The efficient use of renewable X/γ-rays or accelerated electrons for chemical transformation of CO2 and water to fuels holds promise for a carbon-neutral economy; however, such processes are challenging to implement and require the assistance of catalysts capable of sensitizing secondary electron scattering and providing active metal sites to bind intermediates. Here we show atomic Cu-Ni dual-metal sites embedded in a metal-organic framework enable efficient and selective CH3OH production (~98%) over multiple irradiated cycles. The usage of practical electron-beam irradiation (200 keV; 40 kGy min−1) with a cost-effective hydroxyl radical scavenger promotes CH3OH production rate to 0.27 mmol g−1 min−1. Moreover, time-resolved experiments with calculations reveal the direct generation of CO2•‒ radical anions via aqueous electrons attachment occurred on nanosecond timescale, and cascade hydrogenation steps. Our study highlights a radiolytic route to produce CH3OH with CO2 feedstock and introduces a desirable atomic structure to improve performance.
Rewritable papers, as environmentally friendly alternatives for information delivery, hold great promise to reduce the abundant use of ordinary papers that cause severe environmental problems. In recent decades, photonic crystals (PCs) have shown great potential in developing rewritable papers. However, existing PC papers still confront many challenges, including poor storage stability, short-cycle lifetime, monotonous colors, and absence of copying capability. Herein, we report the fabrication of a rewritable PC paper based on programmable configurations of a synthesized shape memory polymer (SMP). The resulting SMP-based PC paper does not need additional inks and can be facilely used to write by the near- infrared (NIR) light with assistance from a pre-printed black paper as a photothermal layer. Heating from the black paper induces various stable configurations of the PCs, thus creating multiple colors in the irradiated areas. Moreover, the PC paper possesses excellent colorful copying capability that can transform information from a