SEPARATION AND PURIFICATION TECHNOLOGY
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2023
·
IF 8.6
Yangke Long,Shixin Huang,Shiyin Zhao,Guicong Xiao,Jianlin Sun,Dan Peng
The practical application of periodate-based advanced oxidation technologies (PI-AOTs) for wastewater treatment requires efficient and cost-effective activators. Pyrolyzed Fe–N/C materials are potential candidates, however, their actual active sites and activation mechanisms are yet to be fully understood. Herein, a series of Fe–N/C samples (denoted as Fe@NC- X ) with differing structures and iron components were delicately synthesized. Experimental studies on the structure–activity relationship and density functional theory (DFT) computations revealed that Fe–N x species serve as the dominant active site for periodate activation, while the inactive iron-based particles (i.e., Fe 0 and Fe 3 C) optimized the binding affinity of surrounding carbon layers with periodate, resulting in enhanced activity. In-depth exploration of the oxidative mechanism revealed that Fe@NC- X activated periodate through an electron transfer regime. Our results also showed that the optimal Fe@NC-0.2/periodate system was highly effective in catalyzing the oxidation of 4-CP, outperforming many reported activators. These findings provide an indispensable foundation for the rational development of advanced Fe–N/C activators and offer vital insights into the mechanism underlying pollutant destruction through PI-AOTs.
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JOURNAL OF SOLUTION CHEMISTRY
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2023
·Vol. 52
·期 9
·1033-1047
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IF 1.2
Li Ke,Li Renjiang,Duan Xiuzhi,Deng Dongshun
Emission of NH 3 or CO 2 containing tail gases will aggravate environmental problems of global climate warming, fog, and haze. Developing efficient absorbent for them is highly desirable. In present work, new type V pyrazole (Py)/glycerol (Gly) DESs with Py/Gly molar ratios of 1:1 and 1:2 were prepared. Their densities and viscosities with temperature were measured. The solubilities of NH 3 or CO 2 in two DESs were determined, with the near atmospheric solubilities of NH 3 and CO 2 up to 8.7052 mol·kg −1 and 0.0395 mol·kg −1 for Py/Gly DESs (1:1), respectively. Henry’s constant and the dissolution Gibbs free energy, enthalpy, and entropy changes of gas dissolution were obtained by correlating the experimental data. What’s more, Py/Gly DESs (1:1) presents potential ability to preferentially separate NH 3 from the tail gas containing NH 3 and CO 2 due to its ideal selectivity of NH 3 /CO 2 as high as 189.
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JOURNAL OF MOLECULAR LIQUIDS
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2023
·
IF 6
Wentao Zheng,Guangwen Yu,Guibing Xia,Wanghao Shen,Weizhong Shi,Tengteng Zhou,Xiankun Wu
Developing absorbents with highly efficient nitric oxide (NO) absorption and desorption is very important for flue gas denitrification process. Toward this end, a class of DBU-based deep eutectic solvents (DESs) containing alkanones or azoles as functional HBDs for the capture of NO were synthesized in this work, with viscosities of only 7.71–45.57 mPa·s at 303.2 K. Solubilities of NO in these DESs were determined at temperatures from 303.2 to 333.2 K and pressures from zero to 1 bar. It was found that the absorbing abilities of the DESs increased with the increasing HBDs’ alkalinity. Impressively, these DBU-based DESs had remarkable larger absorption capacities than those reported DESs in the literature. According to the solubility curves of NO, chemical absorption was thought to occur accompanying with the physical one in the systems. Therefore, the reaction equilibrium thermodynamic model (RETM) was applied to model the experimental NO solubilities. The corresponding thermodynamic parameters for each system, such as the reaction equilibrium constant, Henry’s law constant, and the enthalpy change were also obtained to assess the NO absorption process in these DESs.
