Aqueous rechargeable zinc‐ion batteries (ZIBs) have attracted considerable attention as a promising candidate for low‐cost and high‐safety electrochemical energy storage. However, the advancement of ...ZIBs is strongly hindered by the sluggish ionic diffusion and structural instability of inorganic metal oxide cathode materials during the Zn2+ insertion/extraction. To address these issues, a new organic host material, poly(2,5‐dihydroxy‐1,4‐benzoquinonyl sulfide) (PDBS), has been designed and applied for zinc ion storage due to its elastic structural factors (tunable space and soft lattice). The aqueous Zn‐organic batteries based on the PDBS cathode show outstanding cycling stability and rate capability. The coordination moieties (O and S) display the strong electron donor character during the discharging process and can act as the coordination arms to host Zn2+. Also, under the electrochemical environment, the malleable polymer structure of PDBS permits the rotation and bending of polymer chains to facilitate the insertion/extraction of Zn2+, manifesting the superiority and uniqueness of organic electrode materials in the polyvalent cation storage. Finally, quasi‐solid‐state batteries based on aqueous gel electrolyte demonstrate highly stable capacity under different bending conditions.
A new organic polymer has been identified as a cathode material for efficient zinc ion storage due to its elastic structural factors. The coordination moieties (O and S) display strong electron donor character during the charging process and can act as the coordination arms to synergistically host Zn2+, manifesting the superiority and uniqueness of organic electrode materials in the multi‐valence cation storage.
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SAZU, SBCE, SBMB, UL, UM, UPUK
The pursuit of harmonic combination of technology and fashion intrinsically points to the development of smart garments. Herein, we present an all-solid tailorable energy textile possessing ...integrated function of simultaneous solar energy harvesting and storage, and we call it tailorable textile device. Our technique makes it possible to tailor the multifunctional textile into any designed shape without impairing its performance and produce stylish smart energy garments for wearable self-powering system with enhanced user experience and more room for fashion design. The “threads” (fiber electrodes) featuring tailorability and knittability can be large-scale fabricated and then woven into energy textiles. The fiber supercapacitor with merits of tailorability, ultrafast charging capability, and ultrahigh bending-resistance is used as the energy storage module, while an all-solid dye-sensitized solar cell textile is used as the solar energy harvesting module. Our textile sample can be fully charged to 1.2 V in 17 s by self-harvesting solar energy and fully discharged in 78 s at a discharge current density of 0.1 mA.
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IJS, KILJ, NUK, PNG, UL, UM
Tin and its derivatives have provoked tremendous progress of high‐capacity sodium‐ion anode materials. However, achieving high areal and volumetric capability with maintained long‐term stability in a ...single electrode remains challenging. Here, an elegant and versatile strategy is developed to significantly extend the lifespan and rate capability of tin sulfide nanobelt electrodes while maintaining high areal and volumetric capacities. In this strategy, in situ bundles of robust hierarchical graphene (hG) are grown uniformly on tin sulfide nanobelt networks through a rapid (5 min) carbon‐plasma method with sustainable oil as the carbon source and the partially reduced Sn as the catalyst. The nucleation of graphene, CN (with size N ranging from 1 to 24), on the Sn(111) surface is systematically explored using density functional theory calculations. It is demonstrated that this chemical‐bonded hG strategy is powerful in enhancing overall electrochemical performance.
Hierarchical graphene bundled tin sulfide (SnS) is fabricated by an ingenious in situ C‐plasma route and tested as a flexible anode for sodium‐ion batteries with unprecedented cycling lifespan, maintaining ultrahigh areal and volumetric capacities. Density functional theory calculation verifies the formation mechanism of graphene by catalysis of Sn.
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SAZU, SBCE, SBMB, UL, UM, UPUK
In photocatalysis, the Schottky barrier in metal–semiconductor hybrids is known to promote charge separation, but a core–shell structure always leads to a charge build‐up and eventually shuts off the ...photocurrent. Here, we show that Au–Cu2O hybrid nanostructures can be continuously tuned, particularly when the Cu2O domains are single‐crystalline. This is in contrast to the conventional systems, where the hybrid configuration is mainly determined by the choice of materials. The distal separation of the Au–Cu2O domains in Janus nanostructures leads to enhanced charge separation and a large improvement of the photocurrent. The activity of the Au–Cu2O Janus structures is 5 times higher than that of the core–shell structure, and 10 times higher than that of the neat Cu2O nanocubes. The continuous structural tuning allows to study the structure–property relationship and an optimization of the photocatalytic performance.
