Facile synthesis of magnetic ionic liquid with magnetic-tuning electrochemical performance

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Facile synthesis of magnetic ionic liquid with magnetic-tuning electrochemical performance | Research Square window.SnipcartSettings = { analytics: { enabled: false } }; (function() { var accessVector = localStorage.getItem('access_vector') || ''; window.dataLayer = window.dataLayer || []; if (accessVector) { window.dataLayer.push({ user: { profile: { profileInfo: { snid: accessVector } } } }); } })(); (function(w,d,s,l,i){w[l]=w[l]||[];w[l].push({'gtm.start':new Date().getTime(),event:'gtm.js'});var f=d.getElementsByTagName(s)[0],j=d.createElement(s),dl=l!='dataLayer'?'&l='+l:'';j.async=true;j.src='https://www.googletagmanager.com/gtm.js?id='+i+dl;f.parentNode.insertBefore(j,f);})(window,document,'script','dataLayer','GTM-K279D39R'); Browse Preprints In Review Journals COVID-19 Preprints AJE Video Bytes Research Tools Research Promotion AJE Professional Editing AJE Rubriq About Preprint Platform In Review Editorial Policies Our Team Advisory Board Help Center Sign In Submit a Preprint Cite Share Download PDF Research Article Facile synthesis of magnetic ionic liquid with magnetic-tuning electrochemical performance Ning Gu, Xiaolin Li, Miao Gao, Zixuan Liu, Qichao Liu, Yang Cao, and 1 more This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-3875532/v1 This work is licensed under a CC BY 4.0 License Status: Published Journal Publication published 16 Mar, 2024 Read the published version in Ionics → Version 1 posted 8 You are reading this latest preprint version Abstract A new magnetic ionic liquid (MIL) based on 1-methylethyl ether-3-butylimidazole and [FeCl 4 ] − is synthesized for application in electrolyte. It is found that the electrochemical performance of magnetic ionic liquid based mixed electrolyte can be improved by applying magnetic field. The enhanced electrochemical performance is attributed to the formation of microdomain in the mixed electrolyte under magnetic field. The ions of MIL can align along the direction of the magnetic field, providing the efficient transmission path for the migration of Li + and Cl − . Under magnetic control, the MI-based electrolyte does not only retain its wide electrochemical window characteristics, but also solves the problem of limiting the high viscosity of IL as electrolyte. The work provides a new method to design and prepare high-performance electrolyte for various electrochemical applications. Magnetic ionic liquid Electrochemical performance Electrolyte Magnetic tuning Simulation Figures Figure 1 Figure 2 Figure 3 Figure 4 Figure 5 Figure 6 Figure 7 1. Introduction In the electrochemical energy storage, work safety and high performance are equally important issues (Choi et al.,2012; Tiago et al., 2020 ). As well-known, the electrolyte material is an key component for work safety and electrochemical performance of electrochemical energy storage. Therefore, there are lots of works reporting the effect of electrolyte materials on electrochemical performance of electrochemical energy storage. Up to now, the most electrolytes are water-based or organic solvent-based systems. Water-based electrolyte exhibits high ionic conductivity, leading to good electrochemical performance. Unfortunately, the electrochemical window of water-based electrolyte is narrow (only about 1.23V) at room temperature. At the same time, it is easy to corrode the device and the operating temperature range is limited to 0 ~ 100°C (Kuhnel et al., 2016 ). Although traditional organic electrolytes have better overall performance than water-based electrolytes, yet they are volatile and flammable. These traditional organic electrolytes often cause serious safety problems (Goodenough & Kim, 2010 ; Mtj et al., 2001). It is found that the introduction of fluorine atoms into the solvent electrolytes can effectively improve electrochemical performance of battery. For example, Hu L et al reported the synthesis and electrochemical performance of fluorinated organic solvents, which showed higher polarity and oxidation resistance comparing to organic solvents without fluorinating (Hu et al., 2013 ). At the same time, other additives (eg. MA, SA, PBF, PPF, etc) were also introduced to the electrolyte and could effectively improve the cycle and energy storage performance of carbonate electrolytes. Furthermore, the effect of the additives (eg. MMDS, DTD, TAP) on electrochemical performance was also investigated, in which these additives could effectively reduce the voltage drop (Xia et al., 2017 ). For examples, Lee Jyh Tsung et al found that the electrochemical window increased from 0.8V to 1.5V after adding allyl ethyl carbonate to PC electrolyte (Lee et al., 2004 ). However, these additives also brought some negative effects. For example, although the additive of VC provided excellent cyclic performance and charge/discharge capacity, yet the initial efficiency in the electrolyte with 2.0wt% VC was only 72.3%, which was lower than that in standard electrolyte (Yao et al., 2015 ). Thermal stability of the electrolyte could be improved by phytic acid, but the capacity of the vanadium flow battery employing the vanadium electrolyte with phytic acid decreased significantly (Wu et al., 2012 ). From above respects, it is still an high interesting to find a new electrolyte for improving the work safety and electrochemical performance. Recently, it is found that ionic liquids (ILs) are a promising type of electrolyte material due to unique physical and chemical properties, such as low saturated vapor pressure, low flammability, high thermal stability, wide electrochemical window and green (Tsunashima et al., 2009 ). EMinato Egashira et al reported synthesis and electrochemical performance of the imidazolium ionic liquids functionalized with cyanomethyl, which showed a higher cycle efficiency comparing to conventional organic solvent electrolytes (Egashira et al., 2007 ). However, the slow kinetics of ionic liquids hinder the migration of ions, reducing the electrochemical storage performance (Armand et al., 2009 ). To solve above problem, a mixed electrolyte based on ionic liquids and other solvents was developed, which could combine the advantages of each component. For example, the organic solvent was added to the ionic liquid electrolyte, which could reduce system viscosity and improve ion migration, thereby increasing in the power density of supercapacitors (Montanino et al., 2014 ). The result was attributed to that the LiTFSI-PYR13TFSI-PYR13FSI mixtures exhibited high ion transport properties with about 10 − 3 S cm − 1 at -20℃ (Appetecchi et al., 2016 ). The magnetic ionic liquids (MILs) are a new class of ILs with special paramagnetic behavior (Hamaguchi. et al., 2004; Lage-Estebanez et al., 2018 ), which are expected to act as electrolyte materials to improve ion transport properties and electrochemical performance. However, although MILs have been reported for various applications, such as catalyst, fluid-fluid separations, and chemical reactions, etc (Mohammad et al., 2020 ; Feng et al., 2018 ; Sajid, 2019 ; Kowsari & Mohammadi, 2016 ), yet, MILs are few reported for application in electrolyte. Here, a new mixed electrolyte based on MILs was developed to improve ion transport properties and electrochemical performance. MILs do not only exhibit the excellent characteristics of ionic liquids, but also show magnetism. It will arrange in a magnetic field and form magnetic chains. The MIL in the mixed electrolyte forms magnetic chains under the magnetic field, and the non-magnetic organic solvent medium in the magnetic chain gap is expected to become a high-speed channel for ion transmission. These works provide a new method to simultaneously improve electrochemical performance and work safety of electrochemical energy storage. 