ORCID Profile
0000-0002-0555-2846
Current Organisation
Universidad del Pais Vasco
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Publisher: Wiley
Date: 02-03-2023
DOI: 10.1002/APP.53809
Abstract: Herein, we describe the use of single‐ion conducting block copolymer (SIC) as an additional lithium salt additive to a ternary solid polymer electrolyte (SPE), consisting of a poly(styrene‐ b ‐1‐((2‐acryloyloxy)ethyl)‐3‐butylimidazolium bis(trifluoromethanesulfo‐nyl)imide) (S‐ImTFSI 64‐16 ) block copolymer, a N ‐propyl‐ N ‐methylpyrrolidinium bis(fluorosulfonyl)imide (C 3 mpyrFSI) ionic liquid (IL) and a lithium bis(fluorosulfonyl) imide (LiFSI) salt. For this purpose, the S‐ImTFSI 64‐16 was substituted by a SIC, based on poly(styrene‐ b ‐((4‐styrenesulfonyl)(trifluoromethanesulfonyl)imide lithium salt)) (S‐STFSILi 64‐16 ), at various molar ratios. The impact of the SIC concentration on the phase behavior and transport properties of the SPEs was investigated by means of differential scanning calorimetry, electrochemical impedance spectroscopy, and diffusion NMR. In addition, the electrochemical performance of the SPEs was assessed in lithium symmetrical cell at 50 and 80°C. Finally, the cycling performance of a selected SPE was also assessed at 80°C in a Li│NMC 111 cell with capacity loading of 1.3 mAh.cm −2 at a C‐rate of 0.1 C. The Li│NMC 111 full cell was able to deliver a stable capacity of 0.94 mAh.cm −2 after 20 cycles, corresponding to a capacity of 117 mAh.g −1 . These results demonstrates that PIL block copolymer—IL—salt composites represent a promising choice of electrolyte for the next generation of solid‐state high energy density lithium metal batteries.
Publisher: Royal Society of Chemistry (RSC)
Date: 2015
DOI: 10.1039/C5CP03797B
Abstract: Impact of polymerizable moiety on the phase behaviour of imidazolium based ionic liquid crystal as a function of water content.
Publisher: Royal Society of Chemistry (RSC)
Date: 2022
DOI: 10.1039/D2PY00592A
Abstract: A perspective on using plastic waste as an alternative feedstock for the energy storage sector through upcycling. Materials for electrodes, electrolytes or binders could be obtained from both advanced combustion and depolymerization methods.
Publisher: Wiley
Date: 15-06-2022
Abstract: Redox‐polymer nanoparticles are a promising solution to avoid the detrimental dissolution of organic electrode materials while showing discrete redox processes. In this work, catechol‐based redox‐active polymer nanoparticles (cRPNs) were synthesized through one‐step emulsion polymerization with a tunable size from 25 to 150 nm. The fresh cRPNs were characterized and showed a reversible redox process centered at 0.50 V (vs. Ag/AgCl) in 1 M H 2 SO 4 . Unexpectedly, the cRPN latex aged after days passing from white to pink. This aging resulted in a shift of its redox potential toward higher values, which could be associated to autoxidation of the catechol groups and subsequent crosslinking of NPs due to catechol dimer formation. Finally, we compared the performance of fresh and aged cRPNs in a hybrid supercapacitor device, proving how the aging effect had some benefits such as an increase in the voltage output, specific capacitance, cyclability and Coulombic efficiencies of the device.
Publisher: American Chemical Society (ACS)
Date: 27-06-2023
Publisher: Royal Society of Chemistry (RSC)
Date: 2020
DOI: 10.1039/D0SE00531B
Abstract: New redox-active polymer nanoparticles present that the redox potential of the catechol group is affected by the presence of the pyridine. This positive potential gain is associated to the proton trap effect, which benefits the performance of lithium-ion–polymer batteries.
Publisher: The Royal Society of Chemistry
Date: 20-10-2020
DOI: 10.1039/9781788019743-00288
Abstract: All-organic batteries based on redox polymers represent an emerging new battery technology with potential application in the Internet of Things, smart packaging and clothing as well as mobile devices. Indeed, organic redox polymers feature highly attractive advantages compared to inorganic-based materials with regards to these applications, such as processability, flexibility, high rate performance, long cycle life and the ability to prepare them from renewable resources. This chapter aims to provide a comprehensive review on the current state of the art of all-organic batteries based on redox polymers, focusing on all battery prototypes reported to date and the nature of the ion carriers involved in their redox reactions. Illustrating the gradual research direction transition observed during the development of the all-organic battery technology, going from an alkali metal-based ion carrier battery system, similar to a lithium-ion battery, to a molecular ion-based and finally a proton-based ion carrier battery system. A general introduction to battery terminology and the various cell configurations is also given. Finally, future perspectives on all-organic batteries are discussed, summarizing the major challenges that remain to be overcome by the current state-of-the-art technology to unlock their commercial implementation.
