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1.
Small ; : e2312086, 2024 Feb 27.
Article in English | MEDLINE | ID: mdl-38412409

ABSTRACT

Rechargeable aqueous aluminum batteries (AABs) are promising energy storage technologies owing to their high safety and ultra-high energy-to-price ratio. However, either the strong electrostatic forces between high-charge-density Al3+ and host lattice, or sluggish large carrier-ion diffusion toward the conventional inorganic cathodes generates inferior cycling stability and low rate-capacity. To overcome these inherent confinements, a series of promising redox-active organic materials (ROMs) are investigated and a π-conjugated structure ROMs with synergistic C═O and C═N groups is optimized as the new cathode in AABs. Benefiting from the joint utilization of multi-redox centers and rich π-π intermolecular interactions, the optimized ROMs with unique ion coordination storage mechanism facilely accommodate complex active ions with mitigated coulombic repulsion and robust lattice structure, which is further validated via theoretical simulations. Thus, the cathode achieves enhanced rate performance (153.9 mAh g-1 at 2.0 A g-1 ) and one of the best long-term stabilities (125.7 mAh g-1 after 4,000 cycles at 1.0 A g-1 ) in AABs. Via molecular exploitation, this work paves the new direction toward high-performance cathode materials in aqueous multivalent-ion battery systems.

2.
Adv Mater ; 35(51): e2301538, 2023 Dec.
Article in English | MEDLINE | ID: mdl-37876329

ABSTRACT

The strong electrostatic interaction between high-charge-density zinc ions (112 C mm-3 ) and the fixed crystallinity of traditional oxide cathodes with delayed charge compensation hinders the development of high-performance aqueous zinc-ion batteries (AZIBs). Herein, to intrinsically promote electron transfer efficiency and improve lattice tolerance, a revolutionary family of high-entropy oxides (HEOs) materials with multipath electron transfer and remarkable structural stability as cathodes for AZIBs is proposed. Benefiting from the unique "cock-tail" effect, the interaction of diverse type metal-atoms in HEOs achieves essentially broadened d-band and lower degeneracy than monometallic oxides, which contribute to convenient electron transfer and one of the best rate-performances (136.2 mAh g-1 at 10.0 A g-1 ) in AZIBs. In addition, the intense lattice strain field of HEOs is highly tolerant to the electrostatic repulsion of high-charge-density Zn2+ , leading to the outstanding cycling stability in AZIBs. Moreover, the super selectability of elements in HEOs exhibits significant potential for AZIBs.

3.
Adv Mater ; 35(8): e2209628, 2023 Feb.
Article in English | MEDLINE | ID: mdl-36480021

ABSTRACT

Due to the unique electronic structure of aluminum ions (Al3+ ) with strong Coulombic interaction and complex bonding situation (simultaneously covalent/ionic bonds), traditional electrodes, mismatching with the bonding orbital of Al3+ , usually exhibit slow kinetic process with inferior rechargeable aluminum batteries (RABs) performance. Herein, to break the confinement of the interaction mismatch between Al3+ and the electrode, a previously unexplored Se2.9 S5.1 -based cathode with sufficient valence electronic energy overlap with Al3+ and easily accessible structure is potentially developed. Through this new strategy, Se2.9 S5.1 encapsulated in multichannel carbon nanofibers with free-standing structure exhibits a high capacity of 606 mAh g-1 at 50 mA g-1 , high rate-capacity (211 mAh g-1 at 2.0 A g-1 ), robust stability (187 mAh g-1 at 0.5 A g-1 after 3,000 cycles), and enhanced flexibility. Simultaneously, in/ex-situ characterizations also reveal the unexplored mechanism of Sex Sy in RABs.

4.
Small Methods ; 6(12): e2201281, 2022 Dec.
Article in English | MEDLINE | ID: mdl-36351768

ABSTRACT

Rechargeable aluminum batteries (RABs), with abundant aluminum reserves, low cost, and high safety, give them outstanding advantages in the postlithium batteries era. However, the high charge density (364 C mm-3 ) and large binding energy of three-electron-charge aluminum ions (Al3+ ) de-intercalation usually lead to irreversible structural deterioration and decayed battery performance. Herein, to mitigate these inherent defects from Al3+ , an unexplored family of superlattice-type tungsten selenide-sodium dodecylbenzene sulfonate (SDBS) (S-WSe2 ) cathode in RABs with a stably crystal structure, expanded interlayer, and enhanced Al-ion diffusion kinetic process is proposed. Benefiting from the unique advantage of superlattice-type structure, the anionic surfactant SDBS in S-WSe2 can effectively tune the interlayer spacing of WSe2 with released crystal strain from high-charge-density Al3+ and achieve impressively long-term cycle stability (110 mAh g-1 over 1500 cycles at 2.0 A g-1 ). Meanwhile, the optimized S-WSe2 cathode with intrinsic negative attraction of SDBS significantly accelerates the Al3+ diffusion process with one of the best rate performances (165 mAh g-1 at 2.0 A g-1 ) in RABs. The findings of this study pave a new direction toward durable and high-performance electrode materials for RABs.

5.
Carbohydr Polym ; 187: 35-42, 2018 May 01.
Article in English | MEDLINE | ID: mdl-29486842

ABSTRACT

Anatase titania coated CNTs (TCNTs) and sodium lignin sulfonate (SLS) were introduced to chitosan membrane to improve the conductivity based on extra proton transfer channels built by TCNTs and sulfonate groups supplied by SLS. Water uptake, mechanical properties, oxidation stability and methanol-rejecting property of composite membranes were characterized. The results show that TCNTs and SLS doped membranes have enhanced conductivity and the sample with 5% TCNTs and 2% SLS doped (CS/TCNT-5/SLS-2) achieved a conductivity of 0.0367 S cm-1 at room temperature and 0.0647 S cm-1 at 60 °C, which is much higher than pure chitosan membrane. Moreover, with TCNTs incorporation, the mechanical properties, oxidation stability and methanol-rejecting property also improved. Overall, selectivity of CS/TCNT-5/SLS-2 sample achieved 28.2 × 104 S s cm-3 which is much higher than 3.8 × 104 S s cm-3 of pure chitosan membrane. Thus, with enhanced properties, chitosan composite membrane could be promising as proton exchange membrane (PEM) in the use of direct methanol fuel cell (DMFC).

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