ACS Applied Materials & Interfaces
·
2026
·
IF 8.2
Sa Xue,Xiangyang Liu,Yongqi Liu,Maogang He
The construction of stable electrode/electrolyte interphases (EEIs) is crucial for the development of practical lithium metal batteries (LMBs). In this work, we designed locally concentrated ionic liquid electrolytes (signed as FPB2) based on 1,3,5-trifluorobenzene (3FB) diluent to address this challenge. The appropriate addition of 3FB encourages Li+ association with anions, creating a significant amount of anion-dominated aggregate-II solvation structure, which enables profound anion decomposition and rapid Li+ transport. In parallel, the low lowest unoccupied molecular orbital of 3FB allows for its own reductive decomposition on the lithium metal anode (LMA) surface. Benefiting from the synergistic decomposition of anions and 3FB, a uniform and stable solid electrolyte interphase (SEI) is formed on the LMA. Additionally, a thin cathode electrolyte interphase (CEI) abundant in LiF is generated on the LiFePO4 (LFP) cathode, resulting in the effective suppression of electrolyte oxidation. This dual-interphase stabilization endows impressive cycling performance in a Li/LFP full battery under demanding conditions (10.8 mg·cm–2 LFP, 50 μm Li) to achieve 81.5% capacity retention and 99.4% average Coulombic efficiency over 200 cycles. This work presents a new paradigm for electrolyte design in high-performance LMBs by exploiting a functional diluent to proactively stabilize dual EEIs.
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ACS Applied Materials & Interfaces
·
2022
·
IF 10.383
Chenhui Duan,Zihui Liang,Jinguo Cao,Bowen Jin,Yidong Ming,Shimin Wang,Binghe Ma,Tao Ye,Congcong Wu
Formamidinium (FA)-based perovskites remained state-of-the-art in the field of perovskite solar cells (PSCs) owing to the exceptional absorption and carrier transport properties, while the transition from photoactive (α-) to photoinactive (δ-FAPbI3) phase is the impediment that causes performance degradation and thus limits the deployment of FA-based PSCs. The unfavorable phase transition originates from tensile strain in the FAPbI3 crystal lattice, which undergoes structural reorganization for lattice strain balancing. In this work, we found that the ionic liquid (IL) could be used as the strain coordinator to balance the lattice strain for stability improvement of FAPbI3 perovskite. We theoretically studied the electronic coupling between IL and FAPbI3 and unraveled the originality of the IL-induced compressive strain. The strain-relaxed α-FAPbI3 by IL showed robust stability against environmental factors, which can withstand ambient aging for 40 days without any phase transition or decomposition. Moreover, the strain-relaxed perovskite films showed a lower trap density and resulted in conversion efficiency improvement from 18.27 to 19.88%. Based on this novel strain engineering strategy, the unencapsulated PSCs maintained 90% of their initial efficiency under ambient-air aging for 50 days.
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NEW JOURNAL OF CHEMISTRY
·
2022
·Vol. 47
·期 4
·1916-1924
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IF 3.925
Xiaolong Zhou,Pengrui Zhang,Qingfen Meng,Lianjing Mao,Huiqun Ju,Fei Shao,Yan Jing,Yongzhong Jia,Shuxuan Wang,Xingwu Zou,Jinhe Sun
Lithium isotopes play an essential role in the nuclear industry. The extraction method with crown ethers as extractants is considered as one of the promising methods for lithium isotope separation with good application prospects. However, the effects of crown ethers with different cavity sizes in the system containing ionic liquids on isotope enrichment in organic solution/aqueous solution have not been systematically investigated. With three typical benzo crown ethers (B12C4, B15C5 and B18C6) as extractants and the mixtures of ionic liquids and anisole as solvents, the effect of crown ethers on the extraction rate of Li+, separation factor and δ7Li variation in organic solution/aqueous solution was investigated with varied solvent composition, lithium salts and concentration of crown ethers. The order of extraction rates was: B15C5 (40.88%) > B18C6 (38.12%) > B12C4 (23.35%) and the order of isotope separation factors was: B15C5 (1.024) > B12C4 (1.023) > B18C6 (1.010) under optimized conditions. The δ7Li in aqueous solution of B15C5 systems was higher than those corresponding to the B12C4 and B18C6 system while the δ7Li in the organic solution of the B12C4 systems was more negative than those corresponding to the B15C5 and B18C6 system. So, B12C4 systems achieve better 6Li enrichment in the organic phase and B15C5 systems achieve better 7Li enrichment in the aqueous phase.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Mingxia Sun,Juanjuan Feng,Yang Feng,Xubo Xin,Yali Ding,Min Sun
