Designer Self-Assembled Polyelectrolyte Complex Nanoparticle Membrane for a Stable Lithium–Sulfur Battery at Lean Electrolyte Conditions

Jovanović, Petar; Shaibani, Mahdokht; Mirshekarloo, Meysam Sharifzadeh; Huang, Yingyi; Konstas, Kristina; Shehzad, Areeb; Hill, Matthew R.; Majumder, Mainak

doi:10.1021/acsaem.0c01307

Cited by 17 publications

(14 citation statements)

References 72 publications

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“…To this end, Majumder and co‐workers recently designed a separator that requires a minimal electrolyte amount of 4.5 µL mg −1 . [ 218 ] By taking advantage of the self‐assembly chemistry of polyelectrolyte complexation, they synthesized a polyelectrolyte complex nanoparticle on the Celgard separator simply via the dip‐coating process due to the amphiphilicity of the nanoparticles. Owing to the tunable pore size of 1.5–2.0 nm, abundant functional groups, the polyelectrolyte complex nanoparticle modified separator can efficiently adsorb LiPSs and suppress the shuttle effect.…”

Section: Separator Modification and Interlayer Engineeringmentioning

confidence: 99%

Advances in Lithium–Sulfur Batteries: From Academic Research to Commercial Viability

et al. 2021

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to sustain a continuous power supply for our daily life. [2] This is where rechargeable batteries can play a vital role in electrochemically storing and releasing the energy reversibly. [3] Additionally, as the majority of fossil fuel consumption is used for transportation, a shift from combustion engines to electric vehicles is essential in the 21st century. However, lithium-ion batteries, which have dominated the portable electronics over the past three decades, are unable to satisfy the high-energy requirement for electrical vehicles and next-generation energy storage. [2a,4] This is because the conventional lithium-ion batteries rely on the intercalation-type electrode materials and the lithium ions can only be intercalated topologically into certain specific sites, which limits their charge-storage capacity and energy density. [5] Therefore, exploring new battery chemistries beyond the horizon of current lithium-ion batteries is crucial for a sustainable future. [6] To realize a high energy density with new battery chemistries, seeking new types of electrode materials is a prerequisite. [7] Lithium metal, which has the highest theoretical specific capacity of 3860 mA h g −1 among the anode materials and the lowest electrochemical potential of −3.04 V versus the standard hydrogen electrode, is regarded as the "Holy Grail" anode material for next-generation batteries. [8] Sulfur, which is abundant, cheap, and environmentally benign, can offer a high theoretical specific capacity of 1675 mA h g −1 when paired with lithium metal, which is among the highest in solid cathode materials. [9] This is because the sulfur cathode undergoes a conversion reaction mechanism rather than the intercalation chemistry. Together with an average cell voltage of 2.15 V, the coupled lithium-sulfur (Li-S) battery can attain a high theoretical energy density of 2500 W h kg −1 , which is much higher than that of current lithium-ion batteries. [10] The earliest Li-S battery can be traced back to 1962 when Herbert and Ulam first introduced the concept of sulfur cathode (Figure 1). [11] Despite decades of research, the Li-S batteries had been long plagued with low discharge capacity and fast capacity decay upon cycling. Additionally, with the commercialization of lithium-ion batteries by Sony Co. in the 1990s, which have much more stable cycling performance and better safety, the research into Li-S batteries had once ceased for a period. [43] After 2000, as the rapid development of emerging applications such as electric vehicles and grid energy storage placed higher demands on the specific energy Lithium-ion batteries, which have revolutionized portable electronics over the past three decades, were eventually recognized with the 2019 Nobel Prize in chemistry. As the energy density of current lithium-ion batteries is approaching its limit, developing new battery technologies beyond lithiumion chemistry is significant for next-generation high energy storage. Lithiumsulfur (Li-S) batteries, which rely on the reversible redox reactions ...

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Section: Separator Modification and Interlayer Engineeringmentioning

confidence: 99%

Advances in Lithium–Sulfur Batteries: From Academic Research to Commercial Viability

et al. 2021

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“…[94] In our recent work, a capacity of 482 mg LiPS g −1 was achieved for a polyelectrolyte-nanoparticle complex. [6] This is why certain materials, as attractive as the calculated binding energies and mechanisms might be, and even if morphological considerations are overcome, struggle to find success in practical Li-S cells. In simple terms, the low adsorption capacity means that an excessively large amount of the material is required.…”

Section: Batch Equilibrium Adsorptionmentioning

confidence: 99%

Section: Standardization Of the Cycling Tests And Performance Reportingmentioning

confidence: 99%

Section: Batch Equilibrium Adsorptionmentioning

confidence: 99%

“…[99,100] For instance, the CO bond was found to shift >25 cm −1 for a polyelectrolyte-nanoparticle complex after adsorbing Li 2 S 6 , which may imply chemisorption, while other functional groups such as OH and NH 2 groups, which displayed smaller wavelength shifts, most likely participated in physisorption. [6] XPS can be used in a similar fashion. A biopolymer, carrageenan, was found to interact with LiPS, through its OSO 3 − functionality, by chemisorption through the formation of new SS and CS bonds.…”

