISTRY
·
2019
·Vol. 43
·期 29
·11636-11642
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IF 3.069
Dongshun Deng,Xiuzhi Duan,Bao Gao,Chao Zhang,Xiaoxia Deng,Lei Gong
The hydrogen bond donor (HBD) glycerol (Gly) and hydrogen bond acceptors (HBA) selected among 1,2,4-triazole (Tri), imidazole (Im), tetrazole (Tz), 1-methyl-triazole (Tri-Me), 3-mercapto-1,2,4-triazole (Tri-SH), 3-amino-1,2,4-triazole (Tri-NH2), 3-cyano-1,2,4-triazole (Tri-CN), and 4-formalimidazole (Im-CHO) were paired to construct functional deep eutectic solvents (DESs) that were then utilized as ammonia (NH3) absorbents. The influences of the HBA in DESs, temperature, and partial pressure of NH3 on the NH3 absorption performance were systematically investigated. The results illustrated that all the DESs exhibited efficient and reversible absorption for NH3, and Tri–Gly possessed higher absorption capacity than Im–Gly, with the maximum absorption capacity of 0.115 gram NH3 per gram DES of Tri–Gly (1 : 3) at 313.15 K and 1.0 bar. The NH3-saturated DES could be easily recycled five times with a persistent absorption performance. The absorption mechanism was further deduced by the NMR and FTIR spectroscopy. These DESs acted as potential absorbents for NH3 due to their good absorption performance and reversibility.
研究领域:
化学工程
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环境科学
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产品关联
DOI
高影响因子
GREEN CHEMISTRY
·
2016
·Vol. 19
·期 4
·937-945
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IF 8.506
Dawei Shang,Xiangping Zhang,Shaojuan Zeng,Kun Jiang,Hongshuai Gao,Haifeng Dong,Qingyuan Yang,Suojiang Zhang
Cost-efficient and environmentally benign treatment of NH3-containing exhaust gas has been a challenge. Ionic liquids (ILs) due to their unique structures and properties are recognized as potential solvents to absorb NH3. In this study, three types of ILs, including [Bmim][NTf2], [Bim][NTf2], [HOOC(CH2)3mim][NTf2], were designed and synthesized with various hydrogen bond donating abilities and characterized based on their thermodynamic dissociation constants (pKa). The results showed that protic ionic liquid (PIL) [Bim][NTf2] with a moderate pKa value had the highest NH3 absorption capacity (up to 2.69 mol NH3 per mol IL, 313 K, 100 kPa). Experimental characterization and theoretical calculations verified that such extremely high NH3 absorption capacity for [Bim][NTf2] resulted from the interactions between H-3 on the imidazole ring and the NH3 molecule and NH3 molecules sintering themselves. Furthermore, stable absorption performance was recorded for [Bim][NTf2] over four cycles, implying potential applications in the industry for NH3 recycling.
研究领域:
化学工程
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环境科学
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产品关联
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
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2022
·Vol. 46
·期 45
·21730-21736
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IF 3.925
Ziyue Zhou,Renjiang Li,Ke Li,Kai Zong,Dongshun Deng
The efficient capture and separation of ammonia (NH3), a fundamental raw material as well as widespread pollutant, is significant in the fertilizer industry and for environmental protection protocols. In this work, several new type V deep eutectic solvents (DESs), composed of hydroxypyridine and phenol, were designed as efficient and reversible NH3 absorbents. All the DESs have low viscosity, good NH3 absorption performance and high NH3/CO2 selectivity. The optimal 3-hydroxypyridine/phenol (1 : 5) ratio could respectively capture 10.00 mol kg−1 and 4.63 mol kg−1 NH3 at pressures of 101.3 kPa and 10.0 kPa, better than most other DESs and ILs reported in the literature. The prepared DESs show satisfactory thermal stability and highly reversible absorption performance. By comprehensively analyzing the absorption behavior and spectroscopic results, the effective NH3 absorption ability of DESs was deduced being due to a relatively strong interaction between multiple weak acidic hydroxyl groups and basic NH3.
