Lithium–sulfur batteries (LSBs) can work at high temperatures, but they suffer from poor cycle life stability due to the “shuttle effect” of polysulfides. In this study, pollen‐derived porous carbon/cuprous phosphide (PC/Cu3P) hybrids were rationally synthesized using a one‐step carbonization method using pollen as the source material, acting as the sulfur host for LSBs. In the hybrid, polar Cu3P can markedly inhibit the “shuttle effect” by regulating the adsorption ability toward polysulfides, as confirmed by theoretical calculations and experimental tests. As an example, the camellia pollen porous carbon (CPC)/Cu3P/S electrode shows a high capacity of 1205.6 mAh g−1 at 0.1 C, an ultralow capacity decay rate of 0.038% per cycle after 1000 cycles at 1 C, and a rather high initial Coulombic efficiency of 98.5%. The CPC/Cu3P LSBs can work well at high temperatures, having a high capacity of 545.9 mAh g−1 at 1 C even at 150°C. The strategy of the PC/Cu3P hybrid proposed in this study is expected to be an ideal cathode for ultrastable high‐temperature LSBs. We believe that this strategy is universal and worthy of in‐depth development for the next generation energy storage devices.
High internal phase emulsion (HIPE) living polymerization was proposed in current work. Reversible addition-fragmentation chain transfer polymerization (RAFT), one of the living radical polymerization methods, was introduced to the polymerization of HIPE for the preparation of polystyrene PolyHIPEs. Living polymerization changed the crosslinking process giving a highly homogeneous polymeric wall of PolyHIPEs. The resolving of the heterogeneity problem increased the mechanical strength of PolyHIPEs significantly with the Young's modulus reaching the theoretical value of ∼45 MPa, which was more than 3 times higher than that by the conventional method. Not only the open-cellular structure of PolyHIPEs was maintained but also a higher connectivity was achieved. Both the type and the concentration of RAFT agents were found to have influence on the morphology and mechanical strength of PolyHIPEs.
A many-shot RAFT emulsion polymerization method is proposed to synthesize gradient copolymers with high molecular weight and a tailor-made compositional gradient. In this method each shot consisting of comonomers with pre-set different fractions and targeting the molecular weight of 10 000 g mol−1 was added in a stepwise manner during the reaction. High conversions over 95% were achieved in 35 min after each shot. The compositional variation along the polymer chain was then directly determined by the comonomer fractions added at each shot. Styrene/n-butyl acrylate gradient copolymers (including linear and V-shaped gradient) with molecular weights as high as 90 000 g mol−1 were prepared by this method. The composition profiles along the polymer chains agreed well with the theoretical predictions, and the composition distribution among the polymer chains was narrow. The gradient copolymers showed different thermal and phase separation properties from their block counterparts, as expected. These results demonstrated the successful tailor-making of the gradient copolymers. The current strategy will act as a facile method to prepare tailor-made gradient copolymers with high molecular weights and within a short time.
Soft biological tissues and muscles composed of semiflexible networks exhibit rapid strain-hardening behaviors to protect them from accidental rupture. In contrast, synthetic soft elastomers, usually featuring flexible networks, lack such behaviors, leading to a notorious issue when applying them to a promising artificial muscle technology (dielectric elastomer, DE), that is electromechanical instability (EMI) induced premature breakdown. We report that a facile thermomechanical training method can adaptively reconstruct the network of a soft triblock copolymer elastomer to transform its flexible network strands into semiflexible ones without extra chemical modifications and additives so that the electro-actuation performance is significantly enhanced by avoiding EMI. The free-standing actuators of trained elastomers exhibit a large stable electro-actuation strain and a high theoretical energy density (133%, 307 kJ m−3 at 158.1 V μm−1), and the capacity of actuating at low-temperature environments (−15 °C).