Unconventional Carbon: Alkaline Dehalogenation of Polymers Yields N‐Doped Carbon Electrode for High‐Performance Capacitive Energy Storage

Zhang, Guoxin; Wang, Lin; Hao, Yongchao; Jin, Xiuyan; Xu, Yuqi; Kuang, Yun; Dai, Liming; Sun, Xiaoming

doi:10.1002/adfm.201505533

Cited by 101 publications

(67 citation statements)

References 46 publications

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“…The diffraction profiles of SC-BDSA exhibit two major broad peaks at ≈25.1° and 43.0°, which can be attributed to typical reflections from the (002) and (100) planes of disordered carbon materials, [34] indicating that no pronounced graphitization is occurred under the present sulfurization/carbonization process. [35] The I D /I G ratio of SC-BDSA is 0.48, lower than that of C-BDSA and C-BSA, representing the enhanced density of graphitization, [23,34] which is well consistent with the XRD analysis. The (002) and (100) peaks of C-BDSA is broader and weaker than that of SC-BDSA, especially, in C-BSA, the (100) plane even has not been observed, suggesting its more disordered structure.…”

Section: Preparation and Physical-chemistry Features Of Sulfurized-casupporting

confidence: 76%

Controllable Chain‐Length for Covalent Sulfur–Carbon Materials Enabling Stable and High‐Capacity Sodium Storage

Jing

Yang

et al. 2019

Advanced Energy Materials

159

120

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couple high-capacity sulfur positive electrodes with earth-abundant sodium negative electrodes are unsurprisingly considered as a promising candidate. [8][9][10][11] In the process of cycle, the elemental sulfur of the cathode is dissolvated, reduced to form various soluble polysulfides, that is, S x 2− ions and radicals (1 ≤ x ≤ 8), and eventually the insoluble Na 2 S 2 and Na 2 S. [8,10,12] However, the practical applications are seriously hindered by several obstacles, in which the fundamental challenges are originated from the insulating properties of elemental sulfur and sodium sulfides, the volume changes at the cathode on cycling and the dissolution of sodium poly sulfides in the electrolyte. [9,[13][14][15] To date, extensive efforts have been made toward the enhancement of RT-Na/S batteries, including Na 2 S cathodes, [16,17] carbonaceous buffer matrixes, [12,18,19] a class of sodium polysulfides, [20,21] and the functional carbon-coated Nafion separator. [22] These approaches, while are validated to improve the cyclability of the RT Na-S batteries, tend to result in complicated synthetic processes and decreased theoretical capacity. In addition, it was suggested that the polar-polar interaction is a strong chemical interaction between polar sodium polysulfides and polar host materials. [23,24] Although there is no universal conclusion on the exact configuration of the interactions due to the complexity of carbon matrix, their similar effect in suppressing the polysulfide shuttle has also been reported in Li-S battery systems. [25][26][27] Instead of relying on polar-polar interactions, the suitably tailored hosts can bind sodium polysulfides through metal-sulfur bonding. Examples of such materials are sub-stoichiometric metal chalcogenides, MXene phases and metal-organic frameworks (MOFs). [28][29][30][31] In practice, these oxide and sulfide materials are able to bridge sodium polysulfides through both polar-polar Na-S(O) interaction and Lewis acid-base bonding, depending on the exposed facets to some extent. [25,32] However, to simply increase metal and/or binder content only neutralizes the advantageous energy density of the overall cell. Moreover, most of the sulfur-carbon electrode materials are directly prepared using elemental S and various carbon matrixes as started materials through vapor-infiltration or meltinfusion method. [8,10] As a result, the aggregated particles are Room temperature sodium-sulfur batteries have emerged as promising candidate for application in energy storage. However, the electrodes are usually obtained through infusing elemental sulfur into various carbon sources, and the precipitation of insoluble and irreversible sulfide species on the surface of carbon and sodium readily leads to continuous capacity degradation. Here, a novel strategy is demonstrated to prepare a covalent sulfur-carbon complex (SC-BDSA) with high covalent-sulfur concentration (40.1%) that relies on SO 3 H (Benzenedisulfonic acid, BDSA) and SO 4 2− as the sulfur source rather than elemental sulfur. M...

