Graphene-like g-C3N4 nanosheets/sulfur as cathode for lithium–sulfur battery

Meng, Zhen; Xie, Yang; Cai, Tingwei; Sun, Zixu; Jiang, Kui; Han, Wei‐Qiang

doi:10.1016/j.electacta.2016.06.032

Cited by 80 publications

(43 citation statements)

References 64 publications

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“…[1][2][3][4] Among them, carbon-based 2D materials have always been the research focus. [9] It has attracted a lot of attention and has been demonstrated to be well suited for photosynthesis, [10] lithiumsulfur batteries, [11] and other applications. [5][6][7] C 3 N 4 , a classic nanoporous graphitic carbon nitride which could be easily synthesized from urea, [8] possesses excellent physical and chemical stability and appealing electronic properties with a band gap of 2.70 eV.…”

Section: Introductionmentioning

confidence: 99%

2D Nitrogen‐Containing Carbon Material C₅N as Potential Host Material for Lithium Polysulfides: A First‐Principles Study

Wang

Zhang

et al. 2018

Advcd Theory and Sims

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Two-dimensional (2D) materials are identified to be efficient in many applications. In this work, a novel 2D nitrogen-containing carbon material, C 5 N, is theoretically designed through structure changes in atomic scale, that is, introducing V C -V N bivacancy defects along lines in perfect C 3 N monolayer. C 5 N monolayer is verified to be chemically, mechanically, dynamically, and thermodynamically stable based on cohesive energy, elastic constants, phonon spectrum, and molecular dynamics calculations. C 5 N is determined to be metallic which is an important property for battery electrode. Moreover, the anchoring performance of S 8 and Li 2 S n (n = 1, 2, 4, 6, and 8) on C 5 N monolayer and the anchoring mechanisms are explored. The adsorption energies are calculated to be −0.

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Section: Introductionmentioning

confidence: 99%

2D Nitrogen‐Containing Carbon Material C₅N as Potential Host Material for Lithium Polysulfides: A First‐Principles Study

Wang

Zhang

et al. 2018

Advcd Theory and Sims

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“…[15,16] However, the non-polar nature of carbon surfaces limits the ability of LiPS to adsorb and to remain spatially localized. Recent studies have involved the use of sulfiphillic frameworks such as metal oxides, [17] MXene, [20] and C 3 N 4 , [21] where LiPSs are chemically bound to the positive electrode. Recent studies have involved the use of sulfiphillic frameworks such as metal oxides, [17] MXene, [20] and C 3 N 4 , [21] where LiPSs are chemically bound to the positive electrode.…”

Section: Introductionmentioning

confidence: 99%

Polysulfide Binding to Several Nanoscale Magnéli Phases Synthesized in Carbon for Long‐Life Lithium–Sulfur Battery Cathodes

et al. 2018

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In Li-S batteries, it is important to ensure efficient reversible conversion of sulfur to lithium polysulfide (LiPS). Shuttling effects caused by LiPS dissolution can lead to reduced performance and cycle life. Although carbon materials rely on physical trapping of polysulfides, polar oxide surfaces can chemically bind LiPS to improve the stability of sulfur cathodes. We show a simple synthetic method that allows high sulfur loading into mesoporous carbon preloaded with spatially localized nanoparticles of several Magnéli-phase titanium oxide (Ti O ). This material simultaneously suppresses polysulfide shuttling phenomena by chemically binding Li polysulfides onto several Magnéli-phase surfaces in a single cathode and ensures physical confinement of sulfur and LiPS. The synergy between chemical immobilization of significant quantities of LiPS at the surface of several Ti O phases and physical entrapment results in coulombically efficient high-rate cathodes with long cycle life and high capacity. These cathodes function efficiently at low electrolyte-to-sulfur ratios to provide high gravimetric and volumetric capacities in comparison with their highly porous carbon counterparts. Assembled coin cells have an initial discharge capacity of 1100 mAh g at 0.1C and maintain a reversible capacity of 520 mAh g at 0.2C for more than 500 cycles. Even at 1C, the cell loses only 0.06 % per cycle for 1000 cycles with a coulombic efficiency close to 99 %.

