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Emerging Nanomaterials for Lithium-Sulfur Batteries and Beyond

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A special issue of Nanomaterials (ISSN 2079-4991). This special issue belongs to the section "Energy and Catalysis".

Deadline for manuscript submissions: closed (30 April 2021) | Viewed by 38900

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Prof. Dr. Young-Si Jun

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School of Chemical Engineering, Chonnam National University, Gwangju, Korea
Interests: energy storage; lithium ion batteries; photochemistry; nanomaterials; materials; graphene; nanoparticles; carbon; functionalization; nanotubes
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Dear Colleagues,

Growing demands on electricity storage have triggered tremendous research efforts on rechargeable batteries. As a primary power source, batteries would supply power to emerging energy storage systems, electric vehicles, and portable electronics. Among various battery technologies, lithium-sulfur batteries (LSBs) are at the forefront of meeting the tough requirements. LSBs, consisting of a metallic lithium anode and a chemically active sulfur cathode, have a high theoretical energy density of ~2600 Wh/kg. Moreover, the sulfur active material is environmentally benign, earth-abundant, and cheap ($0.02/g).

The practical application of LSBs is hampered by the intrinsic insulating property of active materials and the shuttle effect of soluble intermediates. In order to circumvent these technical challenges, innovative strategies have been employed over the last decades in almost all aspects of battery development, such as electrode, binder, separator, electrolyte, and cell configuration, where the materials in the nanometer-scale play vital roles in improving the electrochemical performance of LSBs by virtue of unique electronic, thermal, and mechanical properties. Such strategies significantly improve the utilization of sulfur and the cycle stability of LSBs, but only under certain conditions, for example, the areal sulfur loading is as low as ~2 mg sulfur/cm² electrode, which makes a significant gap between the laboratory scale cell tests and the practical ones.

The chronic problems of LSBs deepen further under the high sulfur loading condition (>6 mg sulfur/cm²), which is a crucial factor in order to compete with the current state-of-the-art Li-ion batteries. It is rather unclear how the high sulfur loading conditions affect the fundamental behaviors of the materials at a nanometer-scale in LSBs, thus a more detailed insight is highly demanded. The present Special Issue will thus focus on the most recent advances in the development of materials at a nanometer-scale for LSBs, under high loading conditions. I warmly invite scholars to submit original research articles, letters, and critical reviews on a novel nanomaterial-based electrodes, binders, separators, electrolytes, and cell configuration, which enable the high-performance LSBs under high loading conditions.

Prof. Dr. Young-Si Jun
Guest Editor

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Keywords

Lithium-sulfur batteries
Nanostructure
Electrode
Separator
Electrolyte
Li-metal electrode
High sulfur loading
Cell configuration
Solid or polymer electrolyte
Manufacturing
Flexible

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Research

11 pages, 2842 KiB

Open AccessFeature PaperArticle

Hierarchical Porous, N-Containing Carbon Supports for High Loading Sulfur Cathodes

by Jae-Woo Park, Hyun Jin Hwang, Hui-Ju Kang, Gazi A. K. M. Rafiqul Bari, Tae-Gyu Lee, Byeong-Hyeon An, Sung Yong Cho and Young-Si Jun

Nanomaterials 2021, 11(2), 408; https://doi.org/10.3390/nano11020408 - 5 Feb 2021

Cited by 7 | Viewed by 2694

Abstract

The lithium-polysulfide (LiPS) dissolution from the cathode to the organic electrolyte is the main challenge for high-energy-density lithium-sulfur batteries (LSBs). Herein, we present a multi-functional porous carbon, melamine cyanurate (MCA)-glucose-derived carbon (MGC), with superior porosity, electrical conductivity, and polysulfide affinity as an efficient sulfur support to mitigate the shuttle effect. MGC is prepared via a reactive templating approach, wherein the organic MCA crystals are utilized as the pore-/micro-structure-directing agent and nitrogen source. The homogeneous coating of spherical MCA crystal particles with glucose followed by carbonization at 600 °C leads to the formation of hierarchical porous hollow carbon spheres with abundant pyridinic N-functional groups without losing their microstructural ordering. Moreover, MGC enables facile penetration and intensive anchoring of LiPS, especially under high loading sulfur conditions. Consequently, the MGC cathode exhibited a high areal capacity of 5.79 mAh cm⁻² at 1 mA cm⁻² and high loading sulfur of 6.0 mg cm⁻² with a minor capacity decay rate of 0.18% per cycle for 100 cycles. Full article

