NATURE MATERIALS
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2020
·Vol. 19
·期 5
·552-558
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IF 38.663
Bi Sheng,Banda Harish,Chen Ming,Niu Liang,Chen Mingyu,Wu Taizheng,Wang Jiasheng,Wang Runxi,Feng Jiamao,Chen Tianyang,Dincă Mircea,Kornyshev Alexei A.,Feng Guang
We performed constant-potential molecular dynamics simulations to analyse the double-layer structure and capacitive performance of supercapacitors composed of conductive metal–organic framework (MOF) electrodes and ionic liquids. The molecular modelling clarifies how ions transport and reside inside polarized porous MOFs, and then predicts the corresponding potential-dependent capacitance in characteristic shapes. The transmission line model was adopted to characterize the charging dynamics, which further allowed evaluation of the capacitive performance of this class of supercapacitors at the macroscale from the simulation-obtained data at the nanoscale. These ‘computational microscopy’ results were supported by macroscopic electrochemical measurements. Such a combined nanoscale-to-macroscale investigation demonstrates the potential of MOF supercapacitors for achieving unprecedentedly high volumetric energy and power densities. It gives molecular insights into preferred structures of MOFs for accomplishing consistent performance with optimal energy–power balance, providing a blueprint for future characterization and design of these new supercapacitor systems.
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Chemistry-An Asian Journal
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2020
·Vol. 15
·期 7
·1081-1087
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IF 4.056
Tingting Chen,Shuai Liu,Hao Ying,Zhonghao Li,Jingcheng Hao
Graphical A reactive ionic liquid strategy was demonstrated for fabricating unusual 3D Rh particles toward efficient electrocatalytic N 2 fixation. Until now, the synthesis of Rh particles with unusual three-dimensional (3D) nanostructures is still challenging. A 3D nanostructure enables fast ion/molecule transport and possesses plenty of exposed active surface, and therefore it is of great interest to construct 3D Rh particles catalysts for the N 2 reduction reaction (NRR). Herein, we proposed a reactive ionic liquid strategy for fabricating unusual 3D Rh particles with nanowires as the subunits. The ionic liquid n -octylammonium formate simultaneously worked as reaction medium, reductant and template for the successful construction of 3D Rh particles. The as-prepared 3D Rh particles demonstrated excellent activity for electrocatalytic N 2 fixation in 0.1 M KOH electrolyte under ambient conditions with a high NH 3 yield of 35.58 μg h −1 mg cat. −1 at −0.2 V versus reversible hydrogen electrode (RHE), surpassing most of the state-of-the-art noble metal catalysts. Our reactive ionic liquid strategy thus holds great promise for the rational construction of high-performance electrocatalysts toward NRR.
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CHINESE JOURNAL OF CHEMICAL ENGINEERING
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2020
·
IF 2.627
Xiaozu Wang,Xiaogang Li,Juan Yue,Yangming Cheng,Ke Xu,Qian Wang,Fan Fan,Zhaohui Wang,Zhaoliang Cui
Ionic liquid (IL), 1-butyl-3-methylimidazolium hexafluorophosphate ([BMIM]PF6) as a new and environmentally friendly diluent was introduced to prepare poly(vinylidene fluoride) (PVDF) membranes via thermally induced phase separation (TIPS). Phase diagram of PVDF/[BMIM]PF6 was measured. The effects of polymer concentration and quenching temperature on the morphologies, properties, and performances of the PVDF membranes were investigated. When the polymer concentration was 15 wt%, the pure water flux of the fabricated membrane was up to nearly 2000 L·m −2 ·h −1 , along with adequate mechanical strength. With the increasing of PVDF concentration and quenching temperature, mean pore size and water permeability of the membrane decreased. SEM results showed that PVDF membranes manufactured by ionic liquid (BMImPF6) presented spherulite structure. And the PVDF membranes were represented as β phase by XRD and FTIR characterization. It provides a new way to prepare PVDF membranes with piezoelectric properties.