Publisher: Wiley
Date: 28-01-2019
Publisher: Elsevier BV
Date: 02-2020
Publisher: Royal Society of Chemistry (RSC)
Date: 2023
DOI: 10.1039/D2MH01335E
Abstract: Design of dual redox-active porous polymers towards high-energy density and performance organic electrode materials for lithium metal battery and symmetric all-organic battery applications.
Publisher: Wiley
Date: 17-12-2020
Publisher: Wiley
Date: 04-11-2012
DOI: 10.1002/APP.38666
Publisher: The Electrochemical Society
Date: 05-01-2020
Abstract: In this work, we present a polymerized ionic liquid block copolymer (PBCP) film where relevant properties such as ionic conductivity and electrochemical parameters are tailored by using a ternary system comprised of poly(styrene-b-1-((2-acryloyloxy)ethyl)−3-butylimidazolium bis(tri-fluoromethanesulfonyl)imide), LiFSI salt and ethylene carbonate (EC) as a cosolvent. It was found that EC efficiently decreases the glass transition temperature of the ionic block, resulting in an improved ionic conductivity and efficient platting/stripping of lithium. By using an optimal ratio of EC/LiFSI at relatively high LiFSI amount, Li∣Li symmetrical cells at 50 °C show an overpotential as low as 70 mV at 0.1 mA.cm −2 along with a high lithium transport number of 0.56 (t Li + ). All-solid-state full cells based on lithium iron phosphate cathode paired with a lithium metal anode reveal a rather stable cycling at both 50 °C and 70 °C. A negligible capacity fading is observed up to 30 cycles where a specific capacity as high as 161 mAh.g −1 is achieved with a coulombic efficiency of 99.9%. Thus, this work demonstrates an important pathway for tailoring the properties of solid state polymer electrolytes for emerging and specially designed block copolymer architectures comprising domains that give both excellent ionic conduction along with desirable mechanical properties.
Publisher: Wiley
Date: 21-01-2020
Abstract: With increasing demands for safe, high capacity energy storage to support personal electronics, newer devices such as unmanned aerial vehicles, as well as the commercialization of electric vehicles, current energy storage technologies are facing increased challenges. Although alternative batteries have been intensively investigated, lithium (Li) batteries are still recognized as the preferred energy storage solution for the consumer electronics markets and next generation automobiles. However, the commercialized Li batteries still have disadvantages, such as low capacities, potential safety issues, and unfavorable cycling life. Therefore, the design and development of electromaterials toward high-energy-density, long-life-span Li batteries with improved safety is a focus for researchers in the field of energy materials. Herein, recent advances in the development of novel organic electrolytes are summarized toward solid-state Li batteries with higher energy density and improved safety. On the basis of new insights into ionic conduction and design principles of organic-based solid-state electrolytes, specific strategies toward developing these electrolytes for Li metal anodes, high-energy-density cathode materials (e.g., high voltage materials), as well as the optimization of cathode formulations are outlined. Finally, prospects for next generation solid-state electrolytes are also proposed.
Publisher: Royal Society of Chemistry (RSC)
Date: 2012
DOI: 10.1039/C2CC17143K
Abstract: We have shown that protic ionic liquids, pILs, are effective coagulation solvents for the regenerated of silk fibroin, RSF. We show that the choice of pIL has a dramatic effect on the composition of the RSF. Additionally the use of pILs as the coagulator eliminates the need for volatile organic solvents in silk processing.
Publisher: CSIRO Publishing
Date: 2015
DOI: 10.1071/CH14240
Abstract: The addition of diluents to ionic liquids (ILs) has recently been shown to enhance the transport properties of ILs. In the context of electrolyte design, this enhancement allows the realisation of IL-based electrolytes for metal–air batteries and other storage devices. It is likely that diluent addition not only impacts the viscosity of the IL, but also the ion–ion interactions and structure. Here, we investigate the nano-structured 1-methyl-3-octylimidazolium chloride (OMImCl) with varying water concentrations in the presence of two metal salts, zinc chloride and magnesium chloride. We find that the choice of metal salt has a significant impact on the structure and transport properties of the system this is explained by the water structuring and destructing properties of the metal salt.
Publisher: Wiley
Date: 30-10-2018
Publisher: American Chemical Society (ACS)
Date: 03-11-2021
Publisher: Elsevier BV
Date: 11-2021
Publisher: American Chemical Society (ACS)
Date: 10-10-2023
Publisher: American Chemical Society (ACS)
Date: 03-10-2018
Publisher: Royal Society of Chemistry (RSC)
Date: 2013
DOI: 10.1039/C3CC43837F
Abstract: We describe a convenient route to the alignment of cyclic peptide nanotubes (CPNs). The key lies in the use of nanostructured ionic liquids. An ionic liquid supported membrane with orientated domains is demonstrated, leading to aligned CPNs within a solid membrane.
