An effective strategy to significantly boost the capacitive properties of Fe2O3‐based anodes by Ti doping and poly(3,4‐ethylenedioxythiophene) (PEDOT) coating is successfully demonstrated. The Ti‐Fe2O3@PEDOT electrode exhibits a significant capacitance improvement and exceptionally cyclic stability. A remarkable energy density of 0.89 mWh cm−3 can be obtained for a high‐performance asymmetric supercapacitor device consisting of Ti‐Fe2O3@PEDOT and a MnO2 anode.
Iron–nitrogen–carbon materials (Fe–N–C) are known for their excellent oxygen reduction reaction (ORR) performance. Unfortunately, they generally show a laggard oxygen evolution reaction (OER) activity, which results in a lethargic charging performance in rechargeable Zn–air batteries. Here porous S‐doped Fe–N–C nanosheets are innovatively synthesized utilizing a scalable FeCl3‐encapsulated‐porphyra precursor pyrolysis strategy. The obtained electrocatalyst exhibits ultrahigh ORR activity (E1/2 = 0.84 V vs reversible hydrogen electrode) and impressive OER performance (Ej
= 10 = 1.64 V). The potential gap (ΔE = Ej
= 10 − E1/2) is 0.80 V, outperforming that of most highly active bifunctional electrocatalysts reported to date. Furthermore, the key role of S involved in the atomically dispersed Fe–Nx species on the enhanced ORR and OER activities is expounded for the first time by ultrasound‐assisted extraction of the exclusive S source (taurine) from porphyra. Moreover, the assembled rechargeable Zn–air battery comprising this bifunctional electrocatalyst exhibits higher power density (225.1 mW cm−2) and lower charging–discharging overpotential (1.00 V, 100 mA cm−2 compared to Pt/C + RuO2 catalyst). The design strategy can expand the utilization of earth‐abundant biomaterial‐derived catalysts, and the mechanism investigations of S doping on the structure–activity relationship can inspire the progress of other functional electrocatalysts.
Vanadium oxides (VOx) have been intensely investigated as cathode materials for SCs due to the multiple stable oxidation states (III–V) of vanadium in its oxides and typical layered structure. Nevertheless, fast capacity fading is always observed for VOx upon cycling in aqueous electrolyte. Developing an efficient strategy to essentially promote the durability of VOx in mild aqueous electrolyte remains a crucial challenge. Here, an innovative and effective method is reported to significantly boost the durability and capacitance of VOx through tuning the valence state of vanadium. The valence state of vanadium is optimized through a very facile electrochemical oxidation method. A superior electrochemical performance and an ultralong cyclic stability of 100 000 cycles are obtained for these electrodes. An in‐depth study on the variation for the valence state of vanadium during the oxidation process and the cyclic stability test indicates that the long cyclic stability has an important relationship with the distribution of the valence state of vanadium.
Advances in solid-state batteries have primarily been driven by the discovery of superionic conducting structural frameworks that function as solid electrolytes. We demonstrate the ability of high-entropy metal cation mixes to improve ionic conductivity in a compound, which leads to less reliance on specific chemistries and enhanced synthesizability. The local distortions introduced into high-entropy materials give rise to an overlapping distribution of site energies for the alkali ions so that they can percolate with low activation energy. Experiments verify that high entropy leads to orders-of-magnitude higher ionic conductivities in lithium (Li)–sodium (Na) superionic conductor (Li-NASICON), sodium NASICON (Na-NASICON), and Li-garnet structures, even at fixed alkali content. We provide insight into selecting the optimal distortion and designing high-entropy superionic conductors across the vast compositional space.
In this work, hierarchical core-shell NiMoO@Ni-Co-S nanorods were first successfully grown on nickel foam by a facile two-step method to fabricate a bind-free electrode. The well-aligned electrode wrapped by Ni-Co-S nanosheets displays excellent nanostructural properties and outstanding electrochemical performance, owing to the synergistic effects of both nickel molybdenum oxides and nickel cobalt sulfides. The prepared core-shell nanorods in a three-electrode cell yielded a high specific capacitance of 2.27 F cm (1892 F g) at a current density of 5 mA cm and retained 91.7% of the specific capacitance even after 6000 cycles. Their electrochemical performance was further investigated for their use as positive electrode for asymmetric supercapacitors. Notably, the energy density of the asymmetric supercapacitor device reached 2.45 mWh cm at a power density of 0.131 W cm, and still retained a remarkable 80.3% of the specific capacitance after 3500 cycles. There is great potential for the electrode composed of the core-shell NiMoO@Ni-Co-S nanorods for use in an all-solid-state asymmetric supercapacitor device.
Superionic lithium conductivity has only been discovered in a few classes of materials, mostly found in thiophosphates and rarely in oxides. Herein, we reveal that corner-sharing connectivity of the oxide crystal structure framework promotes superionic conductivity which we rationalize from their distorted lithium environment and reduced interaction between lithium and non-Li cations. By performing a high-throughput search for materials with this feature, we discover 10 novel oxide frameworks predicted to exhibit superionic conductivity-from which we experimentally demonstrate LiGa(SeO3)2 with a bulk ionic conductivity of 0.11 mS/cm and activation energy of 0.17 eV. Our findings provide new insight into the factors that govern fast lithium mobility in oxide materials and will accelerate the development of novel oxide electrolytes for all solid-state batteries.
Hollow fusiform RuO 2 $xH 2 O nanostructures were prepared by using a-Fe 2 O 3 nanospindles as a sacrificial template via a hydrothermal approach and have demonstrated good energy storage capability in pseudocapacitors with high-rate performance and excellent cycling stability.
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