2. Experimental 2.1 Materials 1-Butylimidazole (> 98%), Chloromethyl ether (> 95%) and the FeCl 3 ·6H 2 O (> 99%) were purchased from Aladdin. The dichloromethane, deuterated dimethyl sulfoxide (DMSO-d6 > 99.9%) and ethyl acetate were purchased from Tianjin Kaitong Chemical Reagent Co., Ltd. Besides, the electrode of Platinum electrode, glassy carbon and carbon rod were purchased from Changsha Changjindiantang science and technology Co., Ltd. 2.2 Synthesis of MIL The MIL was synthesized by a two-step method as shown in following. Firstly, 16.2g 1-butyl imidazole and 10g chloromethyl ether were dissolved in 20mL dichloromethane under mechanical stirring at 9℃. The mixture was reacted at 30℃ for 3 h under the protection of N 2 , forming the IL. And then the IL was purified by washing with ethyl acetate and dichloromethane for two times. Secondly, 19.8g FeCl 3 ·6H 2 O was added to 16g IL under mechanical stirring. The mixture was reacted at 30℃ for 3h under the protection of N 2 , forming MIL. Finally, the MIL was purified by rotary evaporator and vacuum at 80 ℃ for 24 h. 2.3 Preparation of mixed electrolyte based on MIL The electrolyte was prepared by blending MIL and an organic electrolyte(4 M LiCl/NMP) with a volume ratio of 5:1. To achieve a homogeneous and anhydrous mixture, the electrolyte was dispersed by ultrasound for 1h and dried under vacuum at 80℃ for 24 h. 2.4 Characterization of MIL The chemical structure of MIL was characterized by 1 H-NMR spectrum on a Avance III 600 MHz NMR spectrometer at room temperature. And the dimethyl sulfoxide-d 6 (DMSO-d 6 ) was used as solvent. Infrared spectroscopy (FT-IR) spectra were obtained on a Thermo Fisher Spectrum One (Thermo Fisher, USA) and scanned from 500 to 4000 cm − 1 . Raman measurements were carried out on In Via at a wavelength of 785 nm at 298 K. The magnetic properties of MIL were measured at room temperature by vibrating sample magnetometer (Micro Sense, LLC, USA) from 0 to 11000 Oe. 2.5 Electrochemical performance The electrochemical measurements of linear sweep voltammetry (LSV), cyclic voltammetry (CV) and electrochemical impedance spectroscopy (EIS) were characterized by CHI 660C workstation with three electrode systems. The working electrode, counter electrode and reference electrode were carbon rod, glassy carbon and Pt metal, respectively (as shown in Fig. 1 ). The galvanostatic charge/discharge (GCD) was performed on LANHE CT2001A. The specific capacitance is calculated by following formula: C = I▪∆t /(A▪∆V) Where A is the area of electrode, I is the applied current, ∆t is the discharge time and ∆V is the change of capacitor voltage (Mirmohseni et al., 2012 ). The diagram of electrochemical cell as shown in Fig. 1 . In the electrochemical cell, diameter of carbon rod and glassy carbon electrodes is both 3.0mm and the length of penetrating into the electrolyte is both 1.0cm. The area of platinum sheet in the electrolyte is about 1.0cm×0.8cm. Besides, U-shaped magnet is used to provide a 0.3T magnetic field, and the distance d between the U-shaped magnet and the electrodes is 5.0mm. 3. Results and discussion Figure 2 A shows the 1 H-NMR spectrum of MIL and the data is listed as follows: δ=9.50 (s, 1H, -N=CH-N-), 7.90 (s, 2H, -N-CH=CH-N-), 5.53 (s, 2H, -N-CH 2 -O-), 4.23 (s, 2H -N-CH 2 -CH 2 -), 4.03 (s, 2H, CH 3 -CH 2 -O-), 1.81 (t, 2H, J=3.6Hz, -CH 2 -CH 2 -CH 3 ), 1.28(s, 2H, -CH 2 -CH 3 ), 0.92(s, 6H,-CH 3 ). The ratio of integral peak area ratio was consistent with the ratio of the number of hydrogen atoms at different chemical shifts. At the same time, no additional peaks were observed in the 1 H-NMR spectrum of the intermediates. The result indicated the formation of MIL. The structure of MIL was further characterized by FT-IR spectrum as shown in Fig. 2 B. The wide absorption band around 3412.0 cm -1 was assigned to intermolecular hydrogen bonding (Chen et al., 2018). The absorption peaks at 3144.0 cm -1 and 2960.0 cm -1 were assigned to C-H stretching modes of the imidazolium ring (Tao et al., 2014 ). The absorbance peaks around 1553.0 cm -1 and 1390.0 cm -1 were assigned to C-H bending modes and C=C stretching vibrations on the imidazolium ring, respectively (Chen et al., 2018). The absorbance bands at 1158.0 cm -1 and 1107.0 cm -1 were assigned to C-N stretching modes and C-O stretching modes of MIL, respectively (Haddad et al., 2017 ; Chen. et al., 2010). The absorbance peaks below 1000 cm -1 were assigned to C-C or C-N bending vibration of MIL. Fig. 2 C shows the Raman spectrum of MIL. A new strong absorption peak at 331.0 cm -1 was observed, which was assigned to FeCl 4 - anion (Melissa et al., 2001 ). These results further confirm the successful synthesis of MIL. The magnetization of MIL was further characterized at a magnetic field range from 0 to 11000 Oe as shown in Fig. 2 D. The magnetization of MIL showed a linear response to the applied magnetic field, indicating that it had paramagnetic behavior (Wang et al., 2019 ). The magnetic susceptibility of MIL was determined to be 1.82×10 -5 emu/g. Linear sweep voltammetry measurements were performed for determining the electrochemical window (ESW) as shown in Fig. 3 . The electrolyte clearly showed the large ESW of approximately 5.0V, ranging from − 7.5 V to -2.5 V. This was consistent with ESW of ILs reported in previous work (Suarez et al., 1997 ), in which also showed wide potential ranges about 4.5-5V. However, the ESW of MIL-based electrolyte was obviously larger than that (eg.2.5V) of organic electrolytes reported in previous work (Liew et al., 2016 ). The result confirmed that the MIL-based electrolyte showed excellent stability at high voltages for application in electrochemical energy storage with high voltage (Bonhote et al., 1996 ). The cyclic voltammetry (CV) curves using MIL-based electrolyte were characterized at different scan rates from 0.1 to 1 V⋅s − 1 in the absence and presence of magnetic field (0.3T) as shown in Fig. 4 A and Fig. 4 B, respectively. It was seen that the CV curves were nearly rectangular shape at the lower scan rate than 0.1V⋅s − 1 , indicating high ion transport properties. The specific capacitance using MIL-based electrolyte was further calculated according to CV curves in the absence and presence of magnetic field as shown in Fig. 4 C. As expected, the specific capacitance decreased significantly with increasing in the scan rate. When the scan rate increased from 0.1 to 1 V⋅s − 1 , the specific capacitance of MIL-based electrolyte drastically decreased from 18.4 (or 13.1) to 4.7 (or 2.4) mF⋅cm − 2 in the presence (or absence) of magnetic field. This result was attributed to that these ions were not enough time for diffusing to the surface of the electrode material at higher scan rates (Melissa et al., 2001 ). Moreover, it was found that the capacitance of electrode with 0.3T magnetic field was obviously larger than that of electrode without magnetic field. The result indicated that the capacitance of electrode using MIL-based electrolyte could be easily tuned and improved by applying magnetic field. The result was attributed to that the MIL was arranged along the direction of the magnetic field, facilitating the migration of ions on the electrode interface. Above result was further confirmed by the CV curves as shown in Fig. 4 D. It clearly showed CV curves using pure MIL as electrolyte in presence and absence of magnetic field. Obviously, the capacitance of electrode using the pure MIL electrolyte became smaller under a magnetic field comparing to no magnetic field. This result was attributed to that the ions of the MIL were arranged in the direction of the magnetic field, inhibiting its diffusion and migration in the electrochemical The effect of magnetic field on GCD curves was also characterized as shown in Fig. 5 A-B. The discharge time after applying a magnetic field was longer comparing to no magnetic field. The specific capacitance as function of current densities was calculated from GCD curves in presence and absence of magnetic field as shown in Fig. 5 C. It clearly showed that the specific capacitance using MIL-based electrolyte in presence of magnetic field (0.3T) is 15.8mF ⋅ cm − 2 at a current density of 0.1mA ⋅ cm − 2 . However, the corresponding value was 10.9 mF ⋅ cm − 2 in absence of magnetic field. These results further proved that MIL in the mixed electrolyte was arranged along the direction of the magnetic field under the magnetic field, while the Li + and Cl − dispersed in the NMP could move freely. At the same time, the magnetic field reduced the viscous resistance of the migration ions in IL, resulting in better electrochemical performance. Moreover, it retained the wide electrochemical window for electrochemical cell device. Long-term stability is a key role for the practical application of electrochemical cell device. The stability of MIL-based electrolyte was evaluated by sequential charge-discharge for 5000 cycles at a current density of 0.3 mA⋅cm − 2 as shown in Fig. 5 D. The specific capacitance still retained 79.0% after 5000 charge-discharge cycles in presence of magnetic field, which was higher than that (70.8%) in absence of magnetic field. These results do not only confirm that the external magnetic field will improve the stability of electrochemical cell device using MIL-based electrolyte, but also further demonstrate the magnetic field controllability of the electrochemical performance of the MIL-based electrolyte. EIS spectra using MIL-based electrolyte were characterized and compared in presence and absence of magnetic field as shown in Fig. 6 . It clearly showed a semicircle and a 45-degree linear section, which represented the resistance of charge transfer and the ions diffusion, respectively (Du et al., 2009 ). The bulk resistance (Rs) of electrolyte and the interfacial charge transfer resistance (Rct) were calculated and concluded in Table 1 . The Rs (51.3Ω) of electrolyte in presence of magnetic field was smaller than that (57.9 Ω) in