Publisher: Wiley
Date: 29-10-2020
Abstract: Single‐ion conducting polymer electrolytes (SIPE) have attracted a lot of interest for application in high energy density lithium metal batteries. SIPEs possess lithium transport numbers close to unity, which does not provoke concentration gradients and holds the promise of limiting lithium dendrite formation. In this article, we have optimized a single‐ion polymer incorporating the most successful chemical units in polymer electrolytes, such as ethylene oxide, carbonate, and a lithium sulfonimide. This single‐ion poly(ethylene oxide carbonate) copolymer was synthesized by polycondensation between polyethylene glycol, dimethyl carbonate, and a functional diol including the pendant sulfonamide anionic group and the lithium counter‐cation. By playing with the monomer stoichiometry, the crystallinity and ionic conductivity were optimized. The best copolymer showed high ionic conductivity values of 1.2×10 −4 S cm −1 at 70 °C. Lithium interactions and mobility were studied by lithium‐pulsed field gradient, lithium diffusion, NMR relaxation time measurements, and FTIR‐ATR analysis. High lithium mobility is observed, which is due to the weakly coordinating chemical environment in the polymer and also that the sulfonamide in the SIPE adopts to a greater extent the cis conformation, which is known to promote lithium mobility. Finally, the performance of the singe‐ion conducting poly(ethylene oxide carbonate) was compared in lithium symmetric cells versus an analogous conventional salt in polymer electrolyte, showing improved performance in lithium plating and stripping.
Publisher: MDPI AG
Date: 03-11-2021
Abstract: Over 30 million ton of poly(ethylene terephthalate) (PET) is produced each year and no more than 60% of all PET bottles are reclaimed for recycling due to material property deteriorations during the mechanical recycling process. Herein, a sustainable approach is proposed to produce redox-active nanoparticles via the chemical upcycling of poly(ethylene terephthalate) (PET) waste for application in energy storage. Redox-active nanoparticles of sizes lower than 100 nm were prepared by emulsion polymerization of a methacrylic-terephthalate monomer obtained by a simple methacrylate functionalization of the depolymerization product of PET (i.e., bis-hydroxy(2-ethyl) terephthalate, BHET). The initial cyclic voltammetry results of the depolymerization product of PET used as a model compound show a reversible redox process, when using a 0.1 M tetrabutylammonium hexafluorophosphate/dimethyl sulfoxide electrolyte system, with a standard redox potential of −2.12 V vs. Fc/Fc+. Finally, the cycling performance of terephthalate nanoparticles was investigated using a 0.1 M TBAPF6 solution in acetonitrile as electrolyte in a three-electrode cell. The terephthalate anode electrode displays good cycling stability and performance at high C-rate (i.e., ≥5C), delivering a stable specific discharge capacity of 32.8 mAh.g−1 at a C-rate of 30 C, with a capacity retention of 94% after 100 cycles. However, a large hysteresis between the specific discharge and charge capacities and capacity fading are observed at lower C-rate (i.e., ≤2C), suggesting some irreversibility of redox reactions associated with the terephthalate moiety, in particular related to the oxidation process.
Publisher: American Chemical Society (ACS)
Date: 03-02-2020
Publisher: Wiley
Date: 13-12-2019
Publisher: American Chemical Society (ACS)
Date: 25-02-2019
DOI: 10.1021/ACS.ACCOUNTS.8B00566
Abstract: Electrolytes based on organic solvents used in current Li-ion batteries are not compatible with the next-generation energy storage technologies including those based on Li metal. Thus, there has been an increase in research activities investigating solid-state electrolytes, ionic liquids (ILs), polymers, and combinations of these. This Account will discuss some of the work from our teams in these areas. Similarly, other metal-based technologies including Na, Mg, Zn, and Al, for ex le, are being considered as alternatives to Li-based energy storage. However, the materials research required to effectively enable these alkali metal based energy storage applications is still in its relative infancy. Once again, electrolytes play a significant role in enabling these devices, and research has for the most part progressed along similar lines to that in advanced lithium technologies. Some of our recent contributions in these areas will also be discussed, along with our perspective on future directions in this field. For ex le, one approach has been to develop single-ion conductors, where the anion is tethered to the polymer backbone, and the dominant charge conductor is the lithium or sodium countercation. Typically, these present with low conductivity, whereas by using a copolymer approach or incorporating bulky quaternary ammonium co-cations, the effective charge separation is increased thus leading to higher conductivities and greater mobility of the alkali metal cation. This has been demonstrated both experimentally and via computer simulations. Further enhancements in ion transport may be possible in the future by designing and tethering more weakly associating anions to the polymer backbone. The second approach considers ion gels or composite polymer electrolytes where a polymerized ionic liquid is the matrix that provides both mechanical robustness and ion conducting pathways. The block copolymer approach is also demonstrated, in this case, to simultaneously provide mechanical properties and high ionic conductivity when used in combination with ionic-liquid electrolytes. The ultimate electrolyte material that will enable all high-performance solid-state batteries will have ion transport decoupled from the mechanical properties. While inorganic conductors can achieve this, their rigid, brittle nature creates difficulties. On the other hand, ionic polymers and their composites provide a rich area of chemistry to design and tune high ionic conductivity together with ideal mechanical properties.
Location: Australia
Start Date: 2021
End Date: 2023
Funder: European Commission
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