Metallic zinc is an attractive anode material for aqueous rechargeable batteries because of its high theoretical capacity and low cost. However, state-of-the-art zinc anodes suffer from low coulombic efficiency and severe dendrite growth during stripping/plating processes, hampering their practical applications. Here we show that eutectic-composition alloying of zinc and aluminum as an effective strategy substantially tackles these irreversibility issues by making use of their lamellar structure, composed of alternating zinc and aluminum nanolamellas. The lamellar nanostructure not only promotes zinc stripping from precursor eutectic Zn 88 Al 12 (at%) alloys, but produces core/shell aluminum/aluminum sesquioxide interlamellar nanopatterns in situ to in turn guide subsequent growth of zinc, enabling dendritefree zinc stripping/plating for more than 2000 h in oxygen-absent aqueous electrolyte. These outstanding electrochemical properties enlist zinc-ion batteries constructed with Zn 88 Al 12 alloy anode and K x MnO 2 cathode to deliver high-density energy at high levels of electrical power and retain 100% capacity after 200 hours.
Aqueous aluminum batteries are promising post-lithium battery technologies for large-scale energy storage applications because of the raw materials abundance, low costs, safety and high theoretical capacity. However, their development is hindered by the unsatisfactory electrochemical behaviour of the Al metal electrode due to the presence of an oxide layer and hydrogen side reaction. To circumvent these issues, we report aluminum-copper alloy lamellar heterostructures as anode active materials. These alloys improve the Al-ion electrochemical reversibility (e.g., achieving dendrite-free Al deposition during stripping/plating cycles) by using periodic galvanic couplings of alternating anodic α-aluminum and cathodic intermetallic Al2Cu nanometric lamellas. In symmetric cell configuration with a low oxygen concentration (i.e., 0.13 mg L−1) aqueous electrolyte solution, the lamella-nanostructured eutectic Al82Cu18 alloy electrode allows Al stripping/plating for 2000 h with an overpotential lower than ±53 mV. When the Al82Cu18 anode is tested in combination with an AlxMnO2 cathode material, the aqueous full cell delivers specific energy of ~670 Wh kg−1 at 100 mA g−1 and an initial discharge capacity of ~400 mAh g−1 at 500 mA g−1 with a capacity retention of 83% after 400 cycles.
Metallic zinc (Zn) is one of the most attractive multivalent-metal anode materials in post-lithium batteries because of its high abundance, low cost and high theoretical capacity. However, it usually suffers from large voltage polarization, low Coulombic efficiency and high propensity for dendritic failure during Zn stripping/plating, hindering the practical application in aqueous rechargeable zinc-metal batteries (AR-ZMBs). Here we demonstrate that anionic surfactant-assisted in situ surface alloying of Cu and Zn remarkably improves Zn reversibility of 3D nanoporous Zn electrodes for potential use as high-performance AR-ZMB anode materials. As a result of the zincophilic ZnxCuy alloy shell guiding uniform Zn deposition with a zero nucleation overpotential and facilitating Zn stripping via the ZnxCuy/Zn galvanic couples, the self-supported nanoporous ZnxCuy/Zn electrodes exhibit superior dendrite-free Zn stripping/plating behaviors in ambient aqueous electrolyte, with ultralow polarizations under current densities up to 50 mA cm‒2, exceptional stability for 1900 h and high Zn utilization. This enables AR-ZMB full cells constructed with nanoporous ZnxCuy/Zn anode and KzMnO2 cathode to achieve specific energy of as high as ~ 430 Wh kg‒1 with ~ 99.8% Coulombic efficiency, and retain ~ 86% after long-term cycles for > 700 h.
The general formula of perovskites can be written as A n BX 2+n , where A is monovalent cation like MA + (CH 3 NH 3 + ), [7] FA + ( + HC(NH 2 ) 2 ), [8] GA + ( + C(NH 2 ) 3 ), [9] and so forth, B is a divalent metal, usually Pb 2+ or Sn 2+ , and X is a halogen anion or hybrid halogen anions. When n = 1, the dimension of the perovskite is 3D, as we insert a larger organic group in A site, the structure dimension of perovskite is thereby transformed to 2D, 1D, or even 0D, which enables to enhance the structural stability against the humidity, and also realize the quantum self-trapped effect toward high photoluminescence quantum yield (PLQY). [10,11] For the displaying application, not only the high PLQY is required, but color-tunable emission is also a necessary characteristic, [12,13] which is generally realized through ion doping and/or substitution, such as Cs 4−x A x Sn(Br 1−y I y ) 6 [14] (A = Rb, K; x ≤ 1, y ≤ 1), Cs 2 AgIn x Fe 1−x Cl 6[15](0 ≤ x ≤ 1), PEA 2 (Rb x Cs 1−x ) n−1 Pb n (Br 1−y Cl y ) 3n+1 , [16] etc. Additionally, dimension regulation is also an effective way to control emission wavelength, e.g.