absence of magnetic field. Similarly, the Rct of electrolyte in presence and absence of magnetic field was about 142.6Ω and 185.5Ω, respectively. After applying a magnetic field, the resistance of the MIL-based electrolyte and the Rct at the interface were significantly reduced, thereby enhancing the capacitive behavior. These results further confirmed the formation of MIL-based electrolyte with high ion transport properties by applying magnetic field. Here, the result was different from previous work (zhang et al., 2016 ), in which the Ionic conductivity decreased with increasing in magnetic field. Here, in an external magnetic field, MIL was aligned along the magnetic field to form micro-domains (Nykaza et al., 2016 ), the viscosity of the system was reduced, and the ions of Li + and Cl − dispersed in NMP could be quickly transferred in the microdomain.The electrochemical performance of different ionic liquid electrolytes is compared in Table 2 . It can be seen that the MIL electrochemical has outstanding performance in terms of electrochemical window and cycle stability. Table 1 The Rs and Rct in absence and presence of magnetic field. R(Ω) Magnetic Field (0.0 T) Magnetic Field (0.3 T) Rs 57.9 51.3 Rct 185.5 142.6 Table 2 Comparison of electrochemical properties of different ionic liquid electrolytes. Electrochemical window The specific capacitance Capacitance retention rate (cycle number) Reference 5.0V 15.8 mF⋅cm − 2 79.0% (5000) 98% (30) This paper - 147mAh.g − 1 96% (30) Tsunashima et al., 2009 2.0V 153mAh.g − 1 90% (4) Montanino et al., 2014 5.0V 135mAh.g − 1 - Appetecchi et al., 2016 3.5V - 90% (50) Egashira et al., 2007 The magnetic tuning mechanism in electrochemical performance of MIL-based electrolyte was further investigated and proposed as shown in Fig. 7 . As shown in Fig. 7 A, the ions of Li + and Cl − were randomly distributed in MIL-based electrolyte in the absence of magnetic field. In a comparison, the MIL is parallel to the magnetic field direction in the presence of magnetic field, forming a ion transport pathway in the gap of flux linkage and then drive Li + and Cl − migrate between two electrodes(Fig. 7 B). Hence, the external magnetic field can improve the electrochemical performance by reducing the internal resistance in the system. These oriented structures are contributed to accelerate ion mobility in the electrolyte, improving the conductivity. Differing from the traditional electrolyte, it can form conductive paths in the direction of the external magnetic field. Above result was further confirmed by the FT-IR spectra of MIL-based electrolyte without and with magnetic field as shown in Fig. 7 C. In the test of FT-IR spectra, a U-shaped magnet is placed at the FT-IR probe to provide magnetic field, which can provide 0.3T magnetic field strength. After applying a magnetic field, the peak position of MIL's γC(2)H decreased from 844.21 cm − 1 to 837.77 cm − 1 . According to the study of the Christopher M. B [32] , the C(2)H is particularly sensitive to the interactions between anions and cations, leading to a reduction in frequency band. So, the change in frequency band is due to the change in the force between the internal anions and cations. The anions form Fe-Cl…Cl-Fe structure in the presence of the external magnetic field, enhancing the interaction between the anions (Abel et al., 2014 ). At the same time, the interaction between anions with the C(2)H on the imidazole ring is correspondingly reduced (Burba et al., 2019). Therefore, the infrared spectrum is blue shift under the magnetic field. The ionic liquid arranged along the magnetic field in the electrolyte, forming a conductive path. In summary, the pure MIL electrolyte undergoes ion alignment under a magnetic field, the capacitance is reduced. In contrast, the capacitance of the mixed electrolyte with the applied magnetic field increases. This suggests that although the movement of MIL anions and cations under the magnetic field is restricted, the gaps formed by the arrangement along the magnetic field provide rapid migration channels for the lithium salt. The capacitance of the MIL-based mixed electrolyte increases under the mutual competition. 4. Conclusion In this study, a new type of MIL-based mixed electrolyte with magnetic response was prepared. The electrochemical performance of the MIL-based mixture electrolyte was significantly improved under external magnetic field. Compared with the absence of a magnetic field, the specific capacitance increases from 10.9 to 15.8 mF⋅cm − 2 at a current density of 0.1 mA⋅cm − 2 after applying 0.3T magnetic field. Similarly, the capacitance retention rate increased from 70.8–79.0% for 5000 charging/discharging cycle. In addition, the EIS test showed that the resistance of the system decreased after applying a magnetic field. Studies proved that MIL could magnetically responsive under a magnetic field and the ions of MIL was aligned along the direction of the magnetic field. The oriented structure provided an efficient transmission path for the migration of Li + and Cl − , thereby improving the electrochemical performance of the system. The work opens up a new direction for improving the performance of electrochemical energy storage. Declarations Author Contribution Ning Gu:Conceptualization,Investigation,Roles/Writing-original draft;Xiaolin Li:Conceptualization,Investigation;Miao Gao:Formal analysis,Investigation;Zixuan Liu:Formal analysis;Qichao Liu:Review & Editing;Yang Cao:Writing - Review & Editing;Youyi Sun:Roles/Writing-original draf,Funding acquisition. Acknowledgments The authors are grateful for the support of Shanxi province and Shanxi Provincial Natural Science Foundation (202104021301059, YDZJSX2021A026, TZLH20230818009, 202204021301049) and Special fund for science and technology innovation teams of Shanxi province. References Choi, NS., Chen, Z., Freunberger, SA., Ji, XL., Sun, YK., Amine, K.,Yushin, G,, Nazar, LF., Cho, J., & Bruce, PG. (2012). Challenges facing lithium batteries and electrical double-layer capacitors. Angew Chem Int Ed Engl, 51, 9994–10024. 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Cite Share Download PDF Status: Published Journal Publication published 16 Mar, 2024 Read the published version in Ionics → Version 1 posted Editorial decision: Revision requested 03 Feb, 2024 Reviewers agreed at journal 01 Feb, 2024 Reviews received at journal 01 Feb, 2024 Reviewers agreed at journal 25 Jan, 2024 Reviewers invited by journal 20 Jan, 2024 Editor assigned by journal 19 Jan, 2024 Submission checks completed at journal 19 Jan, 2024 First submitted to journal 18 Jan, 2024 You are reading this latest preprint version Research Square lets you share your work early, gain feedback from the community, and start making changes to your manuscript prior to peer review in a journal. As a division of Research Square Company, we’re committed to making research communication faster, fairer, and more useful. We do this by developing innovative software and high quality services for the global research community. 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Also discoverable on Platform About Our Team In Review Editorial Policies Advisory Board Help Center Resources Author Services Accessibility API Access RSS feed Manage Cookie Preferences © Research Square 2026 | ISSN 2693-5015 (online) Privacy Policy Terms of Service Do Not Sell My Personal Information {"props":{"pageProps":{"initialData":{"identity":"rs-3875532","acceptedTermsAndConditions":true,"allowDirectSubmit":false,"archivedVersions":[],"articleType":"Research Article","associatedPublications":[],"authors":[{"id":268331795,"identity":"0629f66d-9c3c-481e-9633-9715502641f9","order_by":0,"name":"Ning Gu","email":"","orcid":"","institution":"North University of China","correspondingAuthor":false,"prefix":"","firstName":"Ning","middleName":"","lastName":"Gu","suffix":""},{"id":268331796,"identity":"95b0e948-fd9f-4a80-8f2a-883f4aedf7b2","order_by":1,"name":"Xiaolin Li","email":"","orcid":"","institution":"North University of China","correspondingAuthor":false,"prefix":"","firstName":"Xiaolin","middleName":"","lastName":"Li","suffix":""},{"id":268331797,"identity":"c63e8c77-1c73-4c09-8295-81748394c968","order_by":2,"name":"Miao Gao","email":"","orcid":"","institution":"North University of China","correspondingAuthor":false,"prefix":"","firstName":"Miao","middleName":"","lastName":"Gao","suffix":""},{"id":268331798,"identity":"0bb3a970-27dc-4d9b-86e3-8e6350fbb129","order_by":3,"name":"Zixuan Liu","email":"","orcid":"","institution":"North University of China","correspondingAuthor":false,"prefix":"","firstName":"Zixuan","middleName":"","lastName":"Liu","suffix":""},{"id":268331799,"identity":"56657582-8df0-40d7-ab39-868fc813f125","order_by":4,"name":"Qichao Liu","email":"","orcid":"","institution":"North University of