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ANALYTICAL AND BIOANALYTICAL CHEMISTRY
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2020
·Vol. 412
·期 13
·3063-3071
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IF 3.637
Li Hongmei,Yue Xiaxia,Gao Ningning,Tang Jun,Lv Xiaoyi,Hou Junwei
Clopidol is one of the most widely used anti-coccidiosis drugs. Its residues in poultry products and the environment pose a serious threat to human health. In this work, microwave-assisted synthesis of magnetic ionic liquid/gold nanoparticles (MIL-Au NPs) as the SERS substrates were first designed for sensitive and reliable determination of clopidol residue in egg samples. The experiment shows that MIL(1-methyl-3-hexyl imidazole ferric tetrachloride ([C 6 mim]FeCl 4 )) and microwave play a key role in the dispersion and morphology of Au NPs. Under the optimal conditions, the as-prepared MIL-Au NPs were applied to the SERS detection of clopidol in methanol and egg solution and its detection limits can be as low as to 0.5 μg/kg (equal to 0.5 ppb) in both solutions. The standard curves with regression coefficients of 0.9298 and 0.93496 were constructed in the linear range of 100–1000 ppb and 0.5–50 ppb for clopidol in egg solutions. Moreover, satisfactory recoveries (97.5–103.2%) were obtained for egg samples. The developed SERS method provides a way for quantitation of clopidol and can be applied for the convenient, reliable, and highly sensitive detection of antibiotic residues in food and environment, which has great potential in food safety and biological monitoring.
Graphical abstract
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FUEL
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2020
·
IF 5.578
Guo Qiu,Biaohua Chen,Chongpin Huang,Ning Liu,Xiuliang Sun
Methods for the conversion of carbohydrates into 5-hydroxymethylfurfural (5-HMF), which is an important platform chemical, have been attracted extensive attention. In present study, Sn modified ionic liquid polymer (PIL-Sn) was prepared by one-pot polymerization of imidazole and epichlorohydrin, and utilized as a novel and efficient catalyst for 5-HMF production. The optimal 5-HMF yield of 51.1% with 99% conversion was obtained from glucose catalyzed by PIL-Sn in dimethyl sulfoxide at 130 °C with reaction time of 1 h. This catalytic system can also be applied for the transformation of other carbohydrates with satisfactory yields. The mechanism of PIL-Sn-catalyzed conversion of glucose to 5-HMF has been studied using density functional theory (DFT) calculations. The DFT results showed that the five-coordinated SnCl 5 - as a preferred species played an important role in the isomerization of glucose to fructose. This research provides a new strategy to design efficient catalysts for 5-HMF synthesis.
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APPLIED SURFACE SCIENCE
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2020
·
IF 6.182
Mengran Lou,Ruiying Wang,Lili Yang,Dianzeng Jia,Zhipeng Sun,Luxiang Wang,Yong Guo,Xingchao Wang,Jie Zhang,Hongli Shi
Direct formic acid fuel cells have great application potential in the energy field, but their commercialization is hindered by the CO poisoning and low performance of Pd-based anode catalysts. In this study, novel composite catalysts composed of Pd, organic-inorganic hybrid imidazole ionic liquid polyoxometalates, and N,P-codoped coal-based carbon fibers with good dispersion and smaller Pd nanoparticles were synthesized successfully. Physical and electrochemical characterizations revealed that the as-prepared Pd-based composite catalysts have excellent CO poisoning resistance and enhanced electrocatalytic activity in formic acid electrooxidation. Notably, the CO oxidation onset potential of a catalyst modified by imidazole ionic liquid polyoxometalate with long alkyl chain was 0.1 V lower than that of the unmodified catalyst. The mass activity of the as-prepared Pd catalyst in formic acid oxidation was 754.1 mA mg −1 Pd . It is expected that organic-inorganic hybrid polyoxometalates can be further applied to fuel cell catalysts.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2020
