A heterojunction material involving highly crystalline carbon nitride nanorods with ordered alignment on graphene is successfully synthesized, and it shows a comparably high selectivity of CO 2 /N 2 up to 44, with an isosteric heat of adsorption of 55.2 kJ/mol for CO 2. This material also shows remarkable improvements of light absorption, exciton splitting, and charge transport, which enables the efficient photochemical reduction of wet CO 2 in the gas phase and without any sacrificial agent.
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.
Rechargeable aqueous zinc‐iodine batteries (ZIBs) are considered a promising newly‐developing energy‐storage system, but the corrosion and dendritic growth occurring on the anode seriously hinder their future application. Here, the corrosion mechanism of polyiodide is revealed in detail, showing that it can spontaneously react with zinc and cause rapid battery failure. To address this issue, a sulfonate‐rich ion‐exchange layer (SC‐PSS) is purposely constructed to modulate the transport and reaction chemistry of polyiodide and Zn2+ at the zinc/electrolyte interface. The resulting ZIBs can work properly over 6000 cycles with high‐capacity retention (90.2%) and reversibility (99.89%). Theoretical calculations and experimental characterization reveal that the SC‐PPS layer blocks polyiodide permeation through electrostatic repulsion, while facilitating desolvation of Zn(H2O)62+ and restricting undesirable 2D diffusion of Zn2+ by chemisorption.
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