Rational design of functional binder systems for high-energy lithium-based rechargeable batteries

Zhao, Yun; Liang, Zheng; Kang, Yuqiong; Zhou, Yunan; Li, Yanxi; He, Xiangming; Wang, Li; Mai, Weicong; Wang, Xianshu; Zhou, Guangmin; Wang, Junxiong; Li, Jiangang; Tavajohi, Naser; Li, Baohua

doi:10.1016/j.ensm.2020.11.021

Cited by 62 publications

(39 citation statements)

References 201 publications

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“…Despite the high theoretical capacity (1675 mAh g −1 ), cost effectiveness, natural abundance, and environmental friendliness of elemental sulfur, [ 1–3 ] the commercialization of lithium‐sulfur (Li–S) batteries is seriously restricted by their low sulfur loading and utilization, sluggish reaction kinetics, and poor cycling stability. [ 4,5 ] So far, appropriate active adsorption [ 6,7 ] and catalytic centers, such as metal sulfides, [ 8–10 ] oxides, [ 11–13 ] nitrides, [ 14 ] and vanadium compounds, [ 15 ] have been introduced to enhance the sulfur utilization and accelerate the reversible conversion between lithium polysulfides (LiPSs) and Li 2 S. [ 16,17 ] However, high weight percentages of these additives sacrifice the overall energy density of Li–S batteries. Single‐atom metal catalysts (SACs) comprising monodispersed metal atoms on appropriate substrates have a theoretical 100% atom utilization efficiency, and therefore have a much higher activity than conventional bulk metal and nanoparticle catalysts.…”

Section: Introductionmentioning

confidence: 99%

Engineering d‐p Orbital Hybridization in Single‐Atom Metal‐Embedded Three‐Dimensional Electrodes for Li–S Batteries

et al. 2021

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Li-S) batteries is seriously restricted by their low sulfur loading and utilization, sluggish reaction kinetics, and poor cycling stability. [4,5] So far, appropriate active adsorption [6,7] and catalytic centers, such as metal sulfides, [8][9][10] oxides, [11][12][13] nitrides, [14] and vanadium compounds, [15] have been introduced to enhance the sulfur utilization and accelerate the reversible conversion between lithium polysulfides (LiPSs) and Li 2 S. [16,17] However, high weight percentages of these additives sacrifice the overall energy density of Li-S batteries. Single-atom metal catalysts (SACs) comprising monodispersed metal atoms on appropriate substrates have a theoretical 100% atom utilization efficiency, and therefore have a much higher activity than conventional bulk metal and nanoparticle catalysts. [18,19] Various SACs have been introduced into Li-S batteries to improve their electrochemical performance. [20][21][22] Generally, the effects of SACs have been attributed to their good adsorption ability to LiPSs and their high catalytic activity. However, the lack of a fundamental understanding of the catalysis mechanism and the material properties that govern catalytic activity have hindered the selection and rational design of SACs for Li-S batteries. In previous studies, the SACs were usually Single-atom metal catalysts (SACs) are used as sulfur cathode additives to promote battery performance, although the material selection and mechanism that govern the catalytic activity remain unclear. It is shown that d-p orbital hybridization between the single-atom metal and the sulfur species can be used as a descriptor for understanding the catalytic activity of SACs in Li-S batteries. Transition metals with a lower atomic number are found, like Ti, to have fewer filled anti-bonding states, which effectively bind lithium polysulfides (LiPSs) and catalyze their electrochemical reaction. A series of single-atom metal catalysts (Me = Mn, Cu, Cr, Ti) embedded in threedimensional (3D) electrodes are prepared by a controllable nitrogen coordination approach. Among them, the single-atom Ti-embedded electrode has the lowest electrochemical barrier to LiPSs reduction/Li 2 S oxidation and the highest catalytic activity, matching well with the theoretical calculations. By virtue of the highly active catalytic center of single-atom Ti on the conductive transport network, high sulfur utilization is achieved with a low catalyst loading (1 wt.%) and a high area-sulfur loading (8 mg cm −2 ). With good mechanical stability for bending, these 3D electrodes are suitable for fabricating bendable/foldable Li-S batteries for wearable electronics.