Section: Interaction Mechanismsmentioning

confidence: 99%

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Separator Design Variables and Recommended Characterization Methods for Viable Lithium–Sulfur Batteries

Jovanović

Mirshekarloo

Hill

et al. 2021

Adv Materials Technologies

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technologies that can outperform Li-ion in at least one index of performance. The lithium-sulfur battery (Li-S) is at the forefront of competing battery technologies that on account of being potentially lighter weight, could find immediate use in emerging applications in aviation, provided that solutions to the low cycle-life and poor power delivery can be devised.Extensive research over the past ten years has yielded marked improvements in our control over this complex battery chemistry, as well as a profound understanding of its failure mechanisms, to the extent that commercialization is now much closer to reality.The fact that the Li-S battery could be commercially realized is now pushing the scientific community to devise more practical approaches for implementing what is proving to be a far-from-straightforward technology. The latter feature is no more apparent than in the development of the sulfur cathode, where the competing themes of high sulfur loading, high rate performance, and the irreversible loss of sulfur's reduction products from the cathode have driven much of the research effort to date. Until recently, then, the cathode literature has been dominated by approaches that, while undoubtedly scientifically clever, also involve exotic materials and/or synthetic pathways, thereby rendering the results industrially impractical. Now, in a series of different perspectives, Kaskel and co-workers, [1] Manthiram and co-workers, [2] and Zhang and coworkers [3] have shown the academic community that if they want to be part of the development process of this revolutionary technology, rapid transfer of lab-scale concepts on the prototype cell level is essential. Manthiram and co-workers have simplified the targets of a practical prototype pouch cell and expressed them as the "five 5 s:" sulfur loading >5 mg cm −2 ; carbon content <5%; E/S ratio <5 mL mg −1 ; E/C ratio <5 mL (mA h) −1 ; and negative/ positive (N/P) ratio <5. The successful implementation of all these considerations should, according to Manthiram and co-workers, dramatically transform how lithium-sulfur battery technology is viewed, bridging the gap between academia and industry. [2] Here, however, it seems that feasibility meets the underlying complexity of the Li-S system-often an attempt to fix a deficit in one aspect sees a compromise arising in another. Clearly then, it seemsThe lithium-sulfur (Li-S) battery is at the forefront of technologies that can outperform lithium-ion in at least one index of performance, provided that solutions to poor cycle-life can be devised. One key component of the Li-S battery is the separator, because it holds tremendous promise for improving cycle-life by mitigating the well-known polysulfide shuttle, enabling lean electrolyte configurations, and restricting solid electrolyte interphase growth at the Li-metal anode. However, in response to the advent of the "functional separator" for Li-S batteries, severe misinterpretations of progress have been made due to the often incomplete presentation of the performanc...

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Single‐Ion‐Functionalized Nanocellulose Membranes Enable Lean‐Electrolyte and Deeply Cycled Aqueous Zinc‐Metal Batteries

Zhang

Song

et al. 2022

Adv Funct Materials

102

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Aqueous cells with zinc-metal anodes featuring safety and low cost, are beneficial for diversifying energy-storage technologies, while their energy density and cyclability have been long limited by side-reactions and dendrite issues, especially at the practical device level. Though sustained efforts are underway to renovate electrodes and electrolytes, the roles of other indispensable components, such as separators, in the cell operation have been not fully unexplored thus far. Here, it is demonstrated that both the reversibility and utilization of aqueous zinc anodes can be improved by using a single-ion Zn 2+ -conducting nanocellulose membrane as the separator. Even without any treatments to the electrodes and thereof interfaces, this functional membrane marked by synergetic optimization on key required properties regarding mechanical strength, preferred Zn 2+ conduction and hydrophilicity, mitigates H 2 evolution, corrosion, and dendrite growth on zinc anodes, thus enabling >80% depth-of-discharge stable cycling under practically feasible lean electrolyte (electrolyte-to-capacity ratio = 1.0 g Ah −1 ) and high areal capacity (8.0 mAh cm −2 ) conditions. These findings translate to an excellent capacity retention of exceeding 95% after 150 cycles for full cells with practically highloading cathodes (17 mg cm −2 ). This work provides a simple yet practical avenue to high-energy, long-cycling aqueous zinc-metal batteries.

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Designer Self-Assembled Polyelectrolyte Complex Nanoparticle Membrane for a Stable Lithium–Sulfur Battery at Lean Electrolyte Conditions

Cited by 17 publications

References 72 publications

Advances in Lithium–Sulfur Batteries: From Academic Research to Commercial Viability

Advances in Lithium–Sulfur Batteries: From Academic Research to Commercial Viability

Separator Design Variables and Recommended Characterization Methods for Viable Lithium–Sulfur Batteries

Single‐Ion‐Functionalized Nanocellulose Membranes Enable Lean‐Electrolyte and Deeply Cycled Aqueous Zinc‐Metal Batteries

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