China","correspondingAuthor":false,"prefix":"","firstName":"Qichao","middleName":"","lastName":"Liu","suffix":""},{"id":268331800,"identity":"891b27b7-5fef-438f-998f-292cae1d7357","order_by":5,"name":"Yang Cao","email":"","orcid":"","institution":"North University of China","correspondingAuthor":false,"prefix":"","firstName":"Yang","middleName":"","lastName":"Cao","suffix":""},{"id":268331801,"identity":"205933af-d8da-43ae-958c-63c31dd01adb","order_by":6,"name":"Youyi Sun","email":"data:image/png;base64,iVBORw0KGgoAAAANSUhEUgAAAZAAAAAyAQMAAABI0h/eAAAABlBMVEX///8AAABVwtN+AAAACXBIWXMAAA7EAAAOxAGVKw4bAAAAtUlEQVRIiWNgGAWjYJCCAx8YEkC0AfFaDs4gWQszD0la5GfkGB623ZGW2MDevE2CoeYOYS0GN3IMDueeyUls4DlWJsFw7BkRWiRAWtoqEhskcswkGBsOE+Uwg8OWIC3yb4jUwgByGGMb0GESPERqMTjzrOBg75k04zaetGKLhGPEOKw9efOHnzuSZfvZD2+88aGGGIcJZBgwMDYwMLCBOAlEaGBg4D/+AKxlFIyCUTAKRgFOAADlvzyfgcyU/wAAAABJRU5ErkJggg==","orcid":"","institution":"North University of China","correspondingAuthor":true,"prefix":"","firstName":"Youyi","middleName":"","lastName":"Sun","suffix":""}],"badges":[],"createdAt":"2024-01-18 10:44:15","currentVersionCode":1,"declarations":"","doi":"10.21203/rs.3.rs-3875532/v1","doiUrl":"https://doi.org/10.21203/rs.3.rs-3875532/v1","draftVersion":[],"editorialEvents":[{"content":"https://doi.org/10.1007/s11581-024-05466-9","type":"published","date":"2024-03-16T14:30:52+00:00"}],"editorialNote":"","failedWorkflow":false,"files":[{"id":49984194,"identity":"396c09a3-a1ad-447c-9390-0560741b66f0","added_by":"auto","created_at":"2024-01-22 16:31:16","extension":"jpg","order_by":1,"title":"Figure 1","display":"","copyAsset":false,"role":"figure","size":13948,"visible":true,"origin":"","legend":"\u003cp\u003eThe diagram of electrochemical cellbased on mixed electrolyte.\u003c/p\u003e","description":"","filename":"1.jpg","url":"https://assets-eu.researchsquare.com/files/rs-3875532/v1/5fec5c45359598c92c59c72c.jpg"},{"id":49984195,"identity":"a73ec14b-3aff-4ef8-9789-857129f4c270","added_by":"auto","created_at":"2024-01-22 16:31:17","extension":"jpg","order_by":2,"title":"Figure 2","display":"","copyAsset":false,"role":"figure","size":46567,"visible":true,"origin":"","legend":"\u003cp\u003e(A) \u003csup\u003e1\u003c/sup\u003eH-NMR, (B) FT-IR and (C) Raman spectrum of MIL, (D) Magnetization of MIL as functions of magnetic field at 298 K.\u003c/p\u003e","description":"","filename":"2.jpg","url":"https://assets-eu.researchsquare.com/files/rs-3875532/v1/896bc8fa933b6f55ba44c617.jpg"},{"id":49983371,"identity":"6a55e164-c75b-48a9-a474-6a38a4103186","added_by":"auto","created_at":"2024-01-22 16:23:16","extension":"jpg","order_by":3,"title":"Figure 3","display":"","copyAsset":false,"role":"figure","size":15910,"visible":true,"origin":"","legend":"\u003cp\u003eLinear sweep voltammetry of MIL-based electrolyte.\u003c/p\u003e","description":"","filename":"3.jpg","url":"https://assets-eu.researchsquare.com/files/rs-3875532/v1/0057de20234d4c95d90742a9.jpg"},{"id":49983375,"identity":"381e7d9a-e542-46c2-a3b2-37b222c994a9","added_by":"auto","created_at":"2024-01-22 16:23:17","extension":"jpg","order_by":4,"title":"Figure 4","display":"","copyAsset":false,"role":"figure","size":67802,"visible":true,"origin":"","legend":"\u003cp\u003eCV curves using MIL-based electrolyte in (A) absence and (B) presence of magnetic field at scan rates of (a) 0.1 V×s\u003csup\u003e-1\u003c/sup\u003e, (b) 0.3 V×s\u003csup\u003e-1\u003c/sup\u003e, (c) 0.5 V×s\u003csup\u003e-1\u003c/sup\u003e, (d) 0.8 V×s\u003csup\u003e-1\u003c/sup\u003e and (e) 1.0 V×s\u003csup\u003e-1\u003c/sup\u003e. (C) Specific capacitance as a function of scan rate in (a) absence and (b) presence of magnetic field. (D) CV curves using pure MIL electrolyte in presence of magnetic field at scan rates of (a) 0.1 V×s\u003csup\u003e-1 \u003c/sup\u003eand (c) 1.0 V×s\u003csup\u003e-1\u003c/sup\u003e, and in absence of magnetic field at scan rates of (b) 0.1 V×s\u003csup\u003e-1 \u003c/sup\u003eand (d) 1.0 V×s\u003csup\u003e-1\u003c/sup\u003e .\u003c/p\u003e","description":"","filename":"4.jpg","url":"https://assets-eu.researchsquare.com/files/rs-3875532/v1/9c88ad61856a297729714193.jpg"},{"id":49983373,"identity":"5fb8a697-1e9b-47e4-9cbe-fdec1742d05d","added_by":"auto","created_at":"2024-01-22 16:23:17","extension":"jpg","order_by":5,"title":"Figure 5","display":"","copyAsset":false,"role":"figure","size":60237,"visible":true,"origin":"","legend":"\u003cp\u003eGCD curves using MIL-based electrolyte in (A) absence and (B) presence of magnetic field at various current densities of (a) 0.1 mA×cm\u003csup\u003e-2\u003c/sup\u003e, (b) 0.15 mA×cm\u003csup\u003e-2\u003c/sup\u003e, (c) 0.2 mA×cm\u003csup\u003e-2 \u003c/sup\u003eand (d) 1.0 mA×cm\u003csup\u003e-2\u003c/sup\u003e. (C) Special capacitance using MIL-based electrolyte in (a) and (b) presence of magnetic field as a function of current densities. (D)Specific capacitance retention using MIL-based electrolyte in (a) absence and (b) presence of magnetic field for 5000 cycles.\u003c/p\u003e","description":"","filename":"5.jpg","url":"https://assets-eu.researchsquare.com/files/rs-3875532/v1/4a2a73f00ef8c5bb8fc295b1.jpg"},{"id":49983377,"identity":"810bdf30-b19d-4711-bbc4-8c68405c818f","added_by":"auto","created_at":"2024-01-22 16:23:17","extension":"jpg","order_by":6,"title":"Figure 6","display":"","copyAsset":false,"role":"figure","size":22590,"visible":true,"origin":"","legend":"\u003cp\u003eNyquist plot using electrolyte in (a)absence and (b) presence of magnetic field (0.3T). The inset is the electrical equivalent circuit.\u003c/p\u003e","description":"","filename":"6.jpg","url":"https://assets-eu.researchsquare.com/files/rs-3875532/v1/f9b029e79a818d6e7e11cee2.jpg"},{"id":49983376,"identity":"00bdb9e0-89c3-439c-b115-65f8f45b7b5e","added_by":"auto","created_at":"2024-01-22 16:23:17","extension":"jpg","order_by":7,"title":"Figure 7","display":"","copyAsset":false,"role":"figure","size":39418,"visible":true,"origin":"","legend":"\u003cp\u003eMechanism diagram of the internal structure of the electrolyte in the (A) absence and (B) presence of magnetic field. (C) FT-IR spectra of MIL in the (a) presence and (b)absence of a magnetic field.\u003c/p\u003e","description":"","filename":"7.jpg","url":"https://assets-eu.researchsquare.com/files/rs-3875532/v1/f5abe5b330b346d97fce3f9b.jpg"},{"id":56181854,"identity":"125c605d-4896-478b-bc59-677ab0ccd2ff","added_by":"auto","created_at":"2024-05-09 14:30:59","extension":"pdf","order_by":0,"title":"","display":"","copyAsset":false,"role":"manuscript-pdf","size":662545,"visible":true,"origin":"","legend":"","description":"","filename":"manuscript.pdf","url":"https://assets-eu.researchsquare.com/files/rs-3875532/v1/2fd07ba4-985f-4f86-9d81-c6421dd514f4.pdf"}],"financialInterests":"No competing interests reported.","formattedTitle":"Facile synthesis of magnetic ionic liquid with magnetic-tuning electrochemical performance","fulltext":[{"header":"1. Introduction","content":"\u003cp\u003eIn the electrochemical energy storage, work safety and high performance are equally important issues (Choi et al.,2012; Tiago et al., \u003cspan citationid=\"CR2\" class=\"CitationRef\"\u003e2020\u003c/span\u003e). As well-known, the electrolyte material is an key component for work safety and electrochemical performance of electrochemical energy storage. Therefore, there are lots of works reporting the effect of electrolyte materials on electrochemical performance of electrochemical energy storage. Up to now, the most electrolytes are water-based or organic solvent-based systems. Water-based electrolyte exhibits high ionic conductivity, leading to good electrochemical performance. Unfortunately, the electrochemical window of water-based electrolyte is narrow (only about 1.23V) at room temperature. At the same time, it is easy to corrode the device and the operating temperature range is limited to 0\u0026thinsp;~\u0026thinsp;100\u0026deg;C (Kuhnel et al., \u003cspan citationid=\"CR3\" class=\"CitationRef\"\u003e2016\u003c/span\u003e). Although traditional organic electrolytes have better overall performance than water-based electrolytes, yet they are volatile and flammable. These traditional organic electrolytes often cause serious safety problems (Goodenough \u0026amp; Kim, \u003cspan citationid=\"CR4\" class=\"CitationRef\"\u003e2010\u003c/span\u003e; Mtj et al., 2001). It is found that the introduction of fluorine atoms into the solvent electrolytes can effectively improve electrochemical performance of battery. For example, Hu L et al reported the synthesis and electrochemical performance of fluorinated organic solvents, which showed higher polarity and oxidation resistance comparing to organic solvents without fluorinating (Hu et al., \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e2013\u003c/span\u003e). At the same time, other additives (eg. MA, SA, PBF, PPF, etc) were also introduced to the electrolyte and could effectively improve the cycle and energy storage performance of carbonate electrolytes. Furthermore, the effect of the additives (eg. MMDS, DTD, TAP) on electrochemical performance was also investigated, in which these additives could effectively reduce the voltage drop (Xia et al., \u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e2017\u003c/span\u003e). For examples, Lee Jyh Tsung et al found that the electrochemical window increased from 0.8V to 1.5V after adding allyl ethyl carbonate to PC electrolyte (Lee et al., \u003cspan citationid=\"CR8\" class=\"CitationRef\"\u003e2004\u003c/span\u003e). However, these additives also brought some negative effects. For example, although the additive of VC provided excellent cyclic performance and charge/discharge capacity, yet the initial efficiency in the electrolyte with 2.0wt% VC was only 72.3%, which was lower than that in standard electrolyte (Yao et al., \u003cspan citationid=\"CR9\" class=\"CitationRef\"\u003e2015\u003c/span\u003e). Thermal stability of the electrolyte could be improved by phytic acid, but the capacity of the vanadium flow battery employing the vanadium electrolyte with phytic acid decreased significantly (Wu et al., \u003cspan citationid=\"CR10\" class=\"CitationRef\"\u003e2012\u003c/span\u003e). From above respects, it is still an high interesting to find a new electrolyte for improving the work safety and electrochemical performance.