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![Figure S4 . TGA (black solid line) and DSC (green dot line) curves. (a). CMK-3/S/D[ 7 ]; (b). CMK-3/S/D[ 14 ]; (c). CMK-3/S/D[ 22 ].](profile/Chenggang-Zhou-2/publication/273473005/figure/fig4/AS:303204173664259@1449300916946/Figure-S4-TGA-black-solid-line-and-DSC-green-dot-line-curves-a-CMK-3-S-D-7.png)
Figure S4 . TGA (black solid line) and DSC (green dot line) curves. (a). CMK-3/S/D[ 7 ]; (b). CMK-3/S/D[ 14 ]; (c). CMK-3/S/D[ 22 ].
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![Figure S5. BJH mesopore distributions of CMK-3, CMK-3/S, CMK-3/D/S[14]...](profile/Chenggang-Zhou-2/publication/273473005/figure/fig5/AS:303204173664260@1449300916977/Figure-S5-BJH-mesopore-distributions-of-CMK-3-CMK-3-S-CMK-3-D-S14-and-CMK-3-S-D14_Q320.jpg)
Prohibiting lithium polysulfides from being dissolved to electrolyte is the most critical challenge for pursuing high-performance Li/S batteries. Taking full advantage of interactions between polysulfides and functional groups of third-party additives has been proven to be an efficient strategy. In the present work, we selected DNA to decorate CMK-...
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... For example, the development of novel biomaterials holds promise in the energy sector. Specifically, nucleic acids have been explored as a way to enhance lithium-sulfur batteries (Li et al., 2015). Alternatively, there is increasing interest in the design of nucleic acid biosensors to detect toxic metals in the environment or body (Zhou et al., 2017). ...
Accurate information about interactions between group I metals and nucleic acids is required to understand the roles these metals play in basic cellular functions, disease progression, and pharmaceuticals, as well as to aid the design of new energy storage materials and nucleic acid sensors that target metal contaminants, among other applications. From this perspective, this work generates a complete CCSD(T)/CBS data set of the binding energies for 64 complexes involving each group I metal (Li⁺, Na⁺, K⁺, Rb⁺, or Cs⁺) directly coordinated to various sites in each nucleic acid component (A, C, G, T, U, or dimethylphosphate). This data have otherwise been challenging to determine experimentally, with highly accurate information missing for many group I metal–nucleic acid combinations and no data available for the (charged) phosphate moiety. Subsequently, the performance of 61 DFT methods in combination with def2-TZVPP is tested against the newly generated CCSD(T)/CBS reference values. Detailed analysis of the results reveals that functional performance is dependent on the identity of the metal (with increased errors as group I is descended) and nucleic acid binding site (with larger errors for select purine coordination sites). Over all complexes considered, the best methods include the mPW2-PLYP double-hybrid and ωB97M-V RSH functionals (≤1.6% MPE; <1.0 kcal/mol MUE). If more computationally efficient approaches are required, the TPSS and revTPSS local meta-GGA functionals are reasonable alternatives (≤2.0% MPE; <1.0 kcal/mol MUE). Inclusion of counterpoise corrections to account for basis set superposition error only marginally improves the computed binding energies, suggesting that these corrections can be neglected with little loss in accuracy when using larger models that are necessary for describing biosystems and biomaterials. Overall, the most accurate functionals identified in this study will permit future works geared towards uncovering the impact of group I metals on the environment and human biology, designing new ways to selectively sense harmful metals, engineering modern biomaterials, and developing improved computational methods to more broadly study group I metal–nucleic acid interactions.
... To overcome these issues, the trapping of sulfur inside the porous carbon material matrix with different arrangements (for example, graphene, graphene oxide, porous carbon, and carbon nanotubes) were employed [9][10][11][12]. Out of these, GO and rGO have attracted extensive consideration [13][14][15][16][17] due to their stability, lightweight, enormous surface territory, high electrical conductivity, incredible adaptability, and mechanical properties compared to other carbon materials [18,19]. GO can easily be deposited on the surface of the material and binds it due to its hydrophilic nature as it contains more oxygen contents as compared to graphene. ...
All-solid-state Li-S batteries (use of solid electrolyte LiBH4) were prepared using cathodes of a homogeneous mixture of graphene oxide (GO) and reduced graphene oxide (rGO) with sulfur (S) and solid electrolyte lithium borohydride (LiBH4), and their electrochemical performance was reported. The use of LiBH4 and its compatibility with Li metal permits the utilization of Li anode that improves the vitality of composite electrodes. The GO-S and rGO-S nanocomposites with different proportions have been synthesized. Their structural and morphological characterizations were performed by X-ray diffraction (XRD) and scanning electron microscopy (SEM), and the results are presented. The electrochemical performance was tested by galvanostatic charge-discharge measurements at a 0.1 C-rate. The results presented here demonstrate the successful implementation of GO-S composites in an all-solid-state battery.
