AICHE JOURNAL
·
2020
·Vol. 66
·期 6
·e16936
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IF 3.519
Xiaomin Zhang,Wenjie Xiong,Lingling Peng,Youting Wu,Xingbang Hu
Recently, the selective removal of H 2 S and CO 2 has been highly desired in natural gas sweetening. Herein, four novel azole-based protic ionic liquids (PILs) were designed and prepared through one-step neutralization reaction. The solubility of H 2 S (0–1.0 bar), CO 2 (0–1.0 bar), and CH 4 (0–5.0 bar) was systematically measured at temperatures from 298.2 to 333.2 K. NMR and theoretical calculation were used to investigate the reaction mechanism between these PILs and H 2 S. Reaction equilibrium thermodynamic model (RETM) was screened to correlate the H 2 S solubility. Impressively, 1,5-diazabicyclo[4,3,0] non-5-ene 1,2,4-1H-imidazolide ([DBNH][1,2,4-triaz]) shows the highest H 2 S solubility (1.4 mol/mol or 7.3 mol/kg at 298.2 K and 1.0 bar) and superior H 2 S/CH 4 (831) and CO 2 /CH 4 (199) selectivities compared with literature results. Considering the excellent absorption capacity of H 2 S, high H 2 S/CH 4 , and CO 2 /CH 4 selectivity, acceptable reversibility, as well as facile preparation process, it is believed that azole-based PILs provide an attractive alternative in natural gas upgrading process.
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JOURNAL OF THE ELECTROCHEMICAL SOCIETY
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2020
·Vol. 167
·期 6
·066506
·
IF 3.721
Liang Qian,Xiaojing Lv,Mi Ouyang,Alexey Tameev,Qian Bi,Lixia Zha,Xinjia Xu,Cheng Zhang
A series of novel thiophene-triphenylamine-based ionic liquids, 1-(2-((4-(bis(4-(thiophene-2-yl)phenyl)amino)benzoyl)oxy)ethyl)-3-methyl-imidazolium tetrafluoroborate/trifluoromethane sulfonate/bis(trifluoromethanesulphonyl)imide/trifluoromethanesulfonate (TTPAC2IL-BF4, TTPAC2IL-PF6, TTPAC2IL-TFSI, TTPAC2IL-TOF) were designed and synthesized successfully. All the monomers exhibit similar electrochemical behaviors together with similar HOMO and LUMO energy levels due to the same conjugated triphenylamine and thiophene units while they present different hydrophilic/hydrophobic behaviors due to different anions. FT-IR and XPS spectrum indicate the anion exchange during the electropolymerization process of monomers. In order to prepare polymeric ionic liquid films with different anions, PTTPAC2IL-BF4 (TBAP), PTTPAC2IL-BF4 (LiClO4) and PTTPAC2IL-BF4 (LiBF4) were obtained by employing TTPAC2IL-BF4 as monomer while TBAP, LiClO4 and LiBF4 were used as electrolytes respectively. Their electrochemical and electrochromic properties were also further studied. The results imply that the polymeric ionic liquid films with pendent ClO4− anions exhibit faster switching time due to the better ion diffusion character. However, PTTPAC2IL-BF4 (LiBF4) film presents better cyclic stability due to the smaller anion size of BF4− anion during the doping/dedoping process. It is more intriguing that these thiophene-triphenylamine-based PILs could exhibit electrochromic behavior in free electrolyte. This work further broadens the application of PILs as electrochromic materials and provides great comprehension on the influence of pendent anions on PILs' properties.
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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 .