\u003c/p\u003e \u003cp\u003eRecently, it is found that ionic liquids (ILs) are a promising type of electrolyte material due to unique physical and chemical properties, such as low saturated vapor pressure, low flammability, high thermal stability, wide electrochemical window and green (Tsunashima et al., \u003cspan citationid=\"CR11\" class=\"CitationRef\"\u003e2009\u003c/span\u003e). EMinato Egashira et al reported synthesis and electrochemical performance of the imidazolium ionic liquids functionalized with cyanomethyl, which showed a higher cycle efficiency comparing to conventional organic solvent electrolytes (Egashira et al., \u003cspan citationid=\"CR12\" class=\"CitationRef\"\u003e2007\u003c/span\u003e). However, the slow kinetics of ionic liquids hinder the migration of ions, reducing the electrochemical storage performance (Armand et al., \u003cspan citationid=\"CR13\" class=\"CitationRef\"\u003e2009\u003c/span\u003e). To solve above problem, a mixed electrolyte based on ionic liquids and other solvents was developed, which could combine the advantages of each component. For example, the organic solvent was added to the ionic liquid electrolyte, which could reduce system viscosity and improve ion migration, thereby increasing in the power density of supercapacitors (Montanino et al., \u003cspan citationid=\"CR14\" class=\"CitationRef\"\u003e2014\u003c/span\u003e). The result was attributed to that the LiTFSI-PYR13TFSI-PYR13FSI mixtures exhibited high ion transport properties with about 10\u003csup\u003e\u0026minus;\u0026thinsp;3\u003c/sup\u003e S cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e at -20℃ (Appetecchi et al., \u003cspan citationid=\"CR15\" class=\"CitationRef\"\u003e2016\u003c/span\u003e). The magnetic ionic liquids (MILs) are a new class of ILs with special paramagnetic behavior (Hamaguchi. et al., 2004; Lage-Estebanez et al., \u003cspan citationid=\"CR17\" class=\"CitationRef\"\u003e2018\u003c/span\u003e), which are expected to act as electrolyte materials to improve ion transport properties and electrochemical performance. However, although MILs have been reported for various applications, such as catalyst, fluid-fluid separations, and chemical reactions, etc (Mohammad et al., \u003cspan citationid=\"CR18\" class=\"CitationRef\"\u003e2020\u003c/span\u003e; Feng et al., \u003cspan citationid=\"CR19\" class=\"CitationRef\"\u003e2018\u003c/span\u003e; Sajid, \u003cspan citationid=\"CR20\" class=\"CitationRef\"\u003e2019\u003c/span\u003e; Kowsari \u0026amp; Mohammadi, \u003cspan citationid=\"CR21\" class=\"CitationRef\"\u003e2016\u003c/span\u003e), yet, MILs are few reported for application in electrolyte.\u003c/p\u003e \u003cp\u003eHere, a new mixed electrolyte based on MILs was developed to improve ion transport properties and electrochemical performance. MILs do not only exhibit the excellent characteristics of ionic liquids, but also show magnetism. It will arrange in a magnetic field and form magnetic chains. The MIL in the mixed electrolyte forms magnetic chains under the magnetic field, and the non-magnetic organic solvent medium in the magnetic chain gap is expected to become a high-speed channel for ion transmission. These works provide a new method to simultaneously improve electrochemical performance and work safety of electrochemical energy storage.\u003c/p\u003e"},{"header":"2. Experimental","content":"\u003cdiv id=\"Sec3\" class=\"Section2\"\u003e \u003ch2\u003e2.1 Materials\u003c/h2\u003e \u003cp\u003e1-Butylimidazole (\u0026gt;\u0026thinsp;98%), Chloromethyl ether (\u0026gt;\u0026thinsp;95%) and the FeCl\u003csub\u003e3\u003c/sub\u003e\u0026middot;6H\u003csub\u003e2\u003c/sub\u003eO (\u0026gt;\u0026thinsp;99%) were purchased from Aladdin. The dichloromethane, deuterated dimethyl sulfoxide (DMSO-d6\u0026thinsp;\u0026gt;\u0026thinsp;99.9%) and ethyl acetate were purchased from Tianjin Kaitong Chemical Reagent Co., Ltd. Besides, the electrode of Platinum electrode, glassy carbon and carbon rod were purchased from Changsha Changjindiantang science and technology Co., Ltd.\u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec4\" class=\"Section2\"\u003e \u003ch2\u003e2.2 Synthesis of MIL\u003c/h2\u003e \u003cp\u003eThe MIL was synthesized by a two-step method as shown in following. Firstly, 16.2g 1-butyl imidazole and 10g chloromethyl ether were dissolved in 20mL dichloromethane under mechanical stirring at 9℃. The mixture was reacted at 30℃ for 3 h under the protection of N\u003csub\u003e2\u003c/sub\u003e, forming the IL. And then the IL was purified by washing with ethyl acetate and dichloromethane for two times. Secondly, 19.8g FeCl\u003csub\u003e3\u003c/sub\u003e\u0026middot;6H\u003csub\u003e2\u003c/sub\u003eO was added to 16g IL under mechanical stirring. The mixture was reacted at 30℃ for 3h under the protection of N\u003csub\u003e2\u003c/sub\u003e, forming MIL. Finally, the MIL was purified by rotary evaporator and vacuum at 80 ℃ for 24 h.\u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec5\" class=\"Section2\"\u003e \u003ch2\u003e2.3 Preparation of mixed electrolyte based on MIL\u003c/h2\u003e \u003cp\u003eThe electrolyte was prepared by blending MIL and an organic electrolyte(4 M LiCl/NMP) with a volume ratio of 5:1. To achieve a homogeneous and anhydrous mixture, the electrolyte was dispersed by ultrasound for 1h and dried under vacuum at 80℃ for 24 h.\u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec6\" class=\"Section2\"\u003e \u003ch2\u003e2.4 Characterization of MIL\u003c/h2\u003e \u003cp\u003eThe chemical structure of MIL was characterized by \u003csup\u003e1\u003c/sup\u003eH-NMR spectrum on a Avance III 600 MHz NMR spectrometer at room temperature. And the dimethyl sulfoxide-d\u003csub\u003e6\u003c/sub\u003e (DMSO-d\u003csub\u003e\u003cem\u003e6\u003c/em\u003e\u003c/sub\u003e) was used as solvent.\u003c/p\u003e \u003cp\u003eInfrared spectroscopy (FT-IR) spectra were obtained on a Thermo Fisher Spectrum One (Thermo Fisher, USA) and scanned from 500 to 4000 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e.\u003c/p\u003e \u003cp\u003eRaman measurements were carried out on In Via at a wavelength of 785 nm at 298 K.\u003c/p\u003e \u003cp\u003eThe magnetic properties of MIL were measured at room temperature by vibrating sample magnetometer (Micro Sense, LLC, USA) from 0 to 11000 Oe.\u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec7\" class=\"Section2\"\u003e \u003ch2\u003e2.5 Electrochemical performance\u003c/h2\u003e \u003cp\u003eThe electrochemical measurements of linear sweep voltammetry (LSV), cyclic voltammetry (CV) and electrochemical impedance spectroscopy (EIS) were characterized by CHI 660C workstation with three electrode systems. The working electrode, counter electrode and reference electrode were carbon rod, glassy carbon and Pt metal, respectively (as shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e1\u003c/span\u003e). The galvanostatic charge/discharge (GCD) was performed on LANHE CT2001A. The specific capacitance is calculated by following formula:\u003c/p\u003e \u003cp\u003e \u003cem\u003eC\u0026thinsp;=\u0026thinsp;I▪∆t /(A▪∆V)\u003c/em\u003e \u003c/p\u003e \u003cp\u003eWhere \u003cem\u003eA\u003c/em\u003e is the area of electrode, \u003cem\u003eI\u003c/em\u003e is the applied current, \u003cem\u003e∆t\u003c/em\u003e is the discharge time and \u003cem\u003e∆V\u003c/em\u003e is the change of capacitor voltage (Mirmohseni et al., \u003cspan citationid=\"CR22\" class=\"CitationRef\"\u003e2012\u003c/span\u003e). The diagram of electrochemical cell as shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e1\u003c/span\u003e. In the electrochemical cell, diameter of carbon rod and glassy carbon electrodes is both 3.0mm and the length of penetrating into the electrolyte is both 1.0cm. The area of platinum sheet in the electrolyte is about 1.0cm\u0026times;0.8cm. Besides, U-shaped magnet is used to provide a 0.3T magnetic field, and the distance d between the U-shaped magnet and the electrodes is 5.0mm.