... 13,14 To overcome these drawbacks, signicant efforts have been carried out to improve the performance of Li-S battery by incorporating additives into sulfur cathodes, including carbon materials, [15][16][17] conductive polymers [18][19][20] and metal oxides. 6,21 It was reported that carbon materials added into sulfur cathode are effective in improving the comprehensive performances of sulfur cathode, including CMK-3, 22 carbon nanotubes, 23 and carbon nanobers. 24 Meanwhile some conductive polymers were coated onto the sulfur cathode to reduce the dissolution of lithium polysuldes and increase the conductivity of sulfur, including polyaniline 25,26 and polypyrrole. ...
Composite materials with a stable network structure consisting of natural sepiolite (Sep) powders, carbon nanotubes (CNTs) and conductive polymer (PANI) have been successfully synthesized using a simple vacuum heat treatment and chemical oxidation method, and they have been used as cathode materials for lithium sulfur batteries. It is found that Sep/CNT/S@PANI composites possess high initial discharge capacity, good cyclic stability and good rate performance. The initial discharge capacity of the Sep/CNT/S@PANI-II composite is about 1100 mA h g⁻¹ at 2C, and remained at 650 mA h g⁻¹ after 300 cycles, and the corresponding coulombic efficiency is above 93%. Such performance is attributed to specific porous structure, outstanding adsorption characteristics, and excellent ion exchange capability of sepiolite, as well as excellent conductivity of CNT. Furthermore, the PANI coating has a pinning effect for sulfur, which enhances the utilization of the active mass and improves the cycling stability and the coulombic efficiency of the composites at high current rates.
... R 0 and R ct represent ohmic resistance and charge transfer resistance, respectively; CPE1 and CPE2 are the equivalent link of double-layer capacitance in the solid electrolyte interface (SEI) film and electrodes, respectively, which coordinate with the resistance of SEI films (R s ) and R ct relative to the semicircle at medium and high frequency region; W 0 represents the diffusion-controlled Warburg impedance related to the diffusion of Li + in the electrode. 10,11,27 Figure 6a− c show the Nyquist plots of S-I, S-II, and S-III at different states and cycles. In comparison, the relatively low and overlapped R s of S-II can be ascribed to the introduction of a conductive cathodic interlayer, which effectively hinders the cracking of sulfur particles and guarantees steady surface situations. ...
... (j) Percentage of sulfur in the electrolyte relative to the total sulfur mass on the electrode after cycling at 0.2C using PVP binder in comparison with PVDF binder (k) Specific capacity of Li 2 S cathodes using PVP binder cycled over 200 cycles at 0.2C, in comparison with PVDF binder. Adapted with permission from Ref. 25 V C 2013 Royal Society of Chemistry.HIGHLIGHT interface between the carbon and sulfur constituents and/or act as polysulfide hosts during battery operation.[46][47][48][49][50][51][52][53][54][55] Conjugated polymers have been the focus of many examples implementing this strategy.[56][57][58][59][60][61][62][63][64][65][66][67][68][69] ...
Recent developments in the use of polymeric materials as device components in lithium sulfur (Li-S) batteries are reviewed. Li-S batteries have generated tremendous interest as a next generation battery exhibiting charge capacities and energy densities that greatly exceed Li-ion battery technologies. In this Highlight, the first comprehensive review focusing on the use of polymeric materials throughout these devices is provided. The key role polymers play in Li-S technology is presented and organized in terms of the basic components that comprise a Li-S battery: the cathode, separator, electrolyte, and anode. After a straightforward introduction to the construction of a conventional Li-S device and the mechanisms at work during cell operation, the use of polymers as binders, protective coatings, separators, electrolytes, and electroactive materials in Li-S batteries will be reviewed.
... In spite of these advantages, the peripheral polysulfides can still migrate outward from the porous carbon base, and cause ponderable capacity fading. To address this issue, scientific researchers turn to outer coating (oxide [30,31], sulfide [32][33][34], hydroxide [15], conducting polymer [35,36], DNA [37], etc.) on the S/C cathode to hinder the "shuttle effect" to promote the performance. But the majority of outer coatings have poor electrical conductivity compared with pure carbon materials, and is not beneficial for high-rate performance. ...
Tailored design/construction of high-quality sulfur/carbon composite cathode is critical for development of advanced lithium-sulfur batteries. We report a powerful strategy for integrated fabrication of sulfur impregnated into three-dimensional (3D) multileveled carbon nanoflake-nanosphere networks (CNNNs) by means of sacrificial ZnO template plus glucose carbonization. The multileveled CNNNs are not only utilized as large-area host/backbone for sulfur forming an integrated S/CNNNs composite electrode, but also serve as multiple carbon blocking barriers (nanoflake infrastructure andnanosphere superstructure) to physically confine polysulfides at the cathode. The designedself-supported S/CNNNs composite cathodes exhibit superior electrochemical performances with high capacities (1395 mAh g⁻¹ at 0.1C, and 769 mAh g⁻¹ at 5.0C after 200 cycles) and noticeable cycling performance (81.6% retention after 200 cycles). Our results build a new bridge between sulfur and carbon networks with multiple blocking effects for polysulfides, and provide references for construction of other high-performance sulfur cathodes.
