One-Pot Etching Pyrolysis to Defect-Rich Carbon Nanosheets to Construct Multiheteroatom-Coordinated Iron Sites for Efficient Oxygen Reduction.

Constructing multiheteroatom coordination structure in carbonaceous substrates demonstrates an effective method to accelerate the oxygen reduction reaction (ORR) of supported single-atom catalyst. Herein, the novel etching route assisted by potassium thiocyanate (KCNS) is developed to convert metal-organic framework to 2D defect-rich porous N,S-co-doped carbon nanosheets for anchoring atomically dispersed iron sites as the high-performance ORR catalysts (Fe-SACs). The well-designed KCNS-assisted etching route can generate spatial confinement template to direct the carbon nanosheet formation, etching condition to form defect-rich structure, and additional sulfur atoms to coordinate iron species. Spectral and microscopy analysis reveals that the iron element in Fe-SACs is highly isolated on carbon nanosheet and anchored by nitrogen and sulfur atoms in unsymmetrical Fe-S1N3 structure. The optimized Fe-SACs with large specific surface area could show remarkable alkaline ORR performances with a high half-wave potential of 0.920 V versus RHE and excellent durability. The rechargeable zinc-air battery assembled with Fe-SACs air electrodes delivers a large power density of 350 mW cm-2 and a stable voltage platform during charge and discharge over more than 1300 h. This work proposes a novel strategy for the preparation of single-atom catalysts with multiheteroatom coordination structure and highly exposed active sites for efficient ORR.

Hydrophilic Poly(vinylidene Fluoride) Film with Enhanced Inner Channels for Both Water- and Ionic Liquid-Driven Ion-Exchange Polymer Metal Composite Actuators.

This study presents a novel and facile strategy to fabricate a hydrophilic poly(vinylidene fluoride) (PVDF) electrolyte film with enhanced inner channels for a high-performance and cost-effective ion-exchange polymer metal composite (IPMC) actuator. The resultant PVDF composite film is composed of hierarchical micro/nanoscale structures: well-defined polymer grains with a diameter of ∼20 µm and much finer particles with a diameter of ∼390 nm, producing three-dimensional interconnected, hierarchical inner channels to facilitate ion migration of IPMC. Interestingly, the electrolyte matrix film has a high porosity of 15.8% and yields a high water uptake of 44.2% and an ionic liquid (IL, [EMIm]·[BF4]) uptake of 38.1% to make both water-driven and IL-driven IPMC actuators because of the introduction of polar polyvinyl pyrrolidone. Compared to the conventional PVDF/IL-based IPMC, both water-driven and IL-driven PVDF-based IPMCs exhibit high ion migration rates, thus effectively improving the actuation frequency and producing remarkably higher levels of actuation force and displacement. Specifically, the force outputs are increased by 13.4 and 3.0 folds, and the displacement outputs are increased by 2.2 and 1.9 folds. Using an identical electrolyte matrix, water-driven IPMC exhibits stronger electromechanical performance, benefiting to make IPMC actuator with high levels of force and power outputs, whereas IL-driven IPMC exhibits a more stable electromechanical performance, benefiting to make long lifetime IPMC actuator in air. Thus, the resultant IPMCs are promising in the design of artificial muscles with tunable electromechanical performance for flexible actuators or displacement/vibration sensors at low cost.

Sulfonic SiO2 nanocolloid doped perfluorosulfonic acid films with enhanced water uptake and inner channel for IPMC actuators.

This study provides a facile and effective strategy to fabricate sulfonic SiO2 nanocolloid (HSO3-SiO2) doped perfluorosulfonic acid (PFSA) films with enhanced water uptake and inner channel for high-performance and cost-effective ionic exchange polymer metal composite (IPMC) actuators. A commercial precursor of mercaptopropyl trimethoxysilane was hydrolyzed to form thiol functionalized SiO2 nanocolloids (SH-SiO2, ∼25 nm in diameter), which were further oxidized into sulfonic SiO2 nanocolloids (HSO3-SiO2, ∼14 nm in diameter). Both SiO2 nanocolloids were used as additives to dope PFSA film for fabricating IPMC-used matrix films. Due to difference of compatibility, the SH-SiO2 nanocolloids take phase separation in the cocrystallization course, and aggregate into huge, regular spherical particles with a mean diameter of ∼690 µm; while the HSO3-SiO2 nanocolloids are completely compatible with PFSA, forming a very homogeneous hybrid matrix film. Related physiochemical investigations by analytical tools revealed that, the resultant HSO3-SiO2 hybrid film shows better IPMC-related properties compared to the SH-SiO2 hybrid film: 1.59 folds in water uptake, and 2.37 folds in ion exchanging capacity, thus contains an increased number of cations and possesses larger and better interconnected inner channels for IPMC bending. Consequently, the HSO3-SiO2 hybrid IPMC actuator exhibits remarkably higher levels of actuation behaviours such as higher force output, higher displacement output, and longer stable working time, which could be used as a valuable artificial muscle for flexible actuators or displacement/vibration sensors at low cost.