(This article belongs to the Special Issue Emerging Nanomaterials for Lithium-Sulfur Batteries and Beyond)

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12 pages, 2698 KiB

Open AccessArticle

Microalgae-Templated Spray Drying for Hierarchical and Porous Fe₃O₄/C Composite Microspheres as Li-ion Battery Anode Materials

by Jinseok Park, Jungmin Kim, Dae Soo Jung, Isheunesu Phiri, Hyeon-Su Bae, Jinseok Hong, Sojin Kim, Young-Gi Lee, Myung-Hyun Ryou and Kyubock Lee

Nanomaterials 2020, 10(10), 2074; https://doi.org/10.3390/nano10102074 - 20 Oct 2020

Cited by 9 | Viewed by 3464

Abstract

A method of microalgae-templated spray drying to develop hierarchical porous Fe₃O₄/C composite microspheres as anode materials for Li-ion batteries was developed. During the spray-drying process, individual microalgae serve as building blocks of raspberry-like hollow microspheres via self-assembly. In the present study, microalgae-derived carbon matrices, naturally doped heteroatoms, and hierarchical porous structural features synergistically contributed to the high electrochemical performance of the Fe₃O₄/C composite microspheres, enabling a discharge capacity of 1375 mA·h·g⁻¹ after 700 cycles at a current density of 1 A/g. Notably, the microalgal frameworks of the Fe₃O₄/C composite microspheres were maintained over the course of charge/discharge cycling, thus demonstrating the structural stability of the composite microspheres against pulverization. In contrast, the sample fabricated without microalgal templating showed significant capacity drops (up to ~40% of initial capacity) during the early cycles. Clearly, templating of microalgae endows anode materials with superior cycling stability. Full article

(This article belongs to the Special Issue Emerging Nanomaterials for Lithium-Sulfur Batteries and Beyond)

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16 pages, 4505 KiB

Open AccessArticle

Microporous Carbon Nanoparticles for Lithium–Sulfur Batteries

by Hui-Ju Kang, Gazi A. K. M. Rafiqul Bari, Tae-Gyu Lee, Tamal Tahsin Khan, Jae-Woo Park, Hyun Jin Hwang, Sung Yong Cho and Young-Si Jun

Nanomaterials 2020, 10(10), 2012; https://doi.org/10.3390/nano10102012 - 12 Oct 2020

Cited by 20 | Viewed by 3708

Abstract

Rechargeable lithium–sulfur batteries (LSBs) are emerging as some of the most promising next-generation battery alternatives to state-of-the-art lithium-ion batteries (LIBs) due to their high gravimetric energy density, being inexpensive, and having an abundance of elemental sulfur (S₈). However, one main, well-known drawback of LSBs is the so-called polysulfide shuttling, where the polysulfide dissolves into organic electrolytes from sulfur host materials. Numerous studies have shown the ability of porous carbon as a sulfur host material. Porous carbon can significantly impede polysulfide shuttling and mitigate the insulating passivation layers, such as Li₂S, owing to its intrinsic high electrical conductivity. This work suggests a scalable and straightforward one-step synthesis method to prepare a unique interconnected microporous and mesoporous carbon framework via salt templating with a eutectic mixture of LiI and KI at 800 °C in an inert atmosphere. The synthesis step used environmentally friendly water as a washing solvent to remove salt from the carbon–salt mixture. When employed as a sulfur host material, the electrode exhibited an excellent capacity of 780 mAh g⁻¹ at 500 mA g⁻¹ and a sulfur loading mass of 2 mg cm⁻² with a minor capacity loss of 0.36% per cycle for 100 cycles. This synthesis method of a unique porous carbon structure could provide a new avenue for the development of an electrode with a high retention capacity and high accommodated sulfur for electrochemical energy storage applications. Full article

