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Three-dimensional (3D) nanostructured conducting polymer hydrogels represent a group of highperformance electrochemical energy-storage materials. Here, we demonstrate a molecular self-assembly approach toward controlled synthesis of nanostructured polypyrrole (PPy) conducting hydrogels, which was "cross-linked" by a conjugated dopant molecule trypan blue (TB) to form a 3D network with controlled morphology. The protonated TB by ion bonding aligns the free sulfonic acid groups into a certain spatial structure. The sulfonic acid group and the PPy chain are arranged by a self-sorting mechanism to form a PPy nanofiber structure by electrostatic interaction and hydrogen bonding. It is found that PPy hydrogels doped with varying dopant concentrations and changing dopant molecules exhibited controllable morphology and tunable electrochemical properties. In addition, the conjugated TB dopants promoted interchain charge transport, resulting in higher electrical conductivity (3.3 S/ cm) and pseudocapacitance for the TB-doped PPy, compared with PPy synthesized without TB. When used as supercapacitor electrodes, the TB-doped PPy hydrogel reaches maximal specific capacitance of 649 F/g at the current density 1 A/g. The result shows that PPy nanostructured hydrogels can be tuned for potential applications in next-generation energy-storage materials.

Imine-linked covalent organic frameworks (COFs) have received widespread attention because of their structure features such as high crystallinity and tunable pores. However, the intrinsic reversibility of the imine bond leads to the poor stability of imine-linked COFs under strong acid conditions. Also, their thermal stability is significantly lower than that of many other COFs. Herein, we report for the first time that the reversible imine bonds in the skeleton of COFs can be locked through the asymmetric hydrophosphonylation reaction of phosphite. The functionalized COFs not only retain the crystallinity and porous structure but also exhibit evidently improved chemical and thermal stabilities. In addition, the phosphorous acid groups generated by acidic hydrolysis attached to the skeleton endow the COFs with good intrinsic proton conductivity. Due to the diversity of phosphite derivatives and imine-linked COFs, this work may provide an avenue for extending the COF structures and functions through the asymmetric hydrophosphonylation reaction.

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The use of non-metal charge carriers such as ammonium (NH 4 + ) in electrochemical energy storage devices offers advantages in terms of weight, element abundance, and compatibility with aqueous electrolytes. However, the development of suitable electrodes for such carriers lags behind other technologies. Herein, we present a high-performance anode material for ammonium-ion supercapacitors based on a MoO 3 /carbon (MoO 3 @C) composite. The NH 4 + storage performance of such composites and their practical application prospects are evaluated both in a three-electrode configuration and as symmetric supercapacitors. The optimized material reaches an unprecedented specific capacitance of 473 F·g −1 (158 mAh·g −1 ; 1592 mF·cm −2 ) at a current density of 1 A·g −1 , and 92.7% capacitance retention after 5000 cycles in a three-electrode set-up. This outstanding performance is related to the presence of oxygen vacancies that enhance the composites' ionic/ electronic transportation and electrochemical reaction site, while at the same time facilitating the formation of hydrogen bonds between NH 4 + and the host material. Using the optimized composite, symmetric supercapacitors based on an (NH 4 ) 2 SO 4 gel electrolyte are fabricated and demonstrated to provide unmatched energy densities above 78 Wh·kg −1 at a power density of 929 W·kg −1 . Besides, such devices are characterized by extraordinary capacitance retention of 97.6% after 10,000 cycles.

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