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003c/div\u003e"},{"header":"3. Results and discussion","content":"\u003cp\u003eFigure\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003eA shows the \u003csup\u003e1\u003c/sup\u003eH-NMR spectrum of MIL and the data is listed as follows: δ=9.50 (s, 1H, -N=CH-N-), 7.90 (s, 2H, -N-CH=CH-N-), 5.53 (s, 2H, -N-CH\u003csub\u003e2\u003c/sub\u003e-O-), 4.23 (s, 2H -N-CH\u003csub\u003e2\u003c/sub\u003e-CH\u003csub\u003e2\u003c/sub\u003e-), 4.03 (s, 2H, CH\u003csub\u003e3\u003c/sub\u003e-CH\u003csub\u003e2\u003c/sub\u003e-O-), 1.81 (t, 2H, J=3.6Hz, -CH\u003csub\u003e2\u003c/sub\u003e-CH\u003csub\u003e2\u003c/sub\u003e-CH\u003csub\u003e3\u003c/sub\u003e), 1.28(s, 2H, -CH\u003csub\u003e2\u003c/sub\u003e-CH\u003csub\u003e3\u003c/sub\u003e), 0.92(s, 6H,-CH\u003csub\u003e3\u003c/sub\u003e). The ratio of integral peak area ratio was consistent with the ratio of the number of hydrogen atoms at different chemical shifts. At the same time, no additional peaks were observed in the \u003csup\u003e1\u003c/sup\u003eH-NMR spectrum of the intermediates. The result indicated the formation of MIL. The structure of MIL was further characterized by FT-IR spectrum as shown in Fig.\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003eB. The wide absorption band around 3412.0 cm\u003csup\u003e-1\u003c/sup\u003e was assigned to intermolecular hydrogen bonding (Chen et al., 2018). The absorption peaks at 3144.0 cm\u003csup\u003e-1\u003c/sup\u003e and 2960.0 cm\u003csup\u003e-1\u003c/sup\u003e were assigned to C-H stretching modes of the imidazolium ring (Tao et al., \u003cspan citationid=\"CR24\" class=\"CitationRef\"\u003e2014\u003c/span\u003e). The absorbance peaks around 1553.0 cm\u003csup\u003e-1\u003c/sup\u003e and 1390.0 cm\u003csup\u003e-1\u003c/sup\u003e were assigned to C-H bending modes and C=C stretching vibrations on the imidazolium ring, respectively (Chen et al., 2018). The absorbance bands at 1158.0 cm\u003csup\u003e-1\u003c/sup\u003e and 1107.0 cm\u003csup\u003e-1\u003c/sup\u003e were assigned to C-N stretching modes and C-O stretching modes of MIL, respectively (Haddad et al., \u003cspan citationid=\"CR25\" class=\"CitationRef\"\u003e2017\u003c/span\u003e; Chen. et al., 2010). The absorbance peaks below 1000 cm\u003csup\u003e-1\u003c/sup\u003e were assigned to C-C or C-N bending vibration of MIL. Fig.\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003eC shows the Raman spectrum of MIL. A new strong absorption peak at 331.0 cm\u003csup\u003e-1\u003c/sup\u003e was observed, which was assigned to FeCl\u003csub\u003e4\u003c/sub\u003e\u003csup\u003e-\u003c/sup\u003e anion (Melissa et al., \u003cspan citationid=\"CR27\" class=\"CitationRef\"\u003e2001\u003c/span\u003e). These results further confirm the successful synthesis of MIL. The magnetization of MIL was further characterized at a magnetic field range from 0 to 11000 Oe as shown in Fig.\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003eD. The magnetization of MIL showed a linear response to the applied magnetic field, indicating that it had paramagnetic behavior (Wang et al., \u003cspan citationid=\"CR28\" class=\"CitationRef\"\u003e2019\u003c/span\u003e). The magnetic susceptibility of MIL was determined to be 1.82\u0026times;10\u003csup\u003e-5\u003c/sup\u003e emu/g.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003eLinear sweep voltammetry measurements were performed for determining the electrochemical window (ESW) as shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003e. The electrolyte clearly showed the large ESW of approximately 5.0V, ranging from \u0026minus;\u0026thinsp;7.5 V to -2.5 V. This was consistent with ESW of ILs reported in previous work (Suarez et al., \u003cspan citationid=\"CR29\" class=\"CitationRef\"\u003e1997\u003c/span\u003e), in which also showed wide potential ranges about 4.5-5V. However, the ESW of MIL-based electrolyte was obviously larger than that (eg.2.5V) of organic electrolytes reported in previous work (Liew et al., \u003cspan citationid=\"CR30\" class=\"CitationRef\"\u003e2016\u003c/span\u003e). The result confirmed that the MIL-based electrolyte showed excellent stability at high voltages for application in electrochemical energy storage with high voltage (Bonhote et al., \u003cspan citationid=\"CR31\" class=\"CitationRef\"\u003e1996\u003c/span\u003e).\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003eThe cyclic voltammetry (CV) curves using MIL-based electrolyte were characterized at different scan rates from 0.1 to 1 V\u0026sdot;s\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e in the absence and presence of magnetic field (0.3T) as shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003eA and Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003eB, respectively. It was seen that the CV curves were nearly rectangular shape at the lower scan rate than 0.1V\u0026sdot;s\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e, indicating high ion transport properties. The specific capacitance using MIL-based electrolyte was further calculated according to CV curves in the absence and presence of magnetic field as shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003eC. As expected, the specific capacitance decreased significantly with increasing in the scan rate. When the scan rate increased from 0.1 to 1 V\u0026sdot;s\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e, the specific capacitance of MIL-based electrolyte drastically decreased from 18.4 (or 13.1) to 4.7 (or 2.4) mF\u0026sdot;cm\u003csup\u003e\u0026minus;\u0026thinsp;2\u003c/sup\u003e in the presence (or absence) of magnetic field. This result was attributed to that these ions were not enough time for diffusing to the surface of the electrode material at higher scan rates (Melissa et al., \u003cspan citationid=\"CR27\" class=\"CitationRef\"\u003e2001\u003c/span\u003e). Moreover, it was found that the capacitance of electrode with 0.3T magnetic field was obviously larger than that of electrode without magnetic field. The result indicated that the capacitance of electrode using MIL-based electrolyte could be easily tuned and improved by applying magnetic field. The result was attributed to that the MIL was arranged along the direction of the magnetic field, facilitating the migration of ions on the electrode interface. Above result was further confirmed by the CV curves as shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003eD. It clearly showed CV curves using pure MIL as electrolyte in presence and absence of magnetic field. Obviously, the capacitance of electrode using the pure MIL electrolyte became smaller under a magnetic field comparing to no magnetic field. This result was attributed to that the ions of the MIL were arranged in the direction of the magnetic field, inhibiting its diffusion and migration in the electrochemical\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003eThe effect of magnetic field on GCD curves was also characterized as shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003eA-B. The discharge time after applying a magnetic field was longer comparing to no magnetic field. The specific capacitance as function of current densities was calculated from GCD curves in presence and absence of magnetic field as shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003eC. It clearly showed that the specific capacitance using MIL-based electrolyte in presence of magnetic field (0.3T) is 15.8mF\u003cem\u003e\u0026sdot;\u003c/em\u003ecm\u003csup\u003e\u0026minus;\u0026thinsp;2\u003c/sup\u003e at a current density of 0.1mA\u003cem\u003e\u0026sdot;\u003c/em\u003ecm\u003csup\u003e\u0026minus;\u0026thinsp;2\u003c/sup\u003e. However, the corresponding value was 10.9 mF\u003cem\u003e\u0026sdot;\u003c/em\u003ecm\u003csup\u003e\u0026minus;\u0026thinsp;2\u003c/sup\u003e in absence of magnetic field. These results further proved that MIL in the mixed electrolyte was arranged along the direction of the magnetic field under the magnetic field, while the Li\u003csup\u003e+\u003c/sup\u003e and Cl\u003csup\u003e\u0026minus;\u003c/sup\u003e dispersed in the NMP could move freely. At the same time, the magnetic field reduced the viscous resistance of the migration ions in IL, resulting in better electrochemical performance. Moreover, it retained the wide electrochemical window for electrochemical cell device. Long-term stability is a key role for the practical application of electrochemical cell device. The stability of MIL-based electrolyte was evaluated by sequential charge-discharge for 5000 cycles at a current density of 0.3 mA\u0026sdot;cm\u003csup\u003e\u0026minus;\u0026thinsp;2\u003c/sup\u003e as shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003eD. The specific capacitance still retained 79.0% after 5000 charge-discharge cycles in presence of magnetic field, which was higher than that (70.8%) in absence of magnetic field. These results do not only confirm that the external magnetic field will improve the stability of electrochemical cell device using MIL-based electrolyte, but also further demonstrate the magnetic field controllability of the electrochemical performance of the MIL-based electrolyte.