(This article belongs to the Special Issue Emerging Nanomaterials for Lithium-Sulfur Batteries and Beyond)

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17 pages, 3418 KiB

Open AccessArticle

Highly Stable Porous Polyimide Sponge as a Separator for Lithium-Metal Secondary Batteries

by Junyoung Choi, Kwansoo Yang, Hyeon-Su Bae, Isheunesu Phiri, Hyun Jeong Ahn, Jong Chan Won, Yong Min Lee, Yun Ho Kim and Myung-Hyun Ryou

Nanomaterials 2020, 10(10), 1976; https://doi.org/10.3390/nano10101976 - 6 Oct 2020

Cited by 7 | Viewed by 4527

Abstract

To inhibit Li-dendrite growth on lithium (Li)-metal electrodes, which causes capacity deterioration and safety issues in Li-ion batteries, we prepared a porous polyimide (PI) sponge using a solution-processable high internal-phase emulsion technique with a water-soluble PI precursor solution; the process is not only simple but also environmentally friendly. The prepared PI sponge was processed into porous PI separators and used for Li-metal electrodes. The physical properties (e.g., thermal stability, liquid electrolyte uptake, and ionic conductivity) of the porous PI separators and their effect on the Li-metal anodes (e.g., self-discharge and open-circuit voltage properties after storage, cycle performance, rate capability, and morphological changes) were investigated. Owing to the thermally stable properties of the PI polymer, the porous PI separators demonstrated no dimensional changes up to 180 °C. In comparison with commercialized polyethylene (PE) separators, the porous PI separators exhibited improved wetting ability for liquid electrolytes; thus, the latter improved not only the physical properties (e.g., improved the electrolyte uptake and ionic conductivity) but also the electrochemical properties of Li-metal electrodes (e.g., maintained stable self-discharge capacity and open-circuit voltage features after storage and improved the cycle performance and rate capability) in comparison with PE separators. Full article

(This article belongs to the Special Issue Emerging Nanomaterials for Lithium-Sulfur Batteries and Beyond)

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11 pages, 3090 KiB

Open AccessArticle

Cinnamon-Derived Hierarchically Porous Carbon as an Effective Lithium Polysulfide Reservoir in Lithium–Sulfur Batteries

by Ranjith Thangavel, Aravindaraj G. Kannan, Rubha Ponraj, Karthikeyan Kaliyappan, Won-Sub Yoon, Dong-Won Kim and Yun-Sung Lee

Nanomaterials 2020, 10(6), 1220; https://doi.org/10.3390/nano10061220 - 22 Jun 2020

Cited by 22 | Viewed by 3546

Abstract

Lithium–sulfur batteries are attractive candidates for next generation high energy applications, but more research works are needed to overcome their current challenges, namely: (a) the poor electronic conductivity of sulfur, and (b) the dissolution and migration of long-chain polysulfides. Inspired by eco-friendly and bio-derived materials, we synthesized highly porous carbon from cinnamon sticks. The bio-carbon had an ultra-high surface area and large pore volume, which serves the dual functions of making sulfur particles highly conductive and acting as a polysulfide reservoir. Sulfur was predominantly impregnated into pores of the carbon, and the inter-connected hierarchical pore structure facilitated a faster ionic transport. The strong carbon framework maintained structural integrity upon volume expansion, and the unoccupied pores served as polysulfide trapping sites, thereby retaining the polysulfide within the cathode and preventing sulfur loss. These mechanisms contributed to the superior performance of the lithium-sulfur cell, which delivered a discharge capacity of 1020 mAh g⁻¹ at a 0.2C rate. Furthermore, the cell exhibited improved kinetics, with an excellent cycling stability for 150 cycles with a very low capacity decay of 0.10% per cycle. This strategy of combining all types of pores (micro, meso and macro) with a high pore volume and ultra-high surface area had a synergistic effect on improving the performance of the sulfur cathode. Full article