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2020
·
IF 5.162
Liurong Huang,Wenxue Zhang,Dongguang Yan,Lixin Ma,Haile Ma
The aim of this study was to evaluate the effects of ionic liquids (ILs) and ultrasound on the solubility and aggregation behavior of soy protein isolate (SPI). A variety of ILs were tested. Results showed that changes in cation or anion altered the physicochemical properties of ionic liquids, which in turn influenced the solubility of SPI. High concentration of ILs resulted in the formation of insoluble aggregates, which lead to the decrease of solubility. In most of the cases, ultrasound pretreatment had a considerable impact on the solubility and aggregation of SPI. The solubility of SPI processed by combination of 1 mg/mL 1-butyl-2,3-dimethyl imidazolium chloride ([BDMIM]Cl) and ultrasound changed remarkably compared with single ultrasound and single [BDMIM]Cl processing, which was increased by 71.8% compared with that of control ( P < .05). Changes in particle size, intrinsic fluorescence spectra and free sulfhydryl (SH) groups indicated that the structure of SPI refolded and reaggregated after the ultrasound and ILs pretreatments. Combined ultrasound and 1 mg/mL [BDMIM]Cl pretreatment showed a synergistic effect on changing the SPI microstructure. In conclusion, ultrasound-assisted ILs could be an effective modification method for the globular proteins .
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CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Yiwen Zhang,Bo Yuan,Yuqing Zhang,Qiping Cao,Chao Yang,Yao Li,Jinghui Zhou
Trees are made of cellulose, hemicellulose and lignin linked by covalent bonds and supramolecular interactions. Among them, the lignin with three-dimensional structure plays a role in supporting the structure of the tree. Inspired by the nature of the tree, we have designed and synthesized a novel lignin/poly(ionic liquids) composite hydrogel dressing with excellent mechanical strength, self-healing properties, bactericidal activity, and antioxidant activity. This self-healing hydrogel dressing is obtained by the supramolecular interactions between the lignin/poly(ionic liquids) compounds. The introduction of lignin can effectively improve the mechanical properties of the hydrogel dressing. And the bactericidal poly (ionic liquid) modified on the lignin surface through covalent bonds endows this hydrogel dressing good antibacterial activity and self-healing properties. Wound healing model of rats and histomorphological evaluation results suggest that this hydrogel dressing promotes wound healing. Furthermore, the hydrogel dressing still maintains its excellent performances after simple high-temperature disinfection, and can be reused for many times.
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ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Shaocong Duan,Qing Sun,Gang Liu,Jianguo Deng,Xiangxin Meng,Bo Shen,Die Hu,Bonan Kang,S. Ravi P. Silva
Organic–inorganic hybrid perovskite solar cells are fabricated using polycrystalline perovskite thin films, which possess high densities of point and surface defects. The surface defects of perovskite thin films are the key factors that affect the device performance. Therefore, the reduction of harmful defects is the primary task for improving device performance. Therefore, in this study, high-quality perovskite thin films are prepared using an ionic liquid, dithiocarbamate diethylamine (DADA), to passivate the interface. The electron-rich sulfur atom in the DADA molecule chelates with the uncoordinated lead ion in the perovskite films, and the diethylammonium cation forms a hydrogen bond with the free iodine ion, which further improves the passivation. The synergistic passivation and improved morphology of the perovskite thin films substantially reduce the number of charged defects on the film surface and prolong the carrier lifetime. In addition, the DADA surface treatment increases the work function of the perovskite film, which is beneficial for carrier transport. Under standard solar-lighting conditions, the power conversion efficiency (PCE) of the device increases from 19.13 to 21.36%, and the fill factor is as high as 83.17%. Owing to both the hydrophobicity of DADA molecules and the passivation of ion defects, the PCE of the device remains above 80%, even for the device stored for 500 h in air at a relative humidity of 65%, and the device stability is substantially improved.