研究领域:
化学工程
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环境科学
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产品关联
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2020
·
IF 7.632
Rongxing Qiu,Xiaoyan Luo,Le Yang,Jiaran Li,Xiaoyan Chen,Cheng Peng,Jinqing Lin
In this work, flexible hydrogen-bonded frameworks composed of amino pyridinium-based protic ionic liquids (ILs) marked as [X-PyH][Tf2N] were designed as NH3 absorption agents. Interestingly, NH3 absorption isotherm of these ILs present sigmoidal absorption isotherm (S mode), and the threshold pressure (TP) decreases from 75 to 6 mbar with the tunable of hydrogen bonded frameworks by varying the substituted group X. Combined with XRD characterizations, Fourier transform infrared and 1H NMR spectroscopies, thermometric analyses, and theory calculations, it indicates NH3 fixed by these ILs via acid–base interaction as well as hydrogen bonding based on the activation of sites through the fracture of the hydrogen-bonded frameworks, which would reform along with heat release when NH3 desorption. Therefore, S mode NH3 absorption with [3NH2-PyH][Tf2N] presents low TP of 6 mbar (6000 ppm) at 30 °C, and its NH3 capacity increases sharply and followed by a continuous increase to 3.85 mol/mol IL (175 mg/g IL) at 1.0 bar, which is higher than that of the reported ILs. The fixed NH3 could be desorbed completely in vacuum at 80 °C and 1 mbar. [3NH2-PyH][Tf2N] maintained its high capacity within 20 time recycles. The sigmoidal NH3 absorption would be considered as one of the potential approaches for its simultaneous efficient absorption and energy-saving separation at low concentrations.
研究领域:
化学工程
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材料科学
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产品关联
DOI
高影响因子
JOURNAL OF MOLECULAR LIQUIDS
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2021
·
IF 6.165
Ke Li,Hao Fang,Xiuzhi Duan,Dongshun Deng
Development of high-efficient solvents for NH 3 capture to improve the quality of atmosphere and ecological environment is a hot research topic. Deep eutectic solvents (DESs) as NH 3 absorbents can overcome some problems troubling the traditional NH 3 capture process. In this work, NH 4 SCN was paired with imidazole (Im) DESs to form low viscous DESs with dual active sites for highly efficient NH 3 absorption. The effects of absorption temperature, gas flow rate, water content, molar ratio on NH 3 absorption performance as well as physical properties of NH 4 SCN/Im DESs were systematically investigated. The results show that NH 4 SCN/Im DESs can rapidly capture NH 3 with good recycling performance, while the gas flow rate only shortens the absorption time. The NH 3 absorption capacity of NH 4 SCN/Im DESs decreased with increasing temperature and NH 4 SCN/Im molar ratio. The absorption capacity of NH 4 SCN/Im (1:2) DES reaches 9.65 mol NH 3 /kg DESs for atmospheric NH 3 . Based on 1 H NMR and IR spectroscopy analysis, the strong hydrogen bond between protic ammonium cation and NH 3 plays the major essence of efficient NH 3 capture for NH 4 SCN/Im DESs.
研究领域:
环境科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
ENERGY & FUELS
·
2025
·
IF 5.3
Yuwan Zhu,Guangquan Wang,Kai Zong,Dongshun Deng
NH3 has attracted increasing attention as a fundamental material and promising hydrogen carrier. The uptake of NH3 from NH3-containing exhausted gas presents economic and environmental issues. In this study, [MEA][SCN] was paired with glycerol, acetamide, formamide, phenol (PhOH), ethylene glycol, urea, glycerolformal, or 1,3-dimethyl-2-imidazolidinone to construct deep eutectic solvents (DESs) for effective NH3 absorption and NH3/CO2 separation investigation. All of the [MEA][SCN]-based DESs exhibited good NH3 absorption and separation performance. Notably, [MEA][SCN]-PhOH (1:1) realized an atmospheric capacity of 0.2459 g of NH3·g–1 DES and NH3/CO2 selectivity of 194.53 at 303.15 K. Based on the experimental data, a new process for NH3 recovery from melamine tail gas using [MEA][SCN]-PhOH (1:1) (DES-M) was developed and simulated from operational parameters optimization, heat exchange network design, and economic evaluation. DES-M can recycle NH3 with purity of 99.6% and save 82.01% utility costs compared to the water scrubbing method. The heat integration network design in DES-M reduces 66.94% low-pressure steam and 9.00% separation costs. Specially, the optimized DES-M can exceed 59% after-tax rate of return using renewable energy.