The efficient sample pretreatment and high-performance chromatographic separation are essential for an accurate analysis of the complex sample. Finding a material that can apply as both sorbent for sample preparation and stationary phase for chromatography is greatly important for analytical chemistry. With a large number of active sites and designable properties, the dendrimers displayed potential performance for sample preparation and chromatographic separation. In order to improve its selectivity restricted by the limited type of functional groups (amide, ethylidene, amino groups), ionic liquid (1,1′-(1,4-butyricdiyl)bis(1-aminopropyl imidazolium)dibromide) were introduced to functionalize dendrimers. With porous silica as the base, ionic liquid-functionalized dendrimer grafted silica (SiO 2 @G1.5-IL) was obtained and characterized by X-ray photoelectron spectroscopy, elemental analyzer, as well as specific surface and porosity analyzer. The material was used as stationary phase for mixed-mode chromatography and sorbent for SPE, respectively. Under reversed-phase liquid chromatography (RPLC), it successfully separated some hydrophobic analytes (five polycyclic aromatic hydrocarbons (PAHs), two bisphenols, diphenylpropane, and diphenylmethane), by utilizing hydrophobic, π-stacking and hydrogen bonding interactions. Based on the hydrophilic effect, it could separate hydrophilic analytes (nucleosides and alkaloids), which coincident with hydrophilic interaction liquid chromatography (HILIC). And it exhibited better separation capacity than NH 2 @SiO 2 and SiO 2 @G1.5 under the above two modes. Furthermore, the thermodynamic parameters (ΔH, ΔS, and ΔG) of the above types of analytes on the SiO 2 @G1.5-IL column were also investigated in detail, revealing the controlling factors during the chromatographic separation. And the relative standard deviations (RSDs, 0.03–2.95%, n = 10) of the repeatability of chromatographic separation were satisfactory. After that, SiO 2 @G1.5-IL-based SPE column was online combined with high-performance liquid chromatography to investigate the extraction selectivity for three types of hydrophobic organic pollutants (PAHs, estrogens, and bisphenols), and compared to SiO 2 and C18 columns. According to their extraction performance, PAHs were selected as the target analytes, and the online analytical method was established. The limits of detection were as low as 0.001 μg L -1 due to the high enrichment factor reach to 3869, limits of quantity were 0.003–0.17 μg L -1 , linear ranges were from 0.003 to 15.0 µg L -1 , the adsorption capacity was 16.10 μg g −1 , as well as RSDs were 0.5–3.7%, 0.6–6.7%, and 4.2–9.0% for intraday, interday tests and reproducibility. Finally, it was applied to analyze the environmental water samples (tap water, snow water, and rainwater), and satisfactory results were obtained (spiked recoveries were 86.8%-120.9%). Therefore, SiO 2 @G1.5-IL was a powerful material that can be used for the chromatographic separation of both hydrophobic and hydrophilic samples by RPLC or HILIC mode, as well as the efficient online extraction of hydrophobic targets prior to C18 column-based high-performance liquid chromatography.
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JOURNAL OF PHARMACEUTICAL AND BIOMEDICAL ANALYSIS
·
2022
·
IF 3.571
Chengchen Zhang,Xiaofei Ma
This work presents a synergistic system for enantioseparation in capillary electrophoresis (CE) with a chiral ionic liquid (CIL) based on D-10-camphorsulfonic acid as additive and carboxymethyl-β-cyclodextrin (CM-β-CD) as the chiral selector. The proposed method showed excellent enantioseparation performance towards sixteen chiral drugs. In contrast to the single CM-β-CD system, the notably improved resolution (Rs) and selectivity factor (α) of model drugs were observed in synergistic system. Several key parameters such as CIL concentration, CM-β-CD concentration, buffer pH and separation voltage were investigated, after which Statistical Product and Service Solutions (SPSS) was used to prove the potential synergistic effect. The nuclear magnetic resonance (NMR) results further demonstrated the function of the CIL and the superiority of synergistic system. Finally, chiral impurity determination of chlorpheniramine maleate sample was successfully carried out using the established method.