The distal arrangement of Au–Cu2O domains in the Janus structure promotes charge separation, leading to a five‐ and tenfold enhancement of the photocurrent of the Au@Cu2O core–shell structure and the neat Cu2O nanocubes, respectively.
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SAZU, SBCE, SBMB, UL, UM, UPUK
Work function strongly impacts the surficial charge distribution, especially for metal‐support electrocatalysts when a built‐in electric field (BEF) is constructed. Therefore, studying the ...correlation between work function and BEF is crucial for understanding the intrinsic reaction mechanism. Herein, we present a Pt@CoOx electrocatalyst with a large work function difference (ΔΦ) and strong BEF, which shows outstanding hydrogen evolution activity in a neutral medium with a 4.5‐fold mass activity higher than 20 % Pt/C. Both experimental and theoretical results confirm the interfacial charge redistribution induced by the strong BEF, thus subtly optimizing hydrogen and hydroxide adsorption energy. This work not only provides fresh insights into the neutral hydrogen evolution mechanism but also proposes new design principles toward efficient electrocatalysts for hydrogen production in a neutral medium.
The metal–support interaction between Pt and CoOx creates a strong built‐in electric field across the interface and modulates the charge distribution. This electric field subtly optimizes both the hydrogen and hydroxide adsorption energy, boosting the hydrogen evolution reaction in neutral media.
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SAZU, SBCE, SBMB, UL, UM, UPUK
Polynary transition‐metal atom catalysts are promising to supersede platinum (Pt)‐based catalysts for oxygen reduction reaction (ORR). Regulating the local configuration of atomic catalysts is the ...key to catalyst performance enhancement. Different from the previously reported single‐atom or dual‐atom configurations, a new type of ternary‐atom catalyst, which consists of atomically dispersed, nitrogen‐coordinated Co–Co dimers, and Fe single sites (i.e., Co2–N6 and Fe–N4 structures) that are coanchored on highly graphitized carbon supports is developed. This unique atomic ORR catalyst outperforms the catalysts with only Co2–N6 or Fe–N4 sites in both alkaline and acid conditions. Density functional theory calculations clearly unravels the synergistic effect of the Co2–N6 and Fe–N4 sites, which can induce higher filling degree of Fe–d orbitals and favors the binding capability to *OH intermediates (the rate determining step). This ternary‐atom catalyst may be a promising alternative to Pt to drive the cathodic ORR in zinc–air batteries.
A ternary‐atom electrocatalyst, in which atomically dispersed Co2–N6 and Fe–N4 sites are coanchored on N‐doped carbon hosts (derived from reaction with ZIF‐8), is synthesized. Synergistic effect is explicitly unraveled, which induces higher filling degree of Fe d‐orbitals and outstanding oxygen reduction reaction activity in both alkaline and acidic media.
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SAZU, SBCE, SBMB, UL, UM, UPUK
In the quest for mass production of hydrogen from water electrolysis, to develop highly efficient, stable and low-cost catalysts is still the central challenge. When designing a novel catalyst, it is ...necessary to optimize the exposure and accessibility of its active sites as well as the reaction kinetics. This can be realized by combining an appropriate chemical composition of the material, including doping with metal elements, and a properly nanostructured morphology offering a high surface contact. We report here on the design and performances of cobalt-based oxide and sulfide nanowires as catalysts that can be used for both hydrogen and oxygen evolution reactions (denoted HER and OER respectively) in the same compatible electrolyte. Following a sulfuration process, Co3O4 nanowires are entirely converted into Co3S4 nanowires showing greatly improved OER catalytic performances with an overpotential of 283 mV (instead of 371 mV for Co3O4) to deliver a current density of 10 mA cm−2. Besides, when doping the surface of these Co3S4 nanowires with small amounts of nickel, the resulting Ni:Co3S4 nanowires exhibit an HER overpotential of 199 mV to reach 10 mA cm−2. But most importantly, two-electrode electrolyzer cells combining Co3S4 and Ni:Co3S4 electrodes show operating voltages as low as 1.70 V at 10 mA cm−2 over 40 hours, a value that competes advantageously with the best reported catalysts in 1.0 M KOH. Meanwhile, density functional theory (DFT) calculations show that the free energy of the intermediates has been reduced after the introduction of sulfur and nickel atoms, which have smaller overpotentials and corresponding enhanced electrocatalytic performance. Our results open a new avenue in the quest for overall water splitting using electrochemical systems.