研究领域:
化学工程
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环境科学
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产品关联
DOI
高影响因子
AICHE JOURNAL
·
2020
·Vol. 66
·期 8
·e16253
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IF 3.519
Yongkang Cao,Xiangping Zhang,Shaojuan Zeng,Yanrong Liu,Haifeng Dong,Chun Deng
The emerging of ionic liquids (ILs) provides an efficient and sustainable way to separate and recover NH 3 due to their unique properties. However, the solid or highly viscous ILs are not suitable for traditional scrubbing. Therefore, an effective strategy was proposed by combining the protic ILs (PILs) with acidic H and low viscous ethylene glycol (EG) to form IL-based deep eutectic solvents (DESs) for NH 3 absorption. The results indicated that these PIL-based DESs not only have fast absorption rate, but also exhibit exceptional NH 3 capacity and excellent recyclability. The highest mass capacity of 211 mg NH 3 /g DES was achieved by [Im][NO 3 ]/EG with molar ratio of 1:3, and was higher than all the reported ILs and IL-based DESs, which was originated from multiple hydrogen bonding between acidic H and hydroxyl groups of the DESs and NH 3 . This work will provide useful idea for designing IL-based solvents for NH 3 separation applications.
研究领域:
化学工程
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环境科学
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产品关联
DOI
高影响因子
Sustainable Energy & Fuels
·
2024
·
IF 5
Yu Cao,Kejie Jiang,Dongshun Deng
Ammonia (NH3) is one of the most important industrial chemicals and also shows potential application as hydrogen energy vector. The separation and storage of NH3 play key role for its safe transportation and effective utilization. In present study, five thiocyanate-based pseudo ionic liquids (PILs) with ultra-high NH3 absorption capacity were proposed as innovative NH3 absorbents. The effects of the cation species, temperature, and pressure on their NH3 absorption performance were experimentally evaluated. PILs involved progressive liquefaction from solid to liquid state upon integration with NH3. The outstanding NH4SCN demonstrated robust and reversible absorption capacity of 0.402 g NH3/g PIL at 303.15 K and 0.1 MPa, markedly higher than the majority of ionic liquids (ILs) and deep eutectic solvents (DESs) reported to date. Furthermore, the NH3 absorption mechanism and liquefaction process were comprehensively elucidated using NMR and FTIR spectroscopy, quantum chemical calculation, and molecular dynamics simulations. Results showed that absorption process involved six consecutive steps of NH3 adsorption, NH4+ formation via proton transfer, NH4+ diffusion, solid surface area expansion, ion migration, and final liquefaction. The binding enthalpy of NH3 was correlated with the molar capacities for PILs and exhibited moderate -58.13 kJ/mol for NH4SCN.