(This article belongs to the Special Issue Emerging Nanomaterials for Lithium-Sulfur Batteries and Beyond)

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22 pages, 5368 KiB

Open AccessArticle

Electrolyte-Dependent Supercapacitor Performance on Nitrogen-Doped Porous Bio-Carbon from Gelatin

by Jie Deng, Jing Li, Shuang Song, Yanping Zhou and Luming Li

Nanomaterials 2020, 10(2), 353; https://doi.org/10.3390/nano10020353 - 18 Feb 2020

Cited by 36 | Viewed by 4008

Abstract

The carbon supercapacitance strongly relies upon the electrolyte’s nature, but the clear-cut structure–performance nexus remains elusive. Herein, a series of bio-carbons with gradually varied pore structure and surface chemistry are derived using a new salt template protocol (with eco-benign KNO₃ as the template, activator, and porogen, and cheap gelatin as the carbon precursor), and are used as model systems to probe the dependence of the electrochemical mechanism of such nanocarbons on two typical electrolytes (KOH and EMIBF₄). By only adjusting the KNO₃ dosage, two pivotal figures of merit of biochar—multiscale porosity and surface functionalization—were finely modulated to construct electric double layers. Electrochemical data clarify that the combined porosity and doping effects all contribute to enhanced supercapacitance, but with only one of the two factors playing the leading role in different electrolytes. Kinetic analysis corroborates the fact that ample heteroatom doping can effectively compensate capacitance by intensive surface redox insertion in KOH, while a suitable pore size dispersion plays a preponderant part in self-amplifying the ion partitioning, and thus dictating a good charge separation in EMIBF₄. A quasi-quantitative model of performance–structure relevance in EMIBF₄ is judiciously conjectured to hint at a superb ion–pore-size compatibility, in which the bi- and mono-layer ion confinement coupling in integrated single and double ion-sized pores is found to be more useful for curbing notorious over-screening effects and for changing the coordination number, Coulombic ordering, and phase conformation of EMIBF₄ in several nm-sized nanopores. This unique energy storage fashion in ion-matching pores promotes the energy density of optimal samples to a novel level of 88.3 Wh kg⁻¹ at 1 kW kg⁻¹, which rivals the overwhelming majority of the reported carbon materials. In short, the comparison case study here reveals a valuable correlation of carbon’s figure of merit and electrolyte type, which may act as a vital rudder to design electrolyte-contingent state-of-the-art supercapacitor materials. Full article

(This article belongs to the Special Issue Emerging Nanomaterials for Lithium-Sulfur Batteries and Beyond)

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19 pages, 4577 KiB

Open AccessArticle

Bulk-Like SnO₂-Fe₂O₃@Carbon Composite as a High-Performance Anode for Lithium Ion Batteries

by Jie Deng, Yu Dai, Zhe Xiao, Shuang Song, Hui Dai, Luming Li and Jing Li

Nanomaterials 2020, 10(2), 249; https://doi.org/10.3390/nano10020249 - 30 Jan 2020