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Section: Preparation and Physical-chemistry Features Of Sulfurized-casupporting

confidence: 76%

Controllable Chain‐Length for Covalent Sulfur–Carbon Materials Enabling Stable and High‐Capacity Sodium Storage

Jing

Yang

et al. 2019

Advanced Energy Materials

159

120

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“…S10). Considering the only N source in this case was the solvent of DMAc, we may safely conclude that the on-site defluorinated carbon atoms were extremely reactive and could even extract heteroatoms from stable organic molecules [39,50], which further demonstrated the effectiveness of our synthetic strategy for various of doped carbon materials. The morphology of control sample (the sample synthesized without melamine addition was annealed at 900°C and denoted as CrG-9-no-ME) was still crumpled form with thin layers (Fig.…”

Section: Resultsmentioning

confidence: 95%

N-doped crumpled graphene: bottom-up synthesis and its superior oxygen reduction performance

Zhang

Jin

et al. 2016

Sci. China Mater.

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The crumpled graphene (CrG) was fabricated by applying defluorination of polyvinylidenefluoride (PVDF) on highly curved surface of CaC2 particle through bottom-up synthetic strategy. The limited reaction depth between PVDF and CaC2 leads to the formation of CrG with thin layer (3−6 layer graphene) and reasonable high specific surface area (~324.8 m 2 g −1 ). CrG with N incorporation (N-CrG) was applied as electrode material for reducing oxygen (i.e., oxygen reduction reaction, ORR) in alkaline, showing close onset potential to that of Pt/C and better mass-diffusion behavior. Surprisingly, with increased mass loading of catalysts, N-CrG exhibits steady current increase while Pt/C shows clear current plateau. Meanwhile, the N-CrG sample reveals high cycling stability and tolerance to contaminant, demonstrating its high potential for practical applications. Additionally, the bottom-up synthetic pathway to CrG via polymer dehalogenation on solid alkaline may find more applications which require controlled morphology and thickness of deposited thin graphitic carbon layers.

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“…Usually, the pyrolysis processes are carried out under an inert atmosphere. As replacements of pyrolysis, some novel techniques like hydrothermal carbonization,36 microwave‐assisted carbonization,34 dehydrogenation/deoxygenation enabled by high concentrated sulfuric acid,28 and dehalogenation of halogenated organic polymers37 have also been applied to perform the carbonization process. These novel carbonization techniques enable the formation of carbonaceous materials with novel structures and different chemical compositions compared with traditional carbonization methods.…”

Section: Carbonization–activation Methodsmentioning

confidence: 99%

“…Recently, dehalogenation became a general method that can transform halogen‐containing polymers into porous carbons. Dai et al discovered that polyvinylidene chloride (PVDC) could be directly transformed into a carbonaceous material using dehalogenation reaction by KOH in ethyl alcohol solution ( Figure a) 37. The dehalogenation of PVDC is composed of multiple processes.…”

Section: New Porogen Engineering Methodsmentioning

confidence: 99%

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Synthesis Strategies of Porous Carbon for Supercapacitor Applications

et al. 2020

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Supercapacitors (SCs) have experienced a significant increase in research activity and commercialization during the past few decades. As the primary and most important electrode active material for commercial SCs, porous carbon is produced at an industrial‐scale through traditional carbonization‐activation strategies. Nevertheless, commercial porous carbon materials have some disadvantages such as high production cost, corrosion of equipment, and emission of toxic gases and byproduct pollutants during production. In recent years, huge efforts have been made to develop novel synthesis strategies for porous carbon materials. This review focuses on the pore formation mechanisms in traditional carbonization‐activation methods, emerging activation methods, template methods, self‐template methods, and novel emerging methods for the synthesis of porous carbons for SCs. Strategies developed so far for the synthesis of porous carbon materials are summarized. The mechanisms and recent advances for each strategy are reviewed. Furthermore, future directions and synthesis strategies for porous carbons are proposed.

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Unconventional Carbon: Alkaline Dehalogenation of Polymers Yields N‐Doped Carbon Electrode for High‐Performance Capacitive Energy Storage

Cited by 101 publications

References 46 publications

Controllable Chain‐Length for Covalent Sulfur–Carbon Materials Enabling Stable and High‐Capacity Sodium Storage

Controllable Chain‐Length for Covalent Sulfur–Carbon Materials Enabling Stable and High‐Capacity Sodium Storage

N-doped crumpled graphene: bottom-up synthesis and its superior oxygen reduction performance

Synthesis Strategies of Porous Carbon for Supercapacitor Applications

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