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Section: Introductionmentioning

confidence: 99%

Engineering d‐p Orbital Hybridization in Single‐Atom Metal‐Embedded Three‐Dimensional Electrodes for Li–S Batteries

et al. 2021

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“…To further investigate the effect of binders on the electrode's morphology and its corresponding stability, the chemical structure of the three binders (as shown in Figure 1b) is compared. A binder having many carboxylate and hydroxide groups can link and form a continuous network of active materials through a strong hydrogen bond, 58 resulting in a tightly connected morphology, as observed in the SEM of the pristine CMC/ZIB and CA/ZIB (Figure 6a,c,e). The type of backbone and functional groups in a binder also plays an important role in keeping all the electrode components intact during Zn 2+ insertion and extraction from the α-MnO 2 structure.…”

Section: Resultsmentioning

confidence: 99%

Impact of Binder Functional Groups on Controlling Chemical Reactions to Improve Stability of Rechargeable Zinc-Ion Batteries

Jaikrajang

Kao-ian

Muramatsu

et al. 2021

ACS Appl. Energy Mater.

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Rechargeable zinc-ion batteries (ZIBs) are promising alternatives for large-scale energy storage systems. However, instability of the cathode during operation leads to rapid capacity fading and poor stability. Binders play a crucial role in keeping all components in the cathode intact during cycling. However, the impact of the binders’ chemical structure on the electrochemical reaction in ZIBs is not well understood. Herein, the effect of the chemical structure of a conventional polyvinylidene fluoride (PVDF) and green binders, that is, sodium carboxymethyl cellulose (CMC) and cellulose acetate (CA), on the performance, cyclability, and reaction of Zn/α-MnO2 aqueous batteries is investigated. Results show that a cathode having a PVDF binder yields the highest specific capacity in a full battery. Besides, the CMC-based ZIB is seen to attain superior cycling stability through 500 galvanostatic charge–discharge (GCD) cycles having no irreversible products confirmed by scanning electron microscopy (SEM) and X-ray diffraction (XRD). It is found that the Na+ ion in the CMC structure plays a critical role in promoting prominent battery reactions. The CMC-based ZIB, therefore, is able to maintain its high ionic diffusivity obtained from the galvanostatic intermittent titration technique (GITT) during prolonged operation. Moreover, the interaction between binders and α-MnO2 has been investigated via density-functional theory (DFT) to affirm the high stability of the ZIB/α-MnO2 with the CMC binder. This work highlights the importance of the selection of functional groups on the binder not only to enhance stability but also to control the preferential reactions of batteries. Such findings are ultimate keys for the development of low-cost, stable, and eco-friendly energy storage devices.

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“…[20,21] Certain heteroatom-containing groups for some blended polymers, such as ester groups, carbonyl groups, amides, are electron-donating groups with high space charge density. [22][23][24] Electron donor groups can provide effective binding sites to form large number of lithium bonds with LiPSs. [25,26] PVP contains abundant of amide groups, which are the typical electron-donating groups with high space charge density.…”

Section: Introductionmentioning

confidence: 99%

Enhanced Cycling Performance of All‐Solid‐State Li‐S Battery Enabled by PVP‐Blended PEO‐Based Double‐Layer Electrolyte

Zou

et al. 2022

Chemistry A European J

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Despite the high specific capacity of LiÀ S battery, shuttle effect of lithium polysulfides (LiPSs) and safety issue pose a great challenge to realize its commercial application. Replacing liquid electrolyte with poly (ethylene oxide) (PEO) -based solid-state electrolyte is considered as a promising method to boost the safety, but the shuttle effect of LiPSs cannot be completely eliminated. In this work, a new kind of double-layer PEO-based polymer electrolyte is designed to restrict the LiPSs. The layer next to cathode consists of PEO and poly(vinylpyrrolidone) (PVP). The other layer consists of PEO. PVP with abundant of amide groups has been proved to have strong affinity to LiPSs. The strong interaction between LiPSs and carbonyl groups in amide is verified by Attenuated Total Reflection-Fourier transform infrared spectroscopy and X-ray photoelectron spectroscopy tests. As a result, the assembled LiÀ S battery exhibits a specific capacity of 1100 mAh g À 1 and capacity retention of 347 mAh g À 1 after 200 cycles at 60 °C and 0.05 C, while the capacity retention of the battery without PVP-blended PEO electrolyte remains only 27 % at the same conditions.

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Rational design of functional binder systems for high-energy lithium-based rechargeable batteries

Cited by 62 publications

References 201 publications

Engineering d‐p Orbital Hybridization in Single‐Atom Metal‐Embedded Three‐Dimensional Electrodes for Li–S Batteries

Engineering d‐p Orbital Hybridization in Single‐Atom Metal‐Embedded Three‐Dimensional Electrodes for Li–S Batteries

Impact of Binder Functional Groups on Controlling Chemical Reactions to Improve Stability of Rechargeable Zinc-Ion Batteries

Enhanced Cycling Performance of All‐Solid‐State Li‐S Battery Enabled by PVP‐Blended PEO‐Based Double‐Layer Electrolyte

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