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RSC Advances
·
2023
·Vol. 13
·期 40
·27865-27872
·
IF 3.9
Fan Wang,Shuai Zhang,Congxia Xie,Xin Jin
Herein, based on the concept of integration of phosphine ligands and ionic liquids (ILs), a class of chiral phosphine-functionalized polyether ionic liquids (CPF-PILs) were synthesized by ion-exchange reaction between polyether imidazolium ILs and a phenyl-sulfonated (S)-(−)-2,2′-bis(diphenylphosphino)-1,1′-binaphthyl (BINAP) chiral diphosphine ligand, and employed in the Ru-catalyzed homogeneous asymmetric hydrogenation of β-keto esters. The resulting CPF-PILs combined the dual functions of the chiral phosphine ligand and ILs, allowing efficient recovery and recycling of the chiral catalysts using only a catalytic amount of CPF-PILs. The effects of various factors, including the chiral catalyst structure, solvent properties, reaction temperature, hydrogen pressure, and hydrobromic acid dosage, on catalytic performance were thoroughly investigated, as well as the cycling stability and universality of the chiral catalysts were examined. The findings of the present study demonstrated that, under optimal reaction conditions, the model substrate methyl acetoacetate underwent quantitative conversion to methyl β-hydroxybutyrate with a 97% enantiomeric excess (ee). The chiral catalyst used in this process can be recycled up to 12 times and showed good applicability to structurally various β-keto esters. The present study presents a novel approach for using ILs in asymmetric hydrogenation reactions in an environmentally friendly manner.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Yi Liu,Shuangjiang Li,Ying Chen,Tianding Hu,Manoj Pudukudy,Lan Shi,Shaoyun Shan,Yunfei Zhi
The chemical conversion of carbon dioxide (CO 2 ) into highly value-added products not only alleviates the environmental issues caused by global warming but also makes an impact on economic benefits in the world. The synthesis of cyclic carbonates by the cycloaddition of CO 2 with epoxides is one of the most attractive methods for CO 2 conversion. However, the development of green and highly efficient heterogeneous catalysts is considered to be a great challenge in catalysis. In this work, alkenyl-modified melamine-based porous organic polymer (MPOP-4A) was firstly synthesized by a one-pot polycondensation method, and it was again modified with imidazolium-based ionic liquids to obtain final modified catalyst (MPOP-4A-IL). Various analytical techniques were used to confirm structure and chemical composition of the prepared materials. The MPOP-4A-IL catalyst synthesized by the post-modification strategy with imidazolium-based ionic liquids exhibited enhanced catalytic activity for CO 2 cycloaddition reaction. The enhanced catalytic performance could be attributed to the presence of abundant active sites in their structure such as hydrogen bond donors (HBD), nitrogen (N) sites, and nucleophilic groups for an effective chemical reaction. The MPOP-4A-IL catalyst was found to be metal-free, easy to recycle and reuse, and has good versatility for a series of different epoxides. The interaction of MPOP-4A-IL catalyst with epoxide and CO 2 was further verified by density functional theory (DFT) calculations, and the possible mechanism of the CO 2 cycloaddition reaction was proposed.
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JOURNAL OF APPLIED POLYMER SCIENCE
·
2023
·
IF 3
Zexi Wu,Caijie Shi,Tao Peng,Qiannan Cheng,Qingquan Tang,Luoxin Wang,Hua Wang,Siwei Xiong
Liquid crystal aromatic polyesters (LCAPs) have been used in wide applications, such as chip packaging and airship skin. The traditional polymerization of LCAP is catalyzed by inorganic salts, for example, sodium acetate. Herein, we reported three kinds of ionic liquids (ILs) as catalysts to promote LCAP polymerization for the first time. The effects of ILs on the polymerization behaviors are investigated by in situ observing the liquid crystal (LC) phase behaviors based on the thin-film polymerization technique. The evolution of LC phase over time was detailly investigated by analyzing the emergence, fusion, and growth of LC phase. The temperature from 170 to 210°C and the catalyst concentration in range from 0 to 0.5 wt% are compared, showing that temperature at 210°C and catalyst concentration at 0.5 wt% are the best polymerization conditions for all ILs catalysts. In comparison with trimethylsulfonium iodide and piperidine acetate, 1-ethyl-3-methylimidazolium acetate has the best catalytic effect for the polymerization of LCAP in all experimental conditions. The successful polymerization was confirmed by FT-IR spectra, showing the increased intensity of vibration peak at 1735 cm −1 attributed to the generation of ester groups while the decreased intensities of vibration peaks at 1759 and 1370 cm −1 .