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003eEIS spectra using MIL-based electrolyte were characterized and compared in presence and absence of magnetic field as shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig6\" class=\"InternalRef\"\u003e6\u003c/span\u003e. It clearly showed a semicircle and a 45-degree linear section, which represented the resistance of charge transfer and the ions diffusion, respectively (Du et al., \u003cspan citationid=\"CR32\" class=\"CitationRef\"\u003e2009\u003c/span\u003e). The bulk resistance (Rs) of electrolyte and the interfacial charge transfer resistance (Rct) were calculated and concluded in Table\u0026nbsp;\u003cspan refid=\"Tab1\" class=\"InternalRef\"\u003e1\u003c/span\u003e. The Rs (51.3Ω) of electrolyte in presence of magnetic field was smaller than that (57.9 Ω) in absence of magnetic field. Similarly, the Rct of electrolyte in presence and absence of magnetic field was about 142.6Ω and 185.5Ω, respectively. After applying a magnetic field, the resistance of the MIL-based electrolyte and the Rct at the interface were significantly reduced, thereby enhancing the capacitive behavior. These results further confirmed the formation of MIL-based electrolyte with high ion transport properties by applying magnetic field. Here, the result was different from previous work (zhang et al., \u003cspan citationid=\"CR33\" class=\"CitationRef\"\u003e2016\u003c/span\u003e), in which the Ionic conductivity decreased with increasing in magnetic field. Here, in an external magnetic field, MIL was aligned along the magnetic field to form micro-domains (Nykaza et al., \u003cspan citationid=\"CR34\" class=\"CitationRef\"\u003e2016\u003c/span\u003e), the viscosity of the system was reduced, and the ions of Li\u003csup\u003e+\u003c/sup\u003e and Cl\u003csup\u003e\u0026minus;\u003c/sup\u003e dispersed in NMP could be quickly transferred in the microdomain.The electrochemical performance of different ionic liquid electrolytes is compared in Table\u0026nbsp;\u003cspan refid=\"Tab2\" class=\"InternalRef\"\u003e2\u003c/span\u003e. It can be seen that the MIL electrochemical has outstanding performance in terms of electrochemical window and cycle stability.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003e \u003cdiv class=\"gridtable\"\u003e\u003ctable float=\"Yes\" id=\"Tab1\" border=\"1\"\u003e \u003ccaption language=\"En\"\u003e \u003cdiv class=\"CaptionNumber\"\u003eTable 1\u003c/div\u003e \u003cdiv class=\"CaptionContent\"\u003e \u003cp\u003eThe Rs and Rct in absence and presence of magnetic field.\u003c/p\u003e \u003c/div\u003e \u003c/caption\u003e \u003ccolgroup cols=\"3\"\u003e \u003cdiv align=\"left\" class=\"colspec\" colname=\"c1\" colnum=\"1\"\u003e\u003c/div\u003e \u003cdiv align=\"char\" char=\".\" class=\"colspec\" colname=\"c2\" colnum=\"2\"\u003e\u003c/div\u003e \u003cdiv align=\"char\" char=\".\" class=\"colspec\" colname=\"c3\" colnum=\"3\"\u003e\u003c/div\u003e \u003cthead\u003e \u003ctr\u003e \u003cth align=\"left\" colname=\"c1\"\u003e \u003cp\u003eR(Ω)\u003c/p\u003e \u003c/th\u003e \u003cth align=\"left\" colname=\"c2\"\u003e \u003cp\u003eMagnetic Field\u003c/p\u003e \u003cp\u003e(0.0 T)\u003c/p\u003e \u003c/th\u003e \u003cth align=\"left\" colname=\"c3\"\u003e \u003cp\u003eMagnetic Field\u003c/p\u003e \u003cp\u003e(0.3 T)\u003c/p\u003e \u003c/th\u003e \u003c/tr\u003e \u003c/thead\u003e \u003ctbody\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eRs\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c2\"\u003e \u003cp\u003e57.9\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e51.3\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eRct\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c2\"\u003e \u003cp\u003e185.5\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e142.6\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003c/tbody\u003e \u003c/colgroup\u003e \u003c/table\u003e\u003c/div\u003e \u003c/p\u003e \u003cp\u003e \u003cdiv class=\"gridtable\"\u003e\u003ctable float=\"Yes\" id=\"Tab2\" border=\"1\"\u003e \u003ccaption language=\"En\"\u003e \u003cdiv class=\"CaptionNumber\"\u003eTable 2\u003c/div\u003e \u003cdiv class=\"CaptionContent\"\u003e \u003cp\u003eComparison of electrochemical properties of different ionic liquid electrolytes.\u003c/p\u003e \u003c/div\u003e \u003c/caption\u003e \u003ccolgroup cols=\"4\"\u003e \u003cdiv align=\"left\" class=\"colspec\" colname=\"c1\" colnum=\"1\"\u003e\u003c/div\u003e \u003cdiv align=\"left\" class=\"colspec\" colname=\"c2\" colnum=\"2\"\u003e\u003c/div\u003e \u003cdiv align=\"left\" class=\"colspec\" colname=\"c3\" colnum=\"3\"\u003e\u003c/div\u003e \u003cdiv align=\"left\" class=\"colspec\" colname=\"c4\" colnum=\"4\"\u003e\u003c/div\u003e \u003cthead\u003e \u003ctr\u003e \u003cth align=\"left\" colname=\"c1\"\u003e \u003cp\u003eElectrochemical window\u003c/p\u003e \u003c/th\u003e \u003cth align=\"left\" colname=\"c2\"\u003e \u003cp\u003eThe specific capacitance\u003c/p\u003e \u003c/th\u003e \u003cth align=\"left\" colname=\"c3\"\u003e \u003cp\u003eCapacitance retention rate (cycle number)\u003c/p\u003e \u003c/th\u003e \u003cth align=\"left\" colname=\"c4\"\u003e \u003cp\u003eReference\u003c/p\u003e \u003c/th\u003e \u003c/tr\u003e \u003c/thead\u003e \u003ctbody\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003e5.0V\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e15.8 mF\u0026sdot;cm\u003csup\u003e\u0026minus;\u0026thinsp;2\u003c/sup\u003e\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003e79.0% (5000)\u003c/p\u003e \u003cp\u003e98% (30)\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003eThis paper\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003e-\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e147mAh.g\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003e96% (30)\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003eTsunashima et al., \u003cspan citationid=\"CR11\" class=\"CitationRef\"\u003e2009\u003c/span\u003e\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003e2.0V\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e153mAh.g\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003e90% (4)\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003eMontanino et al., \u003cspan citationid=\"CR14\" class=\"CitationRef\"\u003e2014\u003c/span\u003e\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003e5.0V\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e135mAh.g\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003e-\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003eAppetecchi et al., \u003cspan citationid=\"CR15\" class=\"CitationRef\"\u003e2016\u003c/span\u003e\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003e3.5V\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e-\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003e90% (50)\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003eEgashira et al., \u003cspan citationid=\"CR12\" class=\"CitationRef\"\u003e2007\u003c/span\u003e\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003c/tbody\u003e \u003c/colgroup\u003e \u003c/table\u003e\u003c/div\u003e \u003c/p\u003e \u003cp\u003eThe magnetic tuning mechanism in electrochemical performance of MIL-based electrolyte was further investigated and proposed as shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig7\" class=\"InternalRef\"\u003e7\u003c/span\u003e. As shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig7\" class=\"InternalRef\"\u003e7\u003c/span\u003eA, the ions of Li\u003csup\u003e+\u003c/sup\u003e and Cl\u003csup\u003e\u0026minus;\u003c/sup\u003e were randomly distributed in MIL-based electrolyte in the absence of magnetic field. In a comparison, the MIL is parallel to the magnetic field direction in the presence of magnetic field, forming a ion transport pathway in the gap of flux linkage and then drive Li\u003csup\u003e+\u003c/sup\u003e and Cl\u003csup\u003e\u0026minus;\u003c/sup\u003e migrate between two electrodes(Fig.