·
IF 3.573
Jingjing Li,Zhiyu Wang,Xiaodong Tang,Xiaojie Lei
The olefin alkylation of thiophenic sulfur (OATS) in model fluid catalytic cracking gasoline was carried out using the temperature-responsive catalyst which was prepared by mixing the temperature-responsive ionic liquid (TRIL) and p-toluenesulfonic acid (PTSA) with the mass ratio 1:10 (10% TRIL–PTSA). The liquid–liquid biphasic system was formed during the OATS and returned to the liquid–solid state automatically after completion of the reaction at cooling temperature, which enhanced the mass transfer efficiency and separation ability of oil and the catalyst. As for 10% TRIL–PTSA, the acid strength was adjusted properly by TRIL, and the anionic cluster of [−SO3(−SO3H)x]– was also found by Fourier transform infrared, 1H NMR, and thermogravimetric–differential scanning calorimetry, which displayed a better catalyst performance over PTSA. Moreover, the effects of various factors were fully discussed, including the reaction temperature, reaction time, and catalyst dosage. Under optimal conditions, the conversion of thiophene (T) can reach 100% and it can remain unchanged during 10 recycles. Furthermore, apparent reaction kinetics for OATS was discussed. It suggested that the alkylation of T conformed to the pseudo-first-order kinetic characteristic, and the apparent activation energy was 47.6 kJ/mol. Finally, the synergistic catalysis mechanism was proposed.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2020
·
IF 5.162
Bo Li,Qi Zhang,Yuanfeng Pan,Yuchen Li,Zhihong Huang,Ming Li,Huining Xiao
Porous magnetic cellulose/Fe 3 O 4 beads (CFBs), consisting of cellulose as matrix and ferrosoferric oxide, were successfully fabricated from microcrystalline cellulose dissolved in an ionic liquid and further modified with glutaric anhydride. The porous structure of modified magnetic cellulose/Fe 3 O 4 beads (MCFBs) was created by nano-sized calcium carbonate (CaCO 3 ). The resulting MCFBs were well characterized and employed as effective adsorbents for removal of dyes from aqueous solution. The adsorption behaviors indicated that the adsorption kinetics was preferably fitted to the pseudo-second-order kinetic model; whereas the adsorption isotherms were well described by Langmuir model with the maximum adsorption capacity of 1186.8 and 151.8 mg/g for methylene blue (MB) and Rhodamine B (RhB), respectively. Moreover, MCFBs are magnetically separable, thus leading to a range of green-based and promising adsorbents towards organic pollutants with easy recovery.
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ACS Sustainable Chemistry & Engineering
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2020
·
IF 7.632
Jiale Yang,Zhiyuan Zhou,You Liang,Jingyue Tang,Yunhao Gao,Junfan Niu,Hongqiang Dong,Rong Tang,Gang Tang,Yongsong Cao
A microcapsule is an ideal choice to realize effective utilization of a pesticide and reduce environmental pollution. A novel preparation method of a microcapsule was developed by complex coacervation of phosphonium ionic liquid (PIL) with gelatin. PIL was newly synthesized and used to dissolve and disperse avermectin (Ave) to form stabilized core–shell structure microcapsules by cross-linking with gelatin in a solution. The results demonstrated that avermectin–phosphonium ionic liquid–gelatin (Ave–PIL–Gel) microcapsules had a high Ave entrapment efficiency (approximately 98% w/w), and could effectively enhance the stability of Ave by reducing its degradation in the environment. The Ave release of synthesized Ave–PIL–Gel microcapsules was governed predominantly by non-Fickian diffusion, and the release rates showed positive correlation with the temperature and the base conditions. Compared with the Ave technical solution, the Ave–PIL–Gel microcapsules had better nematicidal activities against plant-parasitic nematodes and showed great potential for sustainable crop protection. The present study provides an improved controlled release formulation comprising a pesticide, which is sensitive to light and easily degradable in soil encapsulated in negatively charged protein, and also provides an environmentally friendly method for preparing the improved pesticide formulation so that the pesticide release rate and release period can be adjustable.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2020