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Molecular Catalysis
·
2023
·
IF 4.6
Chan Meng,Heming Zhang,Qian Su,Hanwen Yan,Changyuan Du,Yunong Li,Li Dong,Weiguo Cheng
In view of the harsh conditions of cyclic esterification reaction of ethylene glycol (EG) and carbon dioxide (CO 2 ) to synthesize ethylene carbonate (EC), the yield is low and the catalysts are mostly metals, a series of green acid-base bicentric ionic liquids (ABbILs) were developed. Among them, the ABbILs of 1,5,7-Triazabicyclo[4.4.0]dec‑5-ene glutarimide ([TBDH][Glu]) had the best catalytic performance. Under the optimal reaction conditions, the yield of EC reached 29.5%, which was higher than most of the conventional metal-based catalysts. Through activity screening results and DFT calculation, it was found that different cations affect the interaction between N on anion and H proton of EG, and the H on the cation can activate the O on EG, which would affect the ability of ABbILs to activate EG. The acid-base bicentered synergistic catalytic mechanism of Bronsted acid and Lewis base was proposed by characterization and DFT calculation. This study opens up new avenues for the efficient conversion of diols and CO 2 for the preparation of cyclic carbonates.
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ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Hongxing Yuan,Wei Gao,Jianqi Ye,Tuotuo Ma,Fangyuan Ma,Dan Wen
Modulating the surface properties of electrocatalysts with ligands could effectively regulate their catalytic properties, while limited in-depth understanding of the surface ligands restricted their rational combination. Herein, ionic liquids (ILs) with different lengths of hydrophobic side chains were employed to regulate the surface hydrophobicity of noble metal aerogels, for comprehending the relationship between surface hydrophobicity and oxygen reduction reaction (ORR) activity and enhancing electrocatalytic ORR. The volcano-like trends between the hydrophobicity and the ORR activity for various Pt-based aerogels indicated that a suitable hydrophobic surface constructed by ILs was most favorable for contacting with oxygen molecules and the desorption of oxygen intermediates. Typically, the PtPd aerogel modified by ILs (PtPd aer-[MTBD][PFSI]) exhibited an inspiring ORR activity, with a 70 mV increase in half-wave potential and a 7.1-fold mass activity compared to the commercial Pt/C. Therefore, the regularity between the surface hydrophobicity and ORR activity of noble metal aerogels was uncovered and will facilitate the modulation of electrocatalysts for practical applications.
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CHEMICAL ENGINEERING SCIENCE
·
2023
·
IF 4.7
Xinyu Li,Xiaojia Wu,Hui Yu,Chuanqi Geng,Haiguo Wei,Zhiyong Zhou,Zhongqi Ren
Based on the structural designability of ionic liquids (ILs), 1,8-diazabicyclo[5.4.0]undec-7-ene (DBU)-based ILs ([Bz-DBU]NTF 2 ) were designed and synthesized. Their physical properties were analyzed by FT-IR, 1 H NMR, DSC and TGA. Highly selective separation between aromatic and alkane by [Bz-DBU]NTF 2 was achieved. Under the optimal conditions, the distribution coefficient ( D ) and separation selectivity ( S ) of [Bz-DBU]NTF 2 for tetraline were 0.833 and 54.2. The IL was regenerated six times without decrease in separation selectivity, demonstrating good stability. For the multi-component simulated diesel, nearly 100% of the bicyclic alkanes could be removed by five-stage cross-flow extraction processes. While the removal rate of total aromatics reached up to 84.39 and the contents of alkanes and total saturated alkanes reached 56.64% and 96.69%, respectively. For the real diesel, after two-stage cross-flow extraction experiments, the removal rates of monocyclic, bicyclic, tricyclic aromatic hydrocarbons reached 63.9%, 91.3% and 100%, respectively. The final product reached the standard of high quality ethylene cracking feedstock.
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