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ACS Sustainable Chemistry & Engineering
·
2019
·
IF 6.97
Junhai Wu,Bihong Lv,Xiaomin Wu,Zuoming Zhou,Guohua Jing
A series of novel dual-functionalized ionic liquids (FILs) with the combinations of diethylenetriamine cation ([DETAH]+) and aprotic heterocyclic anion (AHA) are explored for efficient and reversible CO2 capture, which was distinguished from the traditional strategy by increasing the amino group number of ionic liquids. The structural features and the interactions between ions and CO2 were performed under the DFT method, at the B3LYP/6-311++G** level. The CO2 absorption loadings of [DETAH][Im], [DETAH][Py], and [DETAH][Tz] were 11.91, 11.36, and 10.10 mol CO2/ kg IL, respectively. After the fifth cycle, their regeneration efficiencies still kept above 90%. Based on the calculation and 13C NMR results, the reaction mechanisms of CO2 capture into [DETAH][AHA] solutions were clarified. The amino groups of [DETAH]+ reacted with CO2 to produce [DETAH]+-carbamates, which guaranteed the high absorption rate. Meanwhile, [AHA]− could also equimolecularly react with CO2 to form carbamate, which subsequently hydrolyzes into HCO3–/CO32–. Notably, the [AHA]− was protonated during the CO2 absorption process, and [AHA]-H could react with [DETAH]+-carbamates to produce [DETAH]+, which helped to recycle the active components of the absorbent and further increased the CO2 capacity and regenerability of the absorbent. The novel dual FILs present as an efficient candidate for CO2 capture.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2019
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IF 3.375
Ying Sun,Shuhang Ren,Yucui Hou,Kai Zhang,Weize Wu
In this work, we demonstrate an innovative strategy for efficient and sustainable absorption of NO in a series of ionic liquids (ILs) containing amine groups and azole groups. The results show that the ILs have low viscosities and high performance for NO absorption. For instance, [TEPA][Im] had a high absorption capacity of 6.79 mol NO per mol IL at 30 °C and ambient pressure. The absorbed NO was easily released by heat treatment, and the regenerated IL had significant reversibility. The results of 1H NMR, UV spectra, and FT-IR spectra of ILs before and after NO absorption indicated that the absorption of NO in the [TEPA][Im] mainly resulted from a chemical interaction. NO interacts with not only the secondary amine groups in the cation but also N-imidazole in the anion through the formation of NONOate, indicating [TEPA][Im] is a dual functional IL. By introducing this efficient and reversible absorption of NO by ILs, our work broadens the method of NO capture.
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JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY
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2018
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IF 2.891
Lin Wang,Qijing Bing,Jianxin Li,Guang Wang
A symmetrical oxadiazole derivative (OXD) containing two pyrazole moieties was synthesized successfully and characterized by single crystal X-ray diffraction, nuclear magnetic resonance and mass spectrometry. The synthesized compound displayed “On-Off” fluorescent sensing towards Cu 2+ with high selectivity and sensitivity. Fluorescence and UV–vis absorbance spectra studies demonstrated that the proposed sensor can detect Cu 2+ directly in acetonitrile solution over a wide range of metal ions including Ag + , Na + , K + , Hg 2+ , Mg 2+ , Cd 2+ , Co 2+ , Ni 2+ , Zn 2+ , Fe 2+ , Pb 2+ , Ca 2+ , Mn 2+ , Ba 2+ , Fe 3+ , Al 3+ , and Cr 3+ . Moreover, the synthesized sensor exhibits an instantaneous naked-eye color change from colorless to yellow with the presence of Cu 2+ ion. The fluorescence intensity of the sensor has shown a linear response to Cu 2+ in the concentration range of 0–15 μM with a detection limit of 2.14 μM. Fluorescence titration, 1 H NMR spectrum, ESI–MS, and DFT calculation confirmed that fluorescence quenching is caused by the complex formation between the sensor and Cu 2+ with 1:1 stoichiometry.