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Separations
·
2022
·Vol. 9
·期 12
·441
·
IF 3.344
Xiaoman Li,Ruobing Qiao,Xuyang Jiu,Minglei Tian
(+)-catechin is one category of flavonoids in cocoa shell waste and it has been reported to have many health benefits. In order to isolate it from aqueous extracted solution of cocoa shell waste by solid phase extraction (SPE), a series of dual ionic liquids@ZIF8-covered silica were prepared as the sorbents. Regarding the operation conditions of SPE and the characteristic structure of (+)-catechin, ZIF8-covered silica was synthesized to establish a stable and porous substrate, and various dual ionic liquids with multiple properties were immobilized on substrate to obtain a high adsorption capacity. Different adsorption conditions were investigated and the highest adsorption capacity (58.0 mg/g) was obtained on Sil@ZIF8@EIM-EIM at 30 °C during 60.0 min. When the sorbent was applied in the SPE process, 96.0% of the total amount of (+)-catechin from cocoa shell waste can be isolated after several washing and elution steps. The satisfactory recoveries of 97.5–100.2% and RSDs of 1.3–3.2% revealed that the SPE process was accurate and precise. The stability of Sil@ZIF8@EIM-EIM was tested in water and the reusability was tested using repeated adsorption/desorption process. The results revealed that Sil@ZIF8@EIM-EIM as an efficient sorbent can isolate (+)-catechin from cocoa shell waste.Keywords:dual ionic liquid;ZIF8;composited silica;solid phase extraction;(+)-catechin;cocoa shell waste
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FUEL
·
2022
·
IF 8.035
Shao-Xu Mao,Qi-Hang Zhou,Hui-Li Guo,Ming Du,Wen-Shuai Zhu,Hua-Ming Li,Jing-Yu Pang,Dong-Bin Dang,Yan Bai
A novel porous phosphomolybdate-based poly(ionic liquid) catalyst containing 70 % water (PDIM-PMo-W 70% ) was assembled with H 3 PMo 12 O 40 (HPMo) and poly-[3-dodecyl-1-vinylimidazolium] bromine (PDIMBr), and characterized by FT-IR, UV–vis, XRD, XPS, Contact angle test, SEM, TEM, TGA, and N 2 adsorption–desorption analysis. The turnover frequency (TOF) value of PDIM-PMo-W 70% for (dibenzothiophene) DBT removal can reach 41.15 h −1 at 50 °C, which is 35.47 and 9.92 times higher than that of HPMo and PDIM-PMo. The catalyst could be recycled at least five times without a significant change in catalytic activity . The water content of the catalyst, reaction temperature, the molar ratio of H 2 O 2 /S, catalyst dosage and different sulfur-containing compounds upon oxidative desulfurization (ODS) performance were studied in detail. Most notably, the effects of water on the microstructure and catalytic activity of polyoxometalate-based poly(ionic liquid) were systematically investigated for the first time. As well as the water absorption behavior on the catalyst was reversible, and the dehydrated catalysts after soaking in water could still show excellent catalytic activity. In addition, a reasonable reaction mechanism was proposed with the aid of EPR analysis and radical quenching experiments.
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RSC Advances
·
2022
·Vol. 12
·期 5
·2947-2958
·
IF 4.036
Jing Wang,Chengbao Liu,Bei Qian
A novel L-histidine based ionic liquid (LHIL) was developed and successfully synthesized. Its structure was confirmed by Fourier-transform infrared spectroscopy, UV-vis spectroscopy, X-ray photoelectron spectroscopy, 1H-NMR and high-resolution mass spectrometry. The outstanding corrosion inhibition effect of the LHIL on mild steel in 1 M hydrochloric acid was thoroughly evaluated by Tafel plots, electrochemical impedance spectroscopy, and localized electrochemical strategies. The results revealed that the corrosion of mild steel was effectively suppressed by the adsorption of LHIL on its surface, and the best inhibition efficiency reached 98.8%. The adsorption behavior of LHIL on steel obeyed the Langmuir adsorption isotherm, which involved both chemisorption and physisorption. Theoretical calculations indicated the strong chemisorption of LHIL on steel, as proved by the low energy gap (ΔE = 0.0522 eV) and high binding energy (Ebinding = 303.47 kcal mol−1), which clearly confirmed the effectiveness of LHIL for steel protection.
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JOURNAL OF MATERIALS SCIENCE
·
2022
·Vol. 57
·期 16
·7896-7908
·
IF 4.682
Xu Tianye,Lu Shun,Wang Yajie,Gan Xiaoyan,Guo Liling,Liu Hanxing
Two-dimensional (2D) perovskite formed by introducing various organic spacer cations into 3D perovskite is considered to be one of the most effective methods to improve the humidity stability of perovskite materials. In order to solve the phase inhomogeneity and phase distribution nonuniformity of two-dimensional perovskites, additive engineering technique is widely used during their fabrication processes. Although many additives are proved to be effective in improving the quality of perovskite films, the mechanism of additive engineering has not been fully understood. In our work, we prepare 2D Ruddlesden–Popper perovskites based on 4-bromophenylethylammonium (BPEA) using a new additive of ionic liquids MAAc (methylammonium acetate). The (BPEA) 2 (MA) 4 Pb 5 I 16 perovskite prepared with the assistance of MAAc exhibits a stable photoelectric conversion efficiency (PCE) of 8.47%, which is much higher than the one without MAAc additive (4.79%). Besides a nearly tenfold increase in electron mobility, the unencapsulated (BPEA) 2 (MA) 4 Pb 5 I 16 -based device with MAAc additive remains 88% of its initial efficiency after 960 h exposure to air with a humidity of 20 ± 5% at room temperature, while the device without additive decreases to 63% of its initial efficiency. Meanwhile, the interactions between PbI 2 and MAAc at different temperatures and molar ratios are investigated and the formation mechanism of 2D perovskites in the presence of MAAc is proposed. It is found that an intermediate perovskite with distorted [PbI 6− x Ac x ] 4− octahedron is formed with the addition of MAAc, making the quality and photoelectric properties of the resultant films greatly enhanced.
