Summary
Easy regenerability of core components such as electrode and electrolyte is highly required in advanced electrochemical devices. This work reports a reliable, regenerable, and stretchable hydrogel electrolyte based on ionic bonds between polyacrylic acid (PAA) and polyallylamine (PAH). PAA-PAH electrolyte (1M LiCl addition) exhibits high ionic conductivity (0.050 S·cm-1) and excellent mechanical property (fracture strain of 1,688%). Notably, the electrolyte can be regenerated to any desired shape under mild conditions and remains 96% and 90% of the initial ionic conductivity after the first and second regeneration, respectively. PAA-PAH/LiCl-based supercapacitor exhibits nearly 100% capacitance retention upon rolling, stretching, and 5,000 charge-discharge cycles, whereas the regenerated device holds 97.6% capacitance of the initial device and 90.9% after 5,000 cycles. This low-cost, high-efficiency, and regenerable hydrogel electrolyte reveals very promising use in solid-state/flexible supercapacitors and possibly becomes a standard commercial hydrogel electrolyte for sustainable electrochemical energy devices.
Catalytic ozone (O3) decomposition at high relative humidity (RH) remains a great challenge due to the catalysts poison and deactivation under high humidity. Here, we firstly elaborate the role of water activation and the corresponding mechanism of the promoted O3 decomposition over the three‐dimensional monolithic molybdenum oxide/graphdiyne (MoO3/GDY) catalyst. The O3 decomposition over MoO3/GDY reaches up to 100% under high humid condition (75% RH) at room temperature, which is 4.0 times as high as that of dry conditions, significantly surpasses other carbon‐based MoO3 materials(≤ 7.1%). The sp‐hybridized carbon in GDY donates electrons to MoO3 along the C‐O‐Mo bond, facilitating water activation to form hydroxyl species. As a result, hydroxyl species dissociated from water act as new active sites, promoting the adsorption of O3 and the generation of new intermediate species (hydroxyl ⋅OH and superoxo ⋅O2−), which significantly lowers the energy barriers of O3 decomposition (0.57 eV lower than dry conditions).
The identification of the decay pathway of the nucleobase uracil after being photoexcited by ultraviolet light has been a long-standing problem. Various theoretical models have been proposed but yet to be verified. Here, we propose an experimental scheme to test the theoretical models of gas phase uracil decay mechanism by a combination of ultrafast x-ray spectroscopy, x-ray diffraction, and electron diffraction methods. Incorporating the signatures of multiple probing methods, we demonstrate an approach that can identify the dominant mechanism of the geometric and electronic relaxation of the photoexcited uracil molecule among several candidate models.
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