Metallic interface engineering is a promising strategy to stabilize Zn anode via promoting Zn2+ uniform deposition. However, strong interactions between the coating and Zn2+ and sluggish transport of Zn2+ lead to high anodic polarization. Here, we present a bio-inspired silk fibroin (SF) coating with amphoteric charges to construct an interface reversible electric field, which manipulates the transfer kinetics of Zn2+ and reduces anodic polarization. The alternating positively and negatively charged surface as a build-in driving force can expedite and homogenize Zn2+ flux via the interplay between the charged coating and adsorbed ions, endowing the Zn-SF anode with low polarization voltage and stable plating/stripping. Experimental analyses with theoretical calculations suggest that SF can facilitate the desolvation of [Zn(H2O)6]2+ and provide nucleation sites for uniform deposition. Consequently, the Zn-SF anode delivers a high-rate performance with low voltage polarization (83 mV at 20 mA cm−2) and excellent stability (1500 h at 1 mA cm−2; 500 h at 10 mA cm−2), realizing exceptional cumulative capacity of 2.5 Ah cm−2. The full cell coupled with ZnxV2O5·nH2O (ZnVO) cathode achieves specific energy of ~ 270.5/150.6 Wh kg−1 (at 0.5/10 A g−1) with ~ 99.8% Coulombic efficiency and retains ~ 80.3% (at 5.0 A g−1) after 3000 cycles.
Aqueous all-polymer proton batteries (APPBs) consisting of redox-active polymer electrodes are considered safe and clean renewable energy storage sources. However, there remain formidable challenges for APPBs to withstand a high current rate while maximizing high cell output voltage within a narrow electrochemical window of aqueous electrolytes. Here, a capacitive-type polymer cathode material is designed by grafting poly(3,4-ethylenedioxythiophene) (PEDOT) with bioinspired redox-active catechol pendants, which delivers high redox potential (0.60 V vs Ag/AgCl) and remarkable rate capability. The pseudocapacitive-dominated proton storage mechanism illustrated by the density functional theory (DFT) calculation and electrochemical kinetics analysis is favorable for delivering fast charge/discharge rates. Coupled with a diffusion-type anthraquinone-based polymer anode, the APPB offers a high cell voltage of 0.72 V, outstanding rate capability (64.8% capacity retention from 0.5 to 25 A g −1 ), and cycling stability (80% capacity retention over 1000 cycles at 2 A g −1 ), which is superior to the state-of-the-art all-organic proton batteries. This strategy and insight provided by DFT and ex situ characterizations offer a new perspective on the delicate design of polymer electrode patterns for high-performance APPBs.
Aluminum is an attractive anode material in aqueous multivalent-metal batteries for large-scale energy storage because of its high Earth abundance, low cost, high theoretic capacity, and safety. However, state-of-the-art aqueous aluminum-ion batteries based on aluminum anode persistently suffer from poor rechargeability and low coulombic efficiency due to irreversibility of aluminum stripping/plating and dendrite growth. Here eutectic aluminumcerium alloys in situ grafted with uniform ultrathin MXene (MXene/E-Al 97 Ce 3 ) as flexible, reversible, and dendrite-free anode materials for rechargeable aqueous aluminum-ion batteries is reported. As a result of the MXene serving as stable solid electrolyte interphase to inhibit side reactions and the lamellananostructured E-Al 97 Ce 3 enabling directional Al stripping and deposition by making use of symbiotic α-Al metal and intermetallic Al 11 Ce 3 lamellas, the MXene/E-Al 97 Ce 3 hybrid electrodes exhibit reversible and dendrite-free Al stripping/plating with low voltage polarization of ± 54 mV for ≥1000 h in a low-oxygen-concentration aqueous aluminum trifluoromethanesulfonate (Al(OTF) 3 ) electrolyte. These superior electrochemical properties endow softpackage aluminum-ion batteries assembled with MXene/E-Al 97 Ce 3 anode and Al x MnO 2 cathode to have high initial discharge capacity of ≈360 mAh g −1 at 1 A g −1 , and retain ≈85% after 500 cycles, along with the coulombic efficiency of as high as 99.5%.
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