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GREEN CHEMISTRY
·
2018
·Vol. 20
·期 18
·4236-4244
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IF 8.586
Xiaoyan Pei,Dazhen Xiong,Yuanchao Pei,Huiyong Wang,Jianji Wang
Phase separation of microemulsions plays an important role in many applications such as oil recovery, nanomaterials synthesis, and chemical reactions. However, reversible switching from ionic liquid-based microemulsions to complete oil–water phase separation has not been reported so far. In this work, we developed a novel class of stimuli-responsive microemulsions composed of CO2-responsive ionic liquids, n-pentanol and water. The microstructures and phase behavior of the microemulsion systems before and after the bubbling of CO2 were investigated by electrical conductivity, dynamic light scattering, small-angle X-ray scattering, cryogenic transmission electron microscopy, and optical microscopy. It was found that these microemulsions could be reversibly switched from W/O monophase to complete oil–water phase separation upon alternate bubbling and removal of CO2 at atmospheric pressure. Furthermore, 13C NMR spectroscopy was used to understand the CO2-driven reversible phase separation of the microemulsions. The results suggest that the mechanism behind the reversible phase separation involved the reversible formation of bicarbonate and carbamate from the reaction between CO2 and the anions of the ionic liquids in the presence of water, which resulted in the increase of ionic strength (or vice versa) in the mixture. Using the microemulsions as microreactors, the phase separation protocol was applied in the Knoevenagel reaction for an efficient coupling of a chemical reaction, product separation, and recycling of the microemulsions.
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RSC Advances
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2019
·Vol. 9
·期 15
·8529-8536
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IF 3.049
Geng Yang,Xia Meng,Shimin Fang,Hongdong Duan,Lizhen Wang,Zhenzheng Wang
An efficient fluorescent probe Pyr-Rhy based on pyrazole was developed, which can detect Hg2+ in water. Its fluorescence properties were studied by UV-vis and fluorescence spectroscopy, and the study results indicated that this probe can selectively detect Hg2+via complexation reaction, and then cause a remarkable color change from colorless to pink and a strong fluorescence enhancement can be observed. Furthermore, this probe showed high sensitivity with the detection limit down to 2.07 × 10−8 M, and its stoichiometric ratio toward Hg2+ ions was 1 : 1. The sensing mechanism was investigated by Job's plot 1H NMR titrations, and FT-IR spectra analysis, which demonstrated a chelation-enhanced fluorescence (CHEF) mechanism. More importantly, obvious color changes of sensor Pyr-Rhy can be observed when it was impregnated on filter paper testing strips and immersed in Hg2+ solution (water as solution), indicating its potential application for trace Hg2+ detection in environmental samples.
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PubMed
高影响因子
JOURNAL OF MOLECULAR LIQUIDS
·
2024
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IF 5.3
Bin Chen,Hegang Shu,Yujun Guo,Yingjie Xu
In this work, the effect of the structure and substitution of azole-based anion on the CO 2 capture and viscosity ( η ) of metal chelate-based dual functional ionic liquids (DFILs) with [K(DGA) 2 ] + cation was investigated. The CO 2 absorption capacity of DFILs at 0.1 MPa and 333.2 K shows that methyl and nitro groups on the azole-based anion, such as pyrazolide ([Pyr] − ) and imidazolide ([Im] − ), attenuate their reactivity with CO 2 through the steric hindrance and electron-withdrawing effects, respectively. Furthermore, the CO 2 absorption capacity of [K(DGA) 2 ][Pyr] is larger than that of [K(DGA) 2 ][Im], which is due to the interaction of the two adjacent N atoms in the [Pyr] − anion with CO 2 , as confirmed by DFT calculations. The CO 2 absorption mechanism shows that both [Pyr] − anion and [K(DGA) 2 ] + cation of [K(DGA) 2 ][Pyr] can chemically interact with CO 2 , making its saturated uptake at 333.2 K as high as 1.47 mol CO 2 per mole IL. Moreover, CO 2 interacts preferentially with [Pyr] − , and the [K(DGA) 2 ] + –CO 2 interaction is enhanced when the CO 2 uptake is greater than 0.5 mol CO 2 per mole IL. η of pure [K(DGA) 2 ][Pyr] is lower than that of pure [K(DGA) 2 ][Im]. η of [K(DGA) 2 ][Pyr] increases with the increase of CO 2 absorption, and the rapid increase in η after CO 2 uptake greater than 0.5 is attributed to the formation of [K(DGA) 2 ] + –CO 2 interactions.
