The development of aqueous rechargeable zinc-iodine (Zn-I 2 ) batteries is still plagued by the polyiodide shuttle issue, which frequently causes batteries to have inadequate cycle lifetimes. In this study, quaternization engineering based on the concept of "electric double layer" is developed on a commercial acrylic fiber skeleton ($1.55-1.7 kg −1 ) to precisely constrain the polyiodide and enhance the cycling durability of Zn-I 2 batteries. Consequently, a high-rate (1 C-146.1 mAh g −1 , 10 C-133.8 mAh g −1 ) as well as, ultra-stable (2000 cycles at 20 C with 97.24% capacity retention) polymer-based Zn-I 2 battery is reported. These traits are derived from the strong electrostatic interaction generated by quaternization engineering, which significantly eliminates the polyiodide shuttle issue and simultaneously realizes peculiar solution-based iodine chemistry (I − /I 3 − ) in Zn-I 2 batteries. The quaternization strategy also presents high practicability, reliability, and extensibility in various complicated environments. In particular, cutting-edge Zn-I 2 batteries based on the concept of derivative material (commercially available quaternized resin) demonstrate ≈100% capacity retention over 17 000 cycles at 20 C. This work provides a general and fresh insight into the design and development of large-scale, low-cost, and high-performance zinc-iodine batteries, as well as, other novel iodine storage systems.
Size engineering is deemed to be an adoptable method to boost the electrochemical properties of potassium‐ion storage; however, it remains a critical challenge to significantly reduce the nanoparticle size without compromising the uniformity. In this work, a series of MoP nanoparticle splotched nitrogen‐doped carbon nanosheets (MoP@NC) is synthesized. Due to the coordinate and hydrogen bonds in the water‐soluble polyacrylamide hydrogel, MoP is uniformly confined in a 3D porous NC to form ultrafine nanoparticles which facilitate the extreme exposure of abundant three‐phase boundaries (MoP, NC, and electrolyte) for ionic binding and storage. Consequently, MoP@NC‐1 delivers an excellent capacity performance (256.1 mAh g−1 at 0.1 A g−1) and long‐term cycling durability (89.9% capacitance retention after 800 cycles). It is further confirmed via density functional theory calculations that the smaller the MoP nanoparticle, the larger the three‐phase boundary achieved for favoring competitive binding energy toward potassium ions. Finally, MoP@NC‐1 is applied as highly electroactive additive for 3D printing ink to fabricate 3D‐printed potassium‐ion hybrid capacitors, which delivers high gravimetric energy/power density of 69.7 Wh kg−1/2041.6 W kg−1, as well as favorable areal energy/power density of 0.34 mWh cm−2/9.97 mW cm−2.
In this work, few layer graphene quantum dots (GQDs) with a size of 3-5 nm are purposely treated with highly concentrated aqueous NaBH4 solutions to obtain the reduced graphene quantum dots (rGQDs). Fourier transform infrared spectroscopy (FT-IR), X-ray photoelectron spectroscopy (XPS) and Raman spectroscopy demonstrate that the number of carbonyl groups decreases but -OH related defects increase during chemical reduction. Green and weak emissions of original GQDs originate from carrier recombination in the disorder-induced localized state (mainly including carbonyl and carboxyl and epoxy groups). As the reduction degree increases, the photoluminescence (PL) quantum efficiency of GQDs increases dramatically from 2.6% to 10.1%. In the meantime, the PL peak position blue shifts rapidly, and full width at half maximum (FWHM) becomes narrower. Thus we can infer that graphenol topological defects (hydroxyl functionalized graphene) are gradually formed during reduction. Besides, graphenol defect related PL features a longer fluorescence lifetime, excitation wavelength dependence but less pH sensitivity.
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