研究领域:
化学工程
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材料科学
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计算化学
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2020
·
IF 5.774
Qi Luo,Jingai Hao,Ligang Wei,Shangru Zhai,Zuoyi Xiao,Qingda An
Ammonia (NH 3 ) is essential for nitrogen fertilizer and is also considered as a promising energy carrier recently. In considering the role of NH 3 for energy storage, the health and environmental risks from NH 3 emission must be minimized and efficiently eliminated. To this end, a wide range of materials such as metal halides, ionic liquids and porous materials have been examined for NH 3 absorption. Deep eutectic solvents (DESs) with unique properties and low cost are considered as potential solvents for absorbing NH 3 . Herein, we report a DES composed of protic ethanolamine hydrochloride (EACl), weakly acidic resorcinol (Res) and neutral glycerol (Gly) can absorb 0.240 g NH 3 /g DES for EACl/Res/Gly (1:4:5) at 293 K and 0.1 MPa, which is much higher than most of reported DESs. The absorption mechanism of NH 3 is hydrogen-bonding interaction from the results of NMR and FT-IR spectra. The ternary DESs EACl/Res/Gly have abundant hydrogen-bonding sites to absorb NH 3 without structural damage, in which EACl and Res play a major role in the interaction with NH 3, while Gly is helpful for structural stability during NH 3 absorption. Besides, DES EACl/Res/Gly (1:4:5) has good reversibility, excellent NH 3 /CO 2 selectivity, is a potential NH 3 absorption and storage material for industrial application.
研究领域:
化学工程
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环境科学
✓ 已验证
DOI
高影响因子
JOURNAL OF MOLECULAR LIQUIDS
·
2023
·
IF 6
Ziyue Zhou,Yu Cao,Kai Zong,Dongshun Deng
In chemical industry, efficient absorption of ammonia (NH 3 ) from industrial exhaust remains a challenge and significant issue for resource utilization and pollution control. Present study proposed a new strategy to design non-ionic deep eutectic solvents (DESs) using phenolic analogues. Several phenol-based DESs with multiple acidic sites were constructed by paring catechol (Cat) or resorcinol (Res) with phenol (PhOH) and investigated as feasible NH 3 absorbents from physical property, NH 3 absorption performance, and mechanism analysis. Among the as-obtained DESs, Res/PhOH (1:3) demonstrated attractive NH 3 absorption capacity at 303.15 K (11.862 mol/kg at 101.3 kPa, and 6.391 mol/kg at 5.0 kPa), surpassing most DESs and ionic liquids (ILs) reported in the literatures. Meanwhile, it displayed good reversibility, satisfactory thermal stability, and high NH 3 /CO 2 selectivity. The mechanism of NH 3 absorption was further elucidated using FTIR and NMR spectra, and Quantum chemistry calculation, and inferred as the strong and multiple interaction between NH 3 and weakly acidic sites of DESs.
研究领域:
化学工程
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环境科学
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产品关联
DOI
高影响因子
ChemSusChem
·
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
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环境科学
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DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2021
·Vol. 45
·期 45
·21108-21115
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IF 3.591
Ziyue Zhou,Ke Li,Kai Zong,Xiaoxia Deng,Dongshun Deng
Ammonia (NH3) is not only an important basic chemical raw material but also a typical polluting gas. The separation and recovery of NH3 from tail gas is of great significance for human health and the environment. In this study, a series of protic ionic liquid-based deep eutectic solvents (PIL-based DESs) were constructed by pairing imidazolium thiocyanate ([Im][SCN]) as the hydrogen-bond acceptor (HBA) with various hydrogen-bond donors (HBDs) [glycerol (Gly), ethylene glycol (EG), formamide (FM), acetamide (AT), and caprolactam (CL)]. Their physical properties and NH3 absorption performance were systematically investigated. The results showed that [Im][SCN] played a role in chemical NH3 absorption in the PIL-based DESs, while the HBDs mainly contributed to physical NH3 capture. HBDs containing hydroxyl groups demonstrated an evident improvement in NH3 absorption capacity compared to those with amide groups. [Im][SCN]–EG (1 : 3) demonstrated the highest mass capacity of 0.233 g NH3/g DES, which exceeded those of all the other IL-based DESs and originated from the multiple interactions between the acidic H as well as the hydroxyl groups in the DES and NH3, according to the 1H NMR and FTIR spectral analysis. Furthermore, [Im][SCN]–EG (1 : 3) indicated a high NH3/CO2 selectivity of 632.2, satisfactory thermal stability and excellent recyclability. [Im][SCN]–EG DESs possess great potential as attractive absorbents in NH3 separation and recovery.
研究领域:
环境科学
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化学工程
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）