Practical application of aqueous Zn‐ion batteries (AZIBs) is significantly limited by poor reversibility of the Zn anode. This is because of 1) dendrite growth, and 2) water‐induced parasitic reactions including hydrogen evolution, during cycling. Here for the first time an elegantly simple method is reported that introduces ethylene diamine tetraacetic acid tetrasodium salt (Na4EDTA) to a ZnSO4 electrolyte. This is shown to concomitantly suppress dendritic Zn deposition and H2 evolution. Findings confirm that EDTA anions are adsorbed on the Zn surface and dominate active sites for H2 generation and inhibit water electrolysis. Additionally, adsorbed EDTA promotes desolvation of Zn(H2O)62+ by removing H2O molecules from the solvation sheath of Zn2+. Side reactions and dendrite growth are therefore suppressed by using the additive. A high Zn reversibility with Coulombic efficiency (CE) of 99.5% and long lifespan of 2500 cycles at 5 mAh cm−2, 2 mAh cm−2 is demonstrated. Additionally, the highly reversible Zn electrode significantly boosts overall performance of VO2//Zn full‐cells. These findings are expected to be of immediate benefit to a range of researchers in using dual‐function additives to suppress Zn dendrite and parasitic reactions for electrochemistry and energy storage applications.
Field effect regulation of DNA nanoparticle translocation through a nanopore using a gate electrode is investigated using a continuum model, composed of the coupled Poisson-Nernst-Planck equations for the ionic mass transport and the Navier-Stokes equations for the hydrodynamic field. The field effect regulation of the DNA translocation relies on the induced electroosmotic flow (EOF) and the particle-nanopore electrostatic interaction. When the electrical double layers (EDLs) formed adjacent to the DNA nanoparticle and the nanopore wall are overlapped, the particle-nanopore electrostatic interaction could dominate over the EOF effect, which enables the DNA trapping inside the nanopore when the applied electric field is relatively low. However, the particle-nanopore electrostatic interaction becomes negligible if the EDLs are not overlapped. When the applied electric field is relatively high, a negative gate potential can slow down the DNA translocation by an order of magnitude, compared to a floating gate electrode. The field effect control offers a more flexible and electrically compatible approach to regulate the DNA translocation through a nanopore for DNA sequencing.
As a compound analogue of black phosphorus, a new 2D semiconductor of SnS layers is proposed. Based on state-of-the-art theoretical calculations, we confirm that such 2D SnS layers are thermally and dynamically stable and can be mechanically exoliated from α-phase SnS bulk materials. The 2D SnS layer has an indirect band gap that can be tuned from 1.96 eV for the monolayer to 1.44 eV for a six-layer structure. Interestingly, the decrease of the band gap with increasing number of layers is not monotonic but shows an odd−even quantum confinement effect, because the interplay of spin−orbit coupling and lack of inversion symmetry in odd-numbered layer structures results in anisotropic spin splitting of the energy bands. It was also found that such 2D SnS layers show high in-plane anisotropy and high carrier mobility (tens of thousands of cm 2 V −1 s −1 ) even superior to that of black phosphorus, which is dominated by electrons. With these intriguing electronic properties, such 2D SnS layers are expected to have great potential for application in future nanoelectronics.