The large‐scale deployment of aqueous Zn‐ion batteries is hindered by Zn anode instability including surface corrosion, hydrogen gas evolution, and irregular Zn deposition. To tackle these ...challenges, a polyhydroxylated organic molecular additive, trehalose, is incorporated to refine the solvation structure and promote planar Zn deposition. Within solvation structure regions involving trehalose, the hydroxy groups participate in the reconstruction of hydrogen bond networks, which increases the overpotential for water decomposition reaction. Moreover, at the Zn metal–molecule interface, the chemisorption of trehalose onto the surface of the zinc anode enhances corrosion resistance and facilitates the deposition of zinc in a planar manner. The optimized electrolyte significantly improves Zn striping/plating reversibility and maintains stable potentials over 1600 h at 5 mA cm−2 with a cutoff capacity of 1 mA h cm−2 in symmetric cells. When combined with the MnO2 cathode, the assembled coin cell retains ≈89% of its capacity after 1000 cycles. This organic molecule additive, emphasizing the role of polyhydroxylated organic molecules in fine‐tuning solvation structures and anode/electrolyte interfaces, holds promise for enhancing various aqueous metal batteries.
Trehalose, a widely used moisturizer, preservative, and stabilizer in the food industry, is proven to be an effective electrolyte additive to the sulfite electrolyte for aqueous zinc ion battery. It optimizes the solvation structure by decreasing free water molecules and forming hydrogen bond networks. Trehalose also stabilizes the metal‐electrolyte interface through chemisorption, benefiting planar zinc deposition and suppressing dendrite growth.
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SAZU, SBCE, SBMB, UL, UM, UPUK
Sodium-ion batteries are a potentially low-cost and safe alternative to the prevailing lithium-ion battery technology. However, it is a great challenge to achieve fast charging and high power density ...for most sodium-ion electrodes because of the sluggish sodiation kinetics. Here we demonstrate a high-capacity and high-rate sodium-ion anode based on ultrathin layered tin(II) sulfide nanostructures, in which a maximized extrinsic pseudocapacitance contribution is identified and verified by kinetics analysis. The graphene foam supported tin(II) sulfide nanoarray anode delivers a high reversible capacity of ∼1,100 mAh g(-1) at 30 mA g(-1) and ∼420 mAh g(-1) at 30 A g(-1), which even outperforms its lithium-ion storage performance. The surface-dominated redox reaction rendered by our tailored ultrathin tin(II) sulfide nanostructures may also work in other layered materials for high-performance sodium-ion storage.
An electrolyte cation additive strategy provides a versatile route for developing high‐energy and long‐life aqueous zinc‐ion hybrid capacitors. However, the mechanisms of energy storage and Zn anode ...protection are still unclear in Zn‐based systems with dual‐ion electrolytes. Here, a dual charge storage mechanism for zinc‐ion hybrid capacitors with both cations and anions adsorption/desorption and the reversible formation of Zn4SO4(OH)6·xH2O enabled by the Mg2+ additive in the common aqueous ZnSO4 electrolyte are proposed. Theoretical calculations verify that the self‐healing electrostatic shield effect and the solvation‐sheath structure regulation rendered by the Mg2+ additive account for the observed uniform Zn deposition and dendrite suppression. As a result, an additional energy storage capacity of ≈50% compared to that in a pure 2 m ZnSO4 electrolyte and an extended cycle life with capacity retention of 98.7% after 10 000 cycles are achieved. This work highlights the effectiveness of electrolyte design for dual‐ion carrier storage mechanism in aqueous devices toward high energy density and long cycle life.
A high‐capacity Zn‐based hybrid capacitor is reported using 0.1 m MgSO4 (Mg cation additive) as an active multivalent metal‐ion charge carrier in 2 m ZnSO4 electrolyte. The Mg2+ additive contributes additional capacity, inhibits side reactions, and suppresses Zn dendrites by facilitating uniform Zn nucleation and deposition.
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FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SAZU, SBCE, SBMB, UL, UM, UPUK
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