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JOURNAL OF FLUORESCENCE
·
2017
·Vol. 27
·期 5
·1721-1727
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IF 1.461
Wang Fanwei,Duan Hongdong,Xing Dianxiang,Yang Geng
One novel turn-on fluorescence probe founded on conjugated pyrazole Schiff base for detecting Al 3+ was invented. The UV–vis and fluorescence spectrometer were employed to explore optical properties of this probe. The results got from those experiments indicated that this fluorescence probe manifested excellent sensitivity and selectivity for Al 3+ compared with other cations examined(Ag + , Co 2+ , Mg 2+ , Cu 2+ , Ni 2+ , Pb 2+ ,and Zn 2+ ). In addition, this probe displayed a more rapid response and remained stable between pH 6 and 9 by investigating the fluorescence intensity under different response time and various pH values. Remarkably, the detection limit for Al 3+ could lower to 1.0×10 −9 M. Therefore, the probe could be potentially applied to the environment for the detection of Al 3+ , and the availability in biological range of pH that could be further studied to make this probe apply to biological systems in the future.
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PubMed
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Journal of CO2 Utilization
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2017
·
IF 4.292
Yingjie Xu
Recently, chemical fixation of CO 2 catalyzed by protic ionic liquids (PILs) has been successfully achieved, suggesting that CO 2 absorption behavior plays an important role on CO 2 activation and transformation. For this reason, the influence of the alkalinity and physicochemical properties on CO 2 absorption behavior of four azole-based PILs, namely [DBNH][Pyr], [DBNH][Im], [DBUH][Pyr], and [DBUH][Im] was discussed in this work. The alkalinity of PILs was determined by potentiometric titration, and free space of PILs was evaluated by thermal expansion coefficient and refractive index. Solubility parameter of PILs was obtained from the activation energy for viscous flow. The results show that PILs with [Pyr] − exhibits stronger alkalinity and larger free space, which can help to improve CO 2 capture capacity. Whereas PILs with larger cation size [DBUH] + exerts higher viscosity, resulting in slower absorption rate of CO 2 . Furthermore, the CO 2 absorption capacity is inversely proportional to the solubility parameter of PILs. The absorption mechanism proved by FT-IR and 13 C NMR spectra indicates that [Pyr] − or [Im] − can react with CO 2 to form carbamate. Accordingly, considering the CO 2 capture capacity and absorption rate, [DBNH][Pyr] may be a good candidate for efficient CO 2 capture and activation with low enthalpy of absorption of −38.2 kJ mol −1 .
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Jiawei Ruan,Lifang Chen,Xinzi Wu,Shaokang Qian,Kunchi Xie,Xiaoyi Zhang,Hongye Cheng,Zhen Song,Zhiwen Qi
Direct synthesis of dimethyl carbonate (DMC) from CO 2 is promising for CO 2 utilization, however its efficiency remains far from industrial-scale implementation for lack of customized catalysts. Herein, a hydroxyl-functionalized ionic liquid (HFIL) was developed to enhance catalytic activity, and importantly, to facilitate IL recovery through spontaneous phase separation. A high DMC yield (6.5 g DMC ·kg cat −1 ·h −1 ) over HFIL was achieved under mild conditions compared to non- hydroxyl IL. Self-diffusion coefficients characterization revealed intensified diffusion of CH 3 OH and HFIL, alongside reduced blockage of active sites after hydroxyl functionalization. Density functional theory calculations elucidated that cation polarization induced by hydroxyl group facilitated the synergistic activation of both substrates and monomethyl carbonate intermediate. The reaction mechanism was further verified through diffuse reflectance infrared Fourier transform spectroscopy and theoretical calculations. The self-separation behavior was demonstrated by molecular dynamics simulations. The deep insights into hydroxyl effects towards direct DMC synthesis provide a pioneering perspective for CO 2 capture and utilization using functionalized ILs.
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