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The year 1975 can be claimed to be the year of inception for the research and development of solid polymer electrolytes (SPEs) for Lithium-Ion Batteries (LIB), when the ionic conductivity of polyethylene oxide–alkaline metal ion complex was found by Peter Wright from the University of Sheffield. However, SPE research has undergone a leapfrog development, with conductivity values improving from 1 × 10–7 S·cm−1 to 1 × 10– 1 S·cm−1. The seed of development of SPEs spurs from the need for introducing design freedom to battery structures as well as the need for leak-proof electrolytes, greater operational safety, higher energy density, and other considerations. While the benefits of SPEs are evident, poor interfacial contact is a major factor limiting their application. This review presents the history of SPEs and shows how the additive manufacturing (AM) could prove beneficial for the improvement of performance and the functional implementation of SPEs. While the article articulates a technical review of additively manufactured SPEs, it also provides a lab-to-market perspective that could aid in shaping the future of green technology in energy storage. It also aims to provide an overall picture about the evolution and diversity of research advances in the development of greener SPEs through AM technology.
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Morphology control in semicrystalline solid polymer electrolytes for lithium batteries
Solid polymer electrolytes (SPEs) are one of the most promising solutions to the safety issues of lithium batteries. Understanding the morphology and dynamic effects on the ion transport properties of SPEs would be essential for future SPE design. In this article, using poly(ethylene oxide) (PEO) as an example, we focus on morphology control in semicrystalline SPEs. We show that the effect of semicrystallinity can be quantitatively separated into volume, structure and dynamic effects. We further demonstrate that morphological control plays an important role in ion transport control in semicrystalline SPE systems.
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- Award ID(s):
- 1709136
- PAR ID:
- 10167116
- Date Published:
- Journal Name:
- Molecular Systems Design & Engineering
- Volume:
- 4
- Issue:
- 4
- ISSN:
- 2058-9689
- Page Range / eLocation ID:
- 793 to 803
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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Because 3D batteries comprise solid polymer electrolytes (SPE) confined to high surface area porous scaffolds, the interplay between polymer confinement and interfacial interactions on total ionic conductivity must be understood. This paper investigates contributions to the structure-conductivity relationship in poly(ethylene oxide) (PEO)–lithium bis(trifluorosulfonylimide) (LiTFSI) complexes confined to microporous nickel scaffolds. For bulk and confined conditions, PEO crystallinity decreases as the salt concentration (Li+:EO (r) = 0.0.125, 0.0167, 0.025, 0.05) increases. For pure PEO and all r values except 0.05, PEO crystallinity under confinement is lower than in the bulk, whereas glass transition temperature remains statistically invariant. At 298 K (semicrystalline), total ionic conductivity under confinement is higher than in the bulk at r = 0.0167, but remains invariant at r = 0.05; however, at 350 K (amorphous), total ionic conductivity is higher than in the bulk for both salt concentrations. Time–of–flight secondary ion mass spectrometry indicates selective migration of ions towards the polymer–scaffold interface. In summary, for the 3D structure studied, polymer crystallinity, interfacial segregation, and tortuosity play an important role in determining total ionic conductivity and, ultimately, the emergence of 3D SPEs as energy storage materials.more » « less
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Abstract This study presents a novel polymer‐in‐salt (PIS) zwitterionic polyurethane‐based solid polymer electrolyte (zPU‐SPE) that offers high ionic conductivity, strong interaction with electrodes, and excellent mechanical and electrochemical stabilities, making it promising for high‐performance all solid‐state lithium batteries (ASSLBs). The zPU‐SPE exhibits remarkable lithium‐ion (Li+) conductivity (3.7 × 10⁻⁴ S cm−1at 25 °C), enabled by exceptionally high salt loading of up to 90 wt.% (12.6 molar ratio of Li salt to polymer unit) without phase separation. It addresses the limitations of conventional SPEs by combining high ionic conductivity with a Li+transference number of 0.44, achieved through the incorporation of zwitterionic groups that enhance ion dissociation and transport. The high surface energy (338.4 J m−2) and elasticity ensure excellent adhesion to Li anodes, reducing interfacial resistance and ensuring uniform Li+flux. When tested in Li||zPU||LiFePO₄ and Li||zPU||S/C cells, the zPU‐SPE demonstrated remarkable cycling stability, retaining 76% capacity after 2000 cycles with the LiFePO4cathode, and achieving 84% capacity retention after 300 cycles with the S/C cathode. Molecular simulations and a range of experimental characterizations confirm the superior structural organization of the zPU matrix, contributing to its outstanding electrochemical performance. The findings strongly suggest that zPU‐SPE is a promising candidate for next‐generation ASSLBs.more » « less
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Abstract Strong light–matter interactions in two-dimensional layered materials (2D materials) have attracted the interest of researchers from interdisciplinary fields for more than a decade now. A unique phenomenon in some 2D materials is their large exciton binding energies (BEs), increasing the likelihood of exciton survival at room temperature. It is this large BE that mediates the intense light–matter interactions of many of the 2D materials, particularly in their monolayer limit, where the interplay of excitonic phenomena poses a wealth of opportunities for high-performance optoelectronics and quantum photonics. Within quantum photonics, quantum information science (QIS) is growing rapidly, where photons are a promising platform for information processing due to their low-noise properties, excellent modal control, and long-distance propagation. A central element for QIS applications is a single photon emitter (SPE) source, where an ideal on-demand SPE emits exactly one photon at a time into a given spatiotemporal mode. Recently, 2D materials have shown practical appeal for QIS which is directly driven from their unique layered crystalline structure. This structural attribute of 2D materials facilitates their integration with optical elements more easily than the SPEs in conventional three-dimensional solid state materials, such as diamond and SiC. In this review article, we will discuss recent advances made with 2D materials towards their use as quantum emitters, where the SPE emission properties maybe modulated deterministically. The use of unique scanning tunneling microscopy tools for thein-situgeneration and characterization of defects is presented, along with theoretical first-principles frameworks and machine learning approaches to model the structure-property relationship of exciton–defect interactions within the lattice towards SPEs. Given the rapid progress made in this area, the SPEs in 2D materials are emerging as promising sources of nonclassical light emitters, well-poised to advance quantum photonics in the future.more » « less
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Abstract This present study illustrates the synthesis and preparation of polyoxanorbornene‐based bottlebrush polymers with poly(ethylene oxide) (PEO) side chains by ring‐opening metathesis polymerization for solid polymer electrolytes (SPE). In addition to the conductive PEO side chains, the polyoxanorbornene backbones may act as another ion conductor to further promote Li‐ion movement within the SPE matrix. These results suggest that these bottlebrush polymer electrolytes provide impressively high ionic conductivity of 7.12 × 10−4S cm−1at room temperature and excellent electrochemical performance, including high‐rate capabilities and cycling stability when paired with a Li metal anode and a LiFePO4cathode. The new design paradigm, which has dual ionic conductive pathways, provides an unexplored avenue for inventing new SPEs and emphasizes the importance of molecular engineering to develop highly stable and conductive polymer electrolytes for lithium‐metal batteries (LMB).more » « less
- Free Publicly Accessible Full Text
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Accepted Manuscript1.0
- Journal Article:
- https://doi.org/10.1039/C9ME00028C