large-scale energy-storage systems. [2] Aqueous zinc-based batteries with high safety and low cost provide a new opportunity for energy storage on a large scale. [3] Among the series of zinc-based batteries, the rechargeable zinc-iodine (Zn-I 2 ) battery is promising owing to abundant reserves of iodine in seawater (55 µg L −1 ), [4] high specific capacity (211 mAh g iodine −1), [5] and high discharge potential plateau (1.38 V vs Zn/Zn 2+ ). [6] Besides, the liquid-phase conversion mechanism of I − /I 2 in cathode endows a Zn-I 2 system with excellent rate capability. [7] However, the state-of-the-art Zn-I 2 batteries are still far from satisfactory due to the challenges of intermediates dissolution as well as Zn-anode corrosion. [4a] In aqueous electrolytes, Zn-I 2 batteries present a reversible I − /I 2 redox reaction, in which polyiodide species work as the intermediate state. [7] However, highly soluble polyiodide intermediates cause the serious shuttle effect, leading to irreversible loss of active mass. Even worse, the direct reaction between shuttling polyiodide and Zn anodes will further aggravate serious Zn corrosion and consumption, leading to the low Coulombic efficiency (CE), and limited durability of Zn-I 2 batteries. Therefore, inhibiting the shuttle effect of polyiodide is of great importance to stabilize the I 2 cathode and alleviate the Zn corrosion toward high-cyclability Zn-I 2 batteries. AqueousZn-iodine (Zn-I 2 ) batteries have been regarded as a promising energy-storage system owing to their high energy/power density, safety, and cost-effectiveness. However, the polyiodide shuttling results in serious active mass loss and Zn corrosion, which limits the cycling life of Zn-I 2 batteries. Inspired by the chromogenic reaction between starch and iodine, a structure confinement strategy is proposed to suppress polyiodide shuttling in Zn-I 2 batteries by hiring starch, due to its unique double-helix structure. In situ Raman spectroscopy demonstrates an I 5 − -dominated I − /I 2 conversion mechanism when using starch. The I 5 − presents a much stronger bonding with starch than I 3 − , inhibiting the polyiodide shuttling in Zn-I 2 batteries, which is confirmed by in situ ultraviolet-visible spectra. Consequently, a highly reversible Zn-I 2 battery with high Coulombic efficiency (≈100% at 0.2 A g −1 ) and ultralong cycling stability (>50 000 cycles) is realized. Simultaneously, the Zn corrosion triggered by polyiodide is effectively inhibited owing to the desirable shuttling-suppression by the starch, as evidenced by X-ray photoelectron spectroscopy analysis. This work provides a new understanding of the failure mechanism of Zn-I 2 batteries and proposes a cheap but effective strategy to realize high-cyclability Zn-I 2 batteries.The ORCID identification number(s) for the author(s) of this article can be found under https://doi.org/10.1002/adma.202201716.
The development of SiO x electrode with high mass loading, which is an important prerequisite for practical lithium-ion batteries, remains an arduous challenge by using existing binders. Herein, we propose a three-in-one design strategy for binder systems in allintegrated SiO x electrodes. "Hard" poly(furfuryl alcohol) (PFA) and "soft" thermoplastic polyurethane (TPU) are interweaved into 3D conformation to confine SiO x particles via in-situ polymerization. In the electrode system, PFA works as a framework and TPU servers as a buffer, and H-bonding interactions are formed between the components. Benefiting from the three-pronged collaborative strategy, PFA-TPU/SiO x electrode exhibits an areal capacity of 2.4 mAh cm −2 at a high mass loading of >3.0 mg cm −2 after 100 cycles. Such a binder system is also extended to other potential metal oxides anode with high mass loading, e.g., Fe 2 O 3 and SnO 2 , thus shedding light on rational design of functional polymer binders for high-areal-capacity electrodes.
Lithium–sulfur (Li–S) batteries are considered to be one of the most promising candidate systems for next‐generation electrochemical energy storage. The major challenge of this system is the polysulfide shuttle, which results in poor cycling efficiency. In this work, a highly N‐doped carbon/graphene (NC/G) sheet is designed as a sulfur host, which combines the merits of abundant N active sites and high electrical conductivity to achieve in situ anchoring–conversion of lithium polysulfides (LiPSs). Such a host not only has strong binding with LiPSs but also promotes redox kinetics, which are revealed by both experimental investigations and theoretical studies. The sulfur cathode based on the NC/G host exhibits a high initial capacity of 1380 mA h g−1 and a superior cycle stability with a low capacity decay of 0.037% per cycle within 500 cycles at 2 C. Steady areal capacity with a high sulfur loading (5.6 mg cm−2) is also attained even without the addition of LiNO3 in the electrolyte. This work proposes and illustrates the importance of in situ anchoring–conversion of LiPSs, offering a new strategy to design multifunctional sulfur hosts for high‐performance Li–S batteries.
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