... Figure 5a illustrates a scanning electron microscopy (SEM) image of CMK-3-S composite, and Figure 5b reveals a schematic diagram of the sulphur (yellow) confined in the interconnected pore structure of mesoporous carbon. From then on, a number of works reported the CMK-3 and CMK-3-based carbon composite as the sulphur host for Li-S batteries [51][52][53][54][55][56][57]. To date, in addition to the mesoporous CMK-3, researchers have developed many other kinds of mesoporous carbon by using various carbon sources as the sulphur host for Li-S batteries (also displayed in Table 1) [58][59][60][61][62][63][64][65][66][67][68][69][70][71][72][73][74][75]. ...
... . The entrapment ensured that a more complete redox process took place, and resulted in enhanced utilization of the active sulphur material.Figure 5aillustrates a scanning electron microscopy (SEM) image of CMK-3-S composite, andFigure 5breveals a schematic diagram of the sulphur (yellow) confined in the interconnected pore structure of mesoporous carbon. From then on, a number of works reported the CMK-3 and CMK-3-based carbon composite as the sulphur host for Li-S batteries[51][52][53][54][55][56][57]. ...
The effects of climate change are just beginning to be felt, and as such, society must work towards strategies of reducing humanity's impact on the environment. Due to the fact that energy production is one of the primary contributors to greenhouse gas emissions, it is obvious that more environmentally friendly sources of power are required. Technologies such as solar and wind power are constantly being improved through research; however, as these technologies are often sporadic in their power generation, efforts must be made to establish ways to store this sustainable energy when conditions for generation are not ideal. Battery storage is one possible supplement to these renewable energy technologies; however, as current Li-ion technology is reaching its theoretical capacity, new battery technology must be investigated. Lithium–sulphur (Li–S) batteries are receiving much attention as a potential replacement for Li-ion batteries due to their superior capacity, and also their abundant and environmentally benign active materials. In the spirit of environmental harm minimization, efforts have been made to use sustainable carbonaceous materials for applications as carbon–sulphur (C–S) composite cathodes, carbon interlayers, and carbon-modified separators. This work reports on the various applications of carbonaceous materials applied to Li–S batteries, and provides perspectives for the future development of Li–S batteries with the aim of preparing a high energy density, environmentally friendly, and sustainable sulphur-based cathode with long cycle life.
... Deoxyribonucleic acid (DNA), a polymer which has many -P¼O and -N¼ sites in its chain structure, has been predicted by DFT calculations to be able to fix polysulfides on these heterosites [136]. To prove this concept, CMK-3 with ordered mesopores was coated with DNA and then impregnated with sulfur at 155°C. ...
Lithium–sulfur (Li–S) battery is one of the most promising candidates for the next generation energy storage solutions, with high energy density and low cost. However, the development and application of this battery have been hindered by the intrinsic lack of suitable electrode materials, both for the cathode and anode. Recently, tremendous progress has been achieved in improving the battery performance by modifying the electrodes by the incorporation of various functional carbon materials. Carbons used in Li–S batteries not only act as conductive additives, but also as shuttling preventers, spatial confiners and anode protectors, etc. In this review, we highlight the evolution of the functionality of carbon materials with the development of Li–S batteries. The scientific understandings of the fundamental design of the materials׳ structure and chemistry in relation to the battery performance are summarized. A way to design next generation Li–S batteries can be drawn through this review.
... V vs Li/Li + ), is capable of anchoring polysulfides during charge/discharge process to enhance the cycle performance of Li/S cells. 49 Consequently, in the present work, we selected the four DN primers as the starting point of the anchoring substrates where Li 2 S 8 was employed as the probe polysulfide. By polymerizing homogeneous or heterogeneous primers, we constructed various adsorption environments to accommodate Li 2 S 8 . ...
Stabilizing lithium polysulfides in cathodes via interactions between polysulfides and affinitive functional groups could prevent polysulfide dissolution, leading to suppressed "shuttle effect" of lithium/sulfur (Li/S) batteries. Herein, four deoxynucleotides (DNs), including A (adenine-DN), T (thymine-DN), G (guanine-DN), and C (cytosine-DN), which own rich polysulfide affinitive groups, are selected to model the anchoring environments of polysulfides. Using the most soluble Li2S8 as probe, our first-principles simulations suggest that the interactions between polysulfides and substrates are highly correlated to the charges of affinitive sites, H-bonding environments and structural tension. The contributions from each type of interactions are quasi-quantitatively assessed. The electrostatic attractions between Li+ and the strong electron lone-pairs dominate the adsorption energetics, while the H-bonds formed between S82- and substrate give rise to excessive stabilization. In contrast, structural distortion or rearrangement of the substrates is detrimental to the anchoring strengths. The quasi-quantitative resolution on the different interaction modes provides a facile and rational scheme for screening more efficient polysufide affinitive additives to sustain the cathode cyclicity of Li/S batteries.
