A General Polymer‐Oriented Acid‐Mediated Self‐Assembly Approach toward Crystalline Mesoporous Metal Sulfides

Zhou, Hongru; Xiong, Hailong; Zhang, Rui; Zhang, Liangliang; Zhang, Ling; Li, Lin; Zhang, Wei; Zhu, Zhu; Qiao, Zhen‐An

doi:10.1002/smll.202100428

Cited by 27 publications

(23 citation statements)

References 54 publications

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“…And the positive slope of RPM also shows the construction of n-n type junctions in RPM by RGO-PANI and MoS 2 . [61] The flat band (E FB ) value of RPM (−0.45 V vs Ag/ AgCl) is between MoS 2 (−0.57 V vs Ag/AgCl) and RGO-PANI (−0.32 V vs Ag/AgCl), meaning a highway of continuous electron transport at Mott-Schottky heterointerface in RPM. [62] Similar results are observed from the high-resolution XPS result (Figure 4b,c).…”

Section: Catalytic Conversion and Reutilization Of Lipssmentioning

confidence: 99%

A Mott–Schottky Heterogeneous Layer for Li–S Batteries: Enabling Both High Stability and Commercial‐Sulfur Utilization

Shi

Zheng

Zhang

et al. 2022

Advanced Energy Materials

108

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electric vehicles. [1,2] However, the further scaled application of commercial LIBs encounters a "bottleneck": the overall energy density is approaching the ceiling due to the restriction of theoretical specific capacity of insertion-type oxide cathodes (≈250 mAh g −1 ) and graphite anodes (372 mAh −1 ). In order to satisfy the increasing demand for higher energy densities particularly under the extended application such as unmanned aerial vehicles, cargo aircraft, electric vehicles, and the exploration of novel storage system is of great significance. [3] Sulfur is earthabundant, low-cost, and environment friendly. More inspiring, lithium-sulfur batteries (LSBs) based on sulfur cathodes exhibit much higher theoretical specific capacity (1675 mAh g −1 ) through the multielectron redox reaction process, showing great potential for high-performance energy storage devices. [4] Despite the promising prospects, the practical application of LSBs is still impeded by several challenges, such as electrical insulation of sulfur and discharge products (Li 2 S/Li 2 S 2 ), severe shuttle effect of long-chain polysulfides (LiPSs, Li 2 S n , 4 ≤ n ≤ 8), low sulfur utilization, and large volume expansion (≈80%), which are critically fatal for the cycle stability and power density. [5] In the last decades, tremendous Lithium-sulfur batteries (LSBs) are severely impeded by their poor cycling stability and low sulfur utilization due to the inevitable polysulfide shuttle effect and sluggish reaction kinetics. This work reports a Mott-Schottky RGO-PANI/MoS 2 (RPM) heterogeneous layer modified separator for commercialsulfur-based LSBs through the vertical growth of molybdenum sulfide (MoS 2 ) arrays on the polyaniline (PANI) in situ reduced graphene oxide (RGO). Due to the synergistic effects of the "reservoir" constructed by MoS 2 and RGO-PANI, strong absorbability, high conductivity, and electrocatalytic activity, RPM exhibits a successive "trapping-interception-conversion" behavior toward lithium polysulfides. As a result, the LSBs assembled using a commercialsulfur as the cathode and RPM as modified layer exhibit high sulfur utilization (3.8 times higher than that of the unmodified separator at 5 C), excellent rate performance (553 mAh g −1 at 10 C), and outstanding high-rate cycle stability (524 mAh g −1 after 700 cycles at 5 C). Moreover, even at a high sulfur loading of 5.4 mg cm −2 , a favorable areal capacity of 3.8 mAh cm −2 is still maintained after 80 cycles. Theoretical calculations elucidate that such a systematic strategy can effectively suppress the shuttling effect and boost the catalytic conversion of intercepted polysulfides. This work may provide a feasible strategy to promote the practical application of commercial-sulfur-based LSBs.

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Section: Catalytic Conversion and Reutilization Of Lipssmentioning

confidence: 99%

A Mott–Schottky Heterogeneous Layer for Li–S Batteries: Enabling Both High Stability and Commercial‐Sulfur Utilization

Shi

Zheng

Zhang

et al. 2022

Advanced Energy Materials

108

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“…Unfortunately, preparing 2D uniform mesoporous materials with zincophilic sites remains intractable. 16,17 ZnS as an example, this material has an ultralow solubility product constant (K sp ) in common neutral solvents, which results in ZnS pre-precipitation 16,17 and thus destroys the mesoscopic structure of the mono-precursor, which is essential for the subsequent 2D assembly. Second, even with the welldesigned mono-precursor, it is challenging to confine the assembly route to achieve 2D morphology by common hydrothermal or solvothermal steps.…”

Section: ■ Introductionmentioning

confidence: 99%

2D Mesoporous Zincophilic Sieve for High-Rate Sulfur-Based Aqueous Zinc Batteries

Liu

Han

et al. 2023

J. Am. Chem. Soc.

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Sulfur-based aqueous zinc batteries (SZBs) attract increasing interest due to their integrated high capacity, competitive energy density, and low cost. However, the hardly reported anodic polarization seriously deteriorates the lifespan and energy density of SZBs at a high current density. Here, we develop an integrated acid-assisted confined self-assembly method (ACSA) to elaborate a two-dimensional (2D) mesoporous zincophilic sieve (2DZS) as the kinetic interface. The as-prepared 2DZS interface presents a unique 2D nanosheet morphology with abundant zincophilic sites, hydrophobic properties, and small-sized mesopores. Therefore, the 2DZS interface plays a bifunctional role in reducing the nucleation and plateau overpotential: (a) accelerating the Zn 2+ diffusion kinetics through the opened zincophilic channels and (b) inhibiting the kinetic competition of hydrogen evolution and dendrite growth via the significant solvation−sheath sieving effect. Therefore, the anodic polarization is reduced to 48 mV at 20 mA cm −2 , and the full-battery polarization is reduced to 42% of an unmodified SZB. As a result, an ultrahigh energy density of 866 Wh kg sulfur −1 at 1 A g −1 and a long lifespan of 10,000 cycles at a high rate of 8 A g −1 are achieved.

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“…Additionally, the experimental conditions, such as temperature and pH values, which are needed for the self-assembly of the soft-template are typically different to the ones needed for the crystallization of the metal sulfide. 9,10 In case of the nanocasting route, even though the exotemplate is not influenced by the conditions needed for the formation of the metal sulfides, as they are produced at an earlier step and it can be stable at very high temperatures, the main problem lies on the use of hazardous chemicals (e.g. HF) for its removal.…”

Section: Introductionmentioning

confidence: 99%

Honeycomb-structured copper indium sulfide thin films obtainedviaa nanosphere colloidal lithography method

et al. 2022

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A General Polymer‐Oriented Acid‐Mediated Self‐Assembly Approach toward Crystalline Mesoporous Metal Sulfides

Cited by 27 publications

References 54 publications

A Mott–Schottky Heterogeneous Layer for Li–S Batteries: Enabling Both High Stability and Commercial‐Sulfur Utilization

A Mott–Schottky Heterogeneous Layer for Li–S Batteries: Enabling Both High Stability and Commercial‐Sulfur Utilization

2D Mesoporous Zincophilic Sieve for High-Rate Sulfur-Based Aqueous Zinc Batteries

Honeycomb-structured copper indium sulfide thin films obtainedviaa nanosphere colloidal lithography method

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