\u0026nbsp;\u003cspan refid=\"Fig7\" class=\"InternalRef\"\u003e7\u003c/span\u003eB). Hence, the external magnetic field can improve the electrochemical performance by reducing the internal resistance in the system. These oriented structures are contributed to accelerate ion mobility in the electrolyte, improving the conductivity. Differing from the traditional electrolyte, it can form conductive paths in the direction of the external magnetic field. Above result was further confirmed by the FT-IR spectra of MIL-based electrolyte without and with magnetic field as shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig7\" class=\"InternalRef\"\u003e7\u003c/span\u003eC. In the test of FT-IR spectra, a U-shaped magnet is placed at the FT-IR probe to provide magnetic field, which can provide 0.3T magnetic field strength. After applying a magnetic field, the peak position of MIL's γC(2)H decreased from 844.21 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e to 837.77 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e. According to the study of the Christopher M. B\u003csup\u003e[32]\u003c/sup\u003e, the C(2)H is particularly sensitive to the interactions between anions and cations, leading to a reduction in frequency band. So, the change in frequency band is due to the change in the force between the internal anions and cations. The anions form Fe-Cl\u0026hellip;Cl-Fe structure in the presence of the external magnetic field, enhancing the interaction between the anions (Abel et al., \u003cspan citationid=\"CR36\" class=\"CitationRef\"\u003e2014\u003c/span\u003e). At the same time, the interaction between anions with the C(2)H on the imidazole ring is correspondingly reduced (Burba et al., 2019). Therefore, the infrared spectrum is blue shift under the magnetic field. The ionic liquid arranged along the magnetic field in the electrolyte, forming a conductive path. In summary, the pure MIL electrolyte undergoes ion alignment under a magnetic field, the capacitance is reduced. In contrast, the capacitance of the mixed electrolyte with the applied magnetic field increases. This suggests that although the movement of MIL anions and cations under the magnetic field is restricted, the gaps formed by the arrangement along the magnetic field provide rapid migration channels for the lithium salt. The capacitance of the MIL-based mixed electrolyte increases under the mutual competition.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e"},{"header":"4. Conclusion","content":"\u003cp\u003eIn this study, a new type of MIL-based mixed electrolyte with magnetic response was prepared. The electrochemical performance of the MIL-based mixture electrolyte was significantly improved under external magnetic field. Compared with the absence of a magnetic field, the specific capacitance increases from 10.9 to 15.8 mF\u0026sdot;cm\u003csup\u003e\u0026minus;\u0026thinsp;2\u003c/sup\u003e at a current density of 0.1 mA\u0026sdot;cm\u003csup\u003e\u0026minus;\u0026thinsp;2\u003c/sup\u003e after applying 0.3T magnetic field. Similarly, the capacitance retention rate increased from 70.8\u0026ndash;79.0% for 5000 charging/discharging cycle. In addition, the EIS test showed that the resistance of the system decreased after applying a magnetic field. Studies proved that MIL could magnetically responsive under a magnetic field and the ions of MIL was aligned along the direction of the magnetic field. The oriented structure provided an efficient transmission path for the migration of Li\u003csup\u003e+\u003c/sup\u003e and Cl\u003csup\u003e\u0026minus;\u003c/sup\u003e, thereby improving the electrochemical performance of the system. The work opens up a new direction for improving the performance of electrochemical energy storage.\u003c/p\u003e"},{"header":"Declarations","content":"\u003ch2\u003eAuthor Contribution\u003c/h2\u003e\u003cp\u003eNing Gu:Conceptualization,Investigation,Roles/Writing-original draft;Xiaolin Li:Conceptualization,Investigation;Miao Gao:Formal analysis,Investigation;Zixuan Liu:Formal analysis;Qichao Liu:Review \u0026amp; Editing;Yang Cao:Writing - Review \u0026amp; Editing;Youyi Sun:Roles/Writing-original draf,Funding acquisition.\u003c/p\u003e\u003ch2\u003eAcknowledgments\u003c/h2\u003e \u003cp\u003eThe authors are grateful for the support of Shanxi province and Shanxi Provincial Natural Science Foundation (202104021301059, YDZJSX2021A026, TZLH20230818009, 202204021301049) and Special fund for science and technology innovation teams of Shanxi province.\u003c/p\u003e"},{"header":"References","content":"\u003col\u003e\u003cli\u003e\u003cspan\u003eChoi, NS., Chen, Z., Freunberger, SA., Ji, XL., Sun, YK., Amine, K.,Yushin, G,, Nazar, LF., Cho, J., \u0026amp; Bruce, PG. (2012). Challenges facing lithium batteries and electrical double-layer capacitors. Angew Chem Int Ed Engl, 51, 9994\u0026ndash;10024.\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eTiago, Gao., Matias, Ias., Ribeiro, APC., \u0026amp; Martins, LMDRS. (2020). Application of ionic liquids in electrochemistry-recent advances. Molecules, 25, 5812\u0026ndash;5839.\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eKuhnel, RS., Reber, D., Remhof, A., Figi, R., Bleiner, D., \u0026amp; Battaglia, C. (2016). Water in salt electrolytes enable the use of cost effective aluminum current collectors for aqueous high voltage batteries. Chemical Communications, 52, 10435\u0026ndash;10438.\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eGoodenough, JB., \u0026amp; Kim, Y. (2010). Challenges for Rechargeable Li Batteries. Chemistry of Materials, 22, 587\u0026ndash;603.\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eMtj, Ma..(2001). 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J Mol Liq, 256, 175\u0026ndash;182.\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eMohammad, RA., Mohammad, AZ., Meysam, Y., Morteza, T., \u0026amp; Saeid, A. (2020). Synthesis, characterization and catalytic application of tributyl(carboxymethyl)phosphonium bromotrichloroferrate as a new magnetic ionic liquid for the preparation of 2,3-dihydroquinazolin-4(1H)-ones and 4H-pyrimidobenzothiazoles. Res Chem Intermed, 46, 3945\u0026ndash;3960.\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eFeng, XT., Zhang, W., Zhang, TH., \u0026amp; Yao, S. (2018). Systematic investigation for extraction and separation of polyphenols in tea leaves by magnetic ionic liquids. J Sci Food Agric, 98, 4550\u0026ndash;4560.\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eSajid, M. (2019). Magnetic ionic liquids in analytical sample preparation: A literature review. 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Appl Spectrosc, 73, 511\u0026ndash;519.\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eAbel, GS., Imanol, DP., \u0026amp; Pedro, M. (2014). Anion-π and halide-halide nonbonding interactions in a new ionic liquid based on imidazolium cation with three dimensional magnetic ordering in the solid state. American Chemical Socity, 53, 8384\u0026ndash;8396.\u003c/span\u003e\u003c/li\u003e\u003c/ol\u003e"}],"fulltextSource":"","fullText":"","funders":[],"hasAdminPriorityOnWorkflow":false,"hasManuscriptDocX":true,"hasOptedInToPreprint":true,"hasPassedJournalQc":"","hasAnyPriority":false,"hideJournal":false,"highlight":"","institution":"","isAcceptedByJournal":true,"isAuthorSuppliedPdf":false,"isDeskRejected":"","isHiddenFromSearch":false,"isInQc":false,"isInWorkflow":false,"isPdf":false,"isPdfUpToDate":true,"isWithdrawnOrRetracted":false,"journal":{"display":true,"email":"[email protected]","identity":"ionics","isNatureJournal":false,"hasQc":true,"allowDirectSubmit":false,"externalIdentity":"","sideBox":" Learn more about [Ionics](https://www.springer.com/journal/11581) ","snPcode":"11581","submissionUrl":"https://mc.manuscriptcentral.com/ionics","title":"Ionics","twitterHandle":"","acdcEnabled":true,"dfaEnabled":true,"editorialSystem":"stoa","reportingPortfolio":"Springer Hybrid","inReviewEnabled":true,"inReviewRevisionsEnabled":false},"keywords":"Magnetic ionic liquid, Electrochemical performance, Electrolyte, Magnetic tuning, Simulation","lastPublishedDoi":"10.21203/rs.3.rs-3875532/v1","lastPublishedDoiUrl":"https://doi.org/10.21203/rs.3.rs-3875532/v1","license":{"name":"CC BY 4.0","url":"https://creativecommons.org/licenses/by/4.0/"},"manuscriptAbstract":"\u003cp\u003eA new magnetic ionic liquid (MIL) based on 1-methylethyl ether-3-butylimidazole and [FeCl\u003csub\u003e4\u003c/sub\u003e]\u003csup\u003e−\u003c/sup\u003e is synthesized for application in electrolyte. It is found that the electrochemical performance of magnetic ionic liquid based mixed electrolyte can be improved by applying magnetic field. The enhanced electrochemical performance is attributed to the formation of microdomain in the mixed electrolyte under magnetic field. The ions of MIL can align along the direction of the magnetic field, providing the efficient transmission path for the migration of Li\u003csup\u003e+\u003c/sup\u003e and Cl\u003csup\u003e−\u003c/sup\u003e. Under magnetic control, the MI-based electrolyte does not only retain its wide electrochemical window characteristics, but also solves the problem of limiting the high viscosity of IL as electrolyte. 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