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“…Very recently, the use of carbon nitride-based materials as sulfur hosts has been investigated in a number of articles. Pang and Nazar employed a nanoporous graphitic C 3 N 4 (g-C 3 N 4 ) with large surface area as a sulfur host.[14] The abundant nitrogen (N) atoms on the g-C 3 N 4 form Li-N chemical interaction with lithium polysulfides, [14][15][16] which retards the diffusion of lithium polysulfides into the electrolyte effectively. However, the g-C 3 N 4 has intrinsically poor electrical conductivity, thus the adsorbed polysulfides are difficult to be reduced directly on the g-C 3 N 4 surface especially at high current density, resulting in relatively low sulfur utilization.…”

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confidence: 99%

From Silica Sphere to Hollow Carbon Nitride‐Based Sphere: Rational Design of Sulfur Host with Both Chemisorption and Physical Confinement

Meng

Ying

et al. 2017

Adv Materials Inter

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namely a high theoretical specific energy of ≈2500 W h kg −1 for Li-S battery. [1,2] What is more, sulfur is low cost, nontoxic, and natural abundant. Despite these considerable advantages, the development of sulfur cathode is still hindered by several obstacles. Foremost among these is the "shuttle effect." The lithium polysulfides with high solubility formed in both charge and discharge processes diffuse into the electrolyte and then react with lithium anodes, which causes low coulombic efficiency, rapid capacity decay, and severe self-discharge of the cells. The second is the relatively low utilization of the active materials resulting from the insulating nature of sulfur, Li 2 S 2 / Li 2 S discharge products. The third is the volumetric and structural change of sulfur during charging and discharging. [3,4] Various materials have been introduced as sulfur hosts in attempt to address the above mentioned issues, including the carbon materials, [1,[5][6][7][8][9] conductive polymers, [10,11] metal oxides, [12,13] etc. Very recently, the use of carbon nitride-based materials as sulfur hosts has been investigated in a number of articles. Pang and Nazar employed a nanoporous graphitic C 3 N 4 (g-C 3 N 4 ) with large surface area as a sulfur host.[14] The abundant nitrogen (N) atoms on the g-C 3 N 4 form Li-N chemical interaction with lithium polysulfides, [14][15][16] which retards the diffusion of lithium polysulfides into the electrolyte effectively. However, the g-C 3 N 4 has intrinsically poor electrical conductivity, thus the adsorbed polysulfides are difficult to be reduced directly on the g-C 3 N 4 surface especially at high current density, resulting in relatively low sulfur utilization. [13] Zhang and co-workers reported a simple method to synthesize graphene-like oxygenated carbon nitride material (OCN) and used it as a sulfur host. Compared with the poorly conductive g-C 3 N 4 host material, the improved capacity performance was obtained for OCN-900 composite. [17] So far, it has been proved utilization of carbon nitride-based materials as lithium polysulfides anchoring hosts is effective. Yet just as most other polar material with lithium polysulfides anchoring abilities, carbon nitride-based materials can only adsorb lithium polysulfides near their surfaces. When the surface area is too low and the sulfur content is higher than a certain value, the host materials are not able to provide sufficient interfaces to anchor all of the lithium polysulfides. [13] Therefore, rational design of the structure of carbon nitride-based materials become important.To suppress the shuttle effect and improve the sulfur utilization in lithiumsulfur battery, a novel hollow carbon nitride-based spheres material (HCN x ) has been synthesized via polymerization of ethylenediamine and carbon tetrachloride on silica spheres and used as a sulfur host. The rational designed structure of HCN x retards diffusion of lithium polysulfides by both chemisorption and physical confinement. The enhanced conductivity of HCN x improves the u...

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Graphene-like g-C3N4 nanosheets/sulfur as cathode for lithium–sulfur battery

Cited by 80 publications

References 64 publications

2D Nitrogen‐Containing Carbon Material C₅N as Potential Host Material for Lithium Polysulfides: A First‐Principles Study

2D Nitrogen‐Containing Carbon Material C₅N as Potential Host Material for Lithium Polysulfides: A First‐Principles Study

Polysulfide Binding to Several Nanoscale Magnéli Phases Synthesized in Carbon for Long‐Life Lithium–Sulfur Battery Cathodes

From Silica Sphere to Hollow Carbon Nitride‐Based Sphere: Rational Design of Sulfur Host with Both Chemisorption and Physical Confinement

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Graphene-like g-C3N4 nanosheets/sulfur as cathode for lithium–sulfur battery

Cited by 80 publications

References 64 publications

2D Nitrogen‐Containing Carbon Material C5N as Potential Host Material for Lithium Polysulfides: A First‐Principles Study

2D Nitrogen‐Containing Carbon Material C5N as Potential Host Material for Lithium Polysulfides: A First‐Principles Study

Polysulfide Binding to Several Nanoscale Magnéli Phases Synthesized in Carbon for Long‐Life Lithium–Sulfur Battery Cathodes

From Silica Sphere to Hollow Carbon Nitride‐Based Sphere: Rational Design of Sulfur Host with Both Chemisorption and Physical Confinement

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2D Nitrogen‐Containing Carbon Material C₅N as Potential Host Material for Lithium Polysulfides: A First‐Principles Study

2D Nitrogen‐Containing Carbon Material C₅N as Potential Host Material for Lithium Polysulfides: A First‐Principles Study