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HIGH PERFORMANCE POLYMERS
·
2022
·
IF 1.73
Peng Qi,Hongge Jia,Qingji Wang,Guiming Su,Shuangping Xu,Mingyu Zhang,Yanqing Qu,Fuying Pei
Leakage of oily industrial waste is not only a serious environmental and ecological hazard but also poses a significant health risk to people. Membrane separation, which is cost-effective and efficient, is one of the best solutions for reducing pollution discharge through oil–water separation. In this study, polydopamine (PDA) was incorporated into electrostatically spun ionic liquid-capped polyimide (IL-PI) membranes through an in situ growth method; the membranes exhibited the strong adsorption properties of PDA. The polyimide fibers were hydrophilically modified with an IL, which contains several hydrophilic groups, and PDA. Adjusting the polymerization time resulted in the formation of a composite membrane, which could effectively separate oil–water emulsions. Scanning electron microscopy analysis showed that with an increase in the PDA coating time, the PDA content in and on the surface of the composite membrane fibers significantly increased. In addition, the surface contact angle of the membrane decreased from 72.87° to 12.06° with the addition of the PDA coating, while the wettability was significantly improved. The PDA-modified fibrous membranes showed good separation of the emulsified oil–water mixtures. The maximum membrane flux and separation efficiency achieved was 280 L·m−2·h−1 and >99%, respectively. After 10 repeated cycles, the separation efficiency was maintained at >92%. This approach can be used for the design of future wastewater treatment solutions.
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MACROMOLECULAR RAPID COMMUNICATIONS
·
2022
·Vol. 43
·期 17
·2200212
·
IF 5.006
Li Wang,Qizeng Sun,Linrong Zhang,Jin Wang,Guozhang Ren,Liuyingzi Yu,Kaili Wang,Yameng Zhu,Gang Lu,Hai-Dong Yu
Organic electrochemical transistors (OECTs), especially the ones with high transconductance, are highly promising in sensitive detection of chemical and biological species. However, it is still a great challenge to design and fabricate OECTs with very high transconductance. Herein, an OECT with ultrahigh transconductance is reported by introducing ionic liquid and dodecylbenzenesulfonate (DBSA) simultaneously in poly(3,4-ethylenedioxythiophene): polystyrenesulfonate (PEDOT:PSS) as the semiconductive channel. Compared with the OECT based on pristine PEDOT:PSS, the OECT based on co-doped PEDOT:PSS demonstrates a significant enhancement of transconductance from 1.85 to 22.7 mS, because of the increase in volumetric capacitance and conductivity. The enhanced transconductance is attributed to the DBSA-facilitated phase separation between the ionic liquid and PEDOT:PSS, which helps to form conductive domains of ionic liquid in PEDOT:PSS matrix, and the partial dispersion of ionic liquid in the PEDOT:PSS phase. Furthermore, by using the interdigitated electrodes as the source and drain electrodes, an ultrahigh transconductance of 180 mS is obtained, which is superior to that of the state-of-the-art OECTs. Because of the ultrahigh transconductance, the obtained OECT demonstrates sensitive detection of hydrogen peroxide and glucose, making it promising in clinical diagnosis, health monitoring, and environmental surveillance.
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EUROPEAN POLYMER JOURNAL
·
2022
·
IF 5.546
Bingxiu Xue,Fang He,Xiaopeng Zhao,Jianbo Yin
By changing the amount of vinylimidazole grafted on phenyl ring, we designed and prepared a series of topological self-crosslinked poly(ionic liquid)s (TS-PILs) with different number of spacer arms by free radical polymerization. The influences of the number of spacer arms on the electrorheological (ER) effect of TS-PILs in insulating carrier liquid were studied by rheological test under electric stimulus and the influence mechanism was analyzed by broadband dielectric spectroscopy. It was found that the ER effect of TS-PILs containing organic counterion bis(trifluoromethane sulfonylimide) (TFSI - ) increased with the increase of the number of spacer arms. Broadband dielectric spectra analysis showed that the increased ER effect with the number of spacer arms was attributed to the increase of interfacial polarization strength and the decrease of electrode polarization with the number of spacer arms. Activation energy analysis indicated that increasing the number of spacer arms could promote ion pair dissociation and ion number density but inhibit long-range movement of ions, which was responsible for the increase of interfacial polarization strength and the decrease of electrode polarization. The results provided a guidance insight for the design and preparation of high-performance crosslinked PIL-based ER materials.
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