·
IF 4.65
Jianfeng Zhu,Dan Wang,Daming Chen,Baorui Song,Yanhuai Li,Fei Liu,Jian Chen
Mixed transition metal oxides with low-cost elements such as ZnFe 2 O 4 have been considered as the promising candidate as anode materials for Li-ion batteries (LIBs) owing to the high capacity originated from versatile redox reactions . However, poor conductivity and huge volume expansion during charging/discharging cause drastic capacity decay, which hinders their commercial application. Herein, we designed a unique core-shell N doped ZnFe 2 O 4 embedded in B, N doped graphene network (B/N-ZFO@rGO) using ionic liquids as multi-heteroatom source through facile hydrothermal reaction . Benefiting from the enhanced conductivity and structural stability, the B/N-ZFO@rGO as anode material for LIBs not only shows significantly improved specific capacity (668.1 mAh g −1 at 1 A g −1 after 100 cycles), but also remarkable rate capacity and long cycle life (377.4 mAh g −1 at 5 A g −1 after 1200 cycles), demonstrating great potential in future applications. Moreover, such rational design of structure as well as multiple elements doping using ionic liquids can be extensively applied in other electrode materials.
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JOURNAL OF POWER SOURCES
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2020
·
IF 8.247
Xinan Shi,Lijian Huang,Daocheng Pan
In this research, a facile and environmentally friendly solution approach is developed to deposit Cu 2 ZnSn(S,Se) 4 thin films by addition of n -butylammonium butyrate ionic liquid . n -Butylammonium butyrate plays a critical role in solution deposition of Cu 2 ZnSnS 4 precursor thin film. We find that liquid n -butylammonium butyrate can dissolve a number of metal oxides , including Cu 2 O, ZnO, and SnO as well as various metal chlorides , metal nitrates and metal acetates. Smell-free Cu 2 ZnSnS 4 precursor solution is synthesized by dissolving Cu 2 O, ZnO, SnCl 2 and thiourea in an ethanol solution of n -butylammonium butyrate. Thermally degradable n -butylammonium butyrate can be completely removed by a low-temperature sintering process , forming high quality Cu 2 ZnSnS 4 nanoparticle thin film. A power conversion efficiency of 8.79% is obtained by this facile and green solution approach.
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JOURNAL OF POWER SOURCES
·
2020
·
IF 8.247
Rui Wu,Xianqiang Liu,Yijing Zheng,Yonghe Li,Huifeng Shi,Xiaopeng Cheng,Wilhelm Pfleging,Yuefei Zhang
Due to the excellent theoretical capacity, silicon-based electrodes have been extensively studied to develop high energy-density lithium-ion batteries (LIBs). Nevertheless, the large volume expansion and unfavorable interface seriously hamper its application, and the underlying physics behind are still unclear. In this work, using in-situ environment scanning electron microscopy (ESEM), the morphological evolution of composite silicon-graphite electrodes with different ionic liquids as electrolytes are compared in the range of 20 °C–60 °C. Surprisingly, combining the microstructure and surface reaction products from transmission electron microscope (TEM) and X-ray photoelectron spectroscopy (XPS), it finds out that the fully reaction of lithium-silicon does not generate huge volume expansion, while the side reaction between graphite and electrolyte decomposition products causes dramatic volume expansion and hinders the further lithiation of silicon . On the other hand, the electrolyte which is capable of rapidly releasing F − to form LiF-rich solid electrolyte interphase (SEI) is favorable to maintain the structure integrity and cycling performance. This work casts new understanding from the perspective of intrinsic reaction between electrode and ionic liquid electrolyte, which suggests that the practical application of silicon-based electrodes with appropriate electrolyte is a promising route for high energy-density LIBs.
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