A Mixed Protonic-Electronic Conductor Base on the Host-Guest Architecture of 2D Metal-Organic Layers and Inorganic Layers.

The key to designing and fabricating highly efficient mixed protonic-electronic conductors materials (MPECs) is to integrate the mixed conductive active sites into a single structure, to break through the shortcomings of traditional physical blending. Herein, based on the host-guest interaction, an MPEC is consisted of 2D metal-organic layers and hydrogen-bonded inorganic layers by the assembly methods of layered intercalation. Noticeably, the 2D intercalated materials (≈1.3 nm) exhibit the proton conductivity and electron conductivity, which are 2.02 × 10-5 and 3.84 × 10-4 S cm-1 at 100 °C and 99% relative humidity, much higher than these of pure 2D metal-organic layers (>>1.0 × 10-10 and 2.01×10-8 S cm-1 ), respectively. Furthermore, combining accurate structural information and theoretical calculations reveals that the inserted hydrogen-bonded inorganic layers provide the proton source and a networks of hydrogen-bonds leading to efficient proton transport, meanwhile reducing the bandgap of hybrid architecture and increasing the band electron delocalization of the metal-organic layer to greatly elevate the electron transport of intrinsic 2D metal-organic frameworks.

Enhancing the activity of metal-organic nanosheets for oxygen evolution reaction by substituent effects.

Rational designing and synthesizing highly efficient oxygen evolution reaction (OER) electrocatalyst plays a key role in energy conversion. However, due to the numerous factors affecting the activity of electrocatalysis, the understanding of their catalytic mechanism is insufficient, and challenges still exist. Herein, the organic group of the metal-organic nanosheets electrocatalyst was replaced by NH2 to CH3 to controllable regulate the catalytic performance of OER, corresponding to the overpotential of OER reducing from 385 mV to 318 mV at 10 mA cm-2, superior to the commercial precious metal based catalyst RuO2. Furthermore, combining the density functional theory (DFT) and electron localization function (ELF) indicates that the type of ligands group can indirectly modulate the electronic structure of metal catalytic center and the degree of electronic localization of the metal-organic nanosheets catalysts, resulting in the change in electrocatalytic activity. This simple catalytic model is more favorable to investigate the catalytic mechanism, providing a new strategy for the development of efficient electrocatalyst.

High ionic conduction, toughness and self-healing poly(ionic liquid)-based electrolytes enabled by synergy between flexible units and counteranions.

Polymer electrolytes offer great potential for emerging wearable electronics. However, the development of a polymer electrolyte that has high ionic conductivity, stretchability and security simultaneously is still a considerable challenge. Herein, we reported an effective approach for fabricating high-performance poly(ionic liquids) (PILs) copolymer (denoted as PIL-BA) electrolytes by the interaction between flexible units (butyl acrylate) and counteranions. The introduction of butyl acrylate units and bis(trifluoromethane-sulfonyl)imide (TFSI-) counteranions can significantly enhance the mobility of polymer chains, resulting in the effective improvement of ion transport, toughness and self-healability. As a result, the PIL-BA copolymer-based electrolytes containing TFSI- counterions achieved the highest ionic conductivity of 2.71 ± 0.17 mS cm-1, 1129% of that of a PIL homopolymer electrolyte containing Cl- counterions. Moreover, the PIL-BA copolymer-based electrolytes also exhibit ultrahigh tensile strain of 1762% and good self-healable capability. Such multifunctional polymer electrolytes can potentially be applied for safe and stable wearable electronics.