Cited by 8 | Viewed by 3483

Abstract

Boosted power handling and the reduced charging duration of Li ion cells critically rests with ionic/electronic mobility. Ion mobility in electrochemically relevant grains normally stands for an essential restriction of the velocity at which the energy of a cell can be stored/released. To offset sluggish solid-state ionic transport and achieve a superior power/energy density rating, electroactive grains often need exquisite nanoscaling, harming crucial virtues on volumetric packing density, tractability, sustainability, durability, and cost. Unlike elaborate nanostructuring, here we describe that a SnO₂-Fe₂O₃@carbon composite—which adopts a metal oxide particles-intercalated bulk-like configuration—can insert many Li⁺ ions at elevated speeds, despite its micro-dimensionality. Analysis of charge transport kinetics in this tailor-made architecture unveils both much improved ion travel through compact monolithic substances and the greatly enhanced ion access to surfaces of SnO₂/Fe₂O₃ grains. According to the well-studied battery degradation mechanism, it is that both the effective stress management and internal electric field in our as-prepared sample that result in recommendable capacity, rate behavior, and cyclic lifespan (exhibiting a high reversible capacity of 927 mAh g⁻¹ at 0.2 A g⁻¹ with a capacity retention of 95.1% after 100 cycles and an ultra-stable capacity of 429 mAh g⁻¹ even over 1800 cycles at 3 A g⁻¹). Unique materials and working rationale which ensure the swift (de)lithiation of such micrometer-dimensional monoliths may open a door for various high-power/density usages. Full article

(This article belongs to the Special Issue Emerging Nanomaterials for Lithium-Sulfur Batteries and Beyond)

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13 pages, 5246 KiB

Open AccessArticle

Lotus Root-Like Nitrogen-Doped Carbon Nanofiber Structure Assembled with VN Catalysts as a Multifunctional Host for Superior Lithium–Sulfur Batteries

by Benben Wei, Chaoqun Shang, Xiaoying Pan, Zhihong Chen, Lingling Shui, Xin Wang and Guofu Zhou

Nanomaterials 2019, 9(12), 1724; https://doi.org/10.3390/nano9121724 - 3 Dec 2019

Cited by 19 | Viewed by 4247

Abstract

Lithium–sulfur batteries (LSBs) are regarded as one of the most promising energy-recycling storage systems due to their high energy density (up to 2600 Wh kg⁻¹), high theoretical specific capacity (as much as 1672 mAh g⁻¹), environmental friendliness, and low cost. Originating from the complicated redox of lithium polysulfide intermediates, Li–S batteries suffer from several problems, restricting their application and commercialization. Such problems include the shuttle effect of polysulfides (Li₂S_x (2 < x ≤ 8)), low electronic conductivity of S/Li₂S/Li₂S₂, and large volumetric expansion of S upon lithiation. In this study, a lotus root-like nitrogen-doped carbon nanofiber (NCNF) structure, assembled with vanadium nitride (VN) catalysts, was fabricated as a 3D freestanding current collector for high performance LSBs. The lotus root-like NCNF structure, which had a multichannel porous nanostructure, was able to provide excellent (ionically/electronically) conductive networks, which promoted ion transport and physical confinement of lithium polysulfides. Further, the structure provided good electrolyte penetration, thereby enhancing the interface contact with active S. VN, with its narrow resolved band gap, showed high electrical conductivity, high catalytic effect and polar chemical adsorption of lithium polysulfides, which is ideal for accelerating the reversible redox kinetics of intermediate polysulfides to improve the utilization of S. Tests showed that the VN-decorated multichannel porous carbon nanofiber structure retained a high specific capacity of 1325 mAh g⁻¹ after 100 cycles at 0.1 C, with a low capacity decay of 0.05% per cycle, and demonstrated excellent rate capability. Full article

(This article belongs to the Special Issue Emerging Nanomaterials for Lithium-Sulfur Batteries and Beyond)

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22 pages, 3724 KiB

Open AccessArticle

Studies on Possible Ion-Confinement in Nanopore for Enhanced Supercapacitor Performance in 4V EMIBF₄ Ionic Liquids

by Jie Deng, Jing Li, Zhe Xiao, Shuang Song and Luming Li

Nanomaterials 2019, 9(12), 1664; https://doi.org/10.3390/nano9121664 - 22 Nov 2019

Cited by 15 | Viewed by 4176

Abstract

Supercapacitors have the rapid charge/discharge kinetics and long stability in comparison with various batteries yet undergo low energy density. Theoretically, square dependence of energy density upon voltage reveals a fruitful but challenging engineering tenet to address this long-standing problem by keeping a large voltage window in the compositionally/structurally fine-tuned electrode/electrolyte systems. Inspired by this, a facile salt-templating enables hierarchically porous biochars for supercapacitors filled by the high-voltage ionic liquids (ILs). Resultant nanostructures possess a coherent/interpenetrated framework of curved atom-thick sidewalls of 0.8-/1.5-nanometer pores to reconcile the pore-size-dependent adlayer structures of ILs in nanopores. Surprisingly, this narrow dual-model pore matches ionic radii of selected ILs to accommodate ions by unique coupled nano-/bi-layer nanoconfinements, augmenting the degree of confinement (DoC). The high DoC efficiently undermines the coulombic ordering networks and induces the local conformational oscillations, thus triggering an anomalous but robust charge separation. This novel bi-/mono-layer nanoconfinement combination mediates harmful overscreening/overcrowding effects to reinforce ion-partitioning, mitigating long-lasting conflicts of power/energy densities. This interesting result differs from a long-held viewpoint regarding the sieving effect that ion-in-pore capacitance peaks only if pore size critically approaches the ion dimension. Optimal biocarbon finally presents a very high/stable operational voltage up to 4 V and specific energy/power rating (88.3 Wh kg⁻¹ at 1 kW kg⁻¹, 47.7 Wh kg⁻¹ albeit at a high battery-accessible specific power density of 20 kW kg⁻¹), overwhelmingly outperforming most hitherto-reported supercapacitors and some batteries. Such attractive charge storage level can preliminarily elucidate an alternative form of a super-ionic-state high-energy storage linked with both the coordination number and coulombic periodism of the few ion-sized mesopores inside carbon electrodes, escalating supercapacitors into a novel criterion of charge delivery. Full article

(This article belongs to the Special Issue Emerging Nanomaterials for Lithium-Sulfur Batteries and Beyond)

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14 pages, 3579 KiB

Open AccessFeature PaperArticle

Polyimide-Coated Glass Microfiber as Polysulfide Perm-Selective Separator for High-Performance Lithium-Sulphur Batteries

by Mi-Jin Kim, Kwansoo Yang, Hui-Ju Kang, Hyun Jin Hwang, Jong Chan Won, Yun Ho Kim and Young-Si Jun

Nanomaterials 2019, 9(11), 1612; https://doi.org/10.3390/nano9111612 - 13 Nov 2019

Cited by 7 | Viewed by 3898

Abstract

Although numerous research efforts have been made for the last two decades, the chronic problems of lithium-sulphur batteries (LSBs), i.e., polysulfide shuttling of active sulphur material and surface passivation of the lithium metal anode, still impede their practical application. In order to mitigate these issues, we utilized polyimide functionalized glass microfibers (PI-GF) as a functional separator. The water-soluble precursor enabled the formation of a homogenous thin coating on the surface of the glass microfiber (GF) membrane with the potential to scale and fine-tune: the PI-GF was prepared by simple dipping of commercial GF into an aqueous solution of poly(amic acid), (PAA), followed by thermal imidization. We found that a tiny amount of polyimide (PI) of 0.5 wt.% is more than enough to endow the GF separator with useful capabilities, both retarding polysulfide migration. Combined with a free-standing microporous carbon cloth-sulphur composite cathode, the PI-GF-based LSB cell exhibits a stable cycling over 120 cycles at a current density of 1 mA/cm² and an areal sulphur loading of 2 mgS/cm² with only a marginal capacity loss of 0.099%/cycle. This corresponds to an improvement in cycle stability by 200%, specific capacity by 16.4%, and capacity loss per cycle by 45% as compared to those of the cell without PI coating. Our study revealed that a simple but synergistic combination of porous carbon supporting material and functional separator enabled us to achieve high-performance LSBs, but could also pave the way for the development of practical LSBs using the commercially viable method without using complicated synthesis or harmful and expensive chemicals. Full article

(This article belongs to the Special Issue Emerging Nanomaterials for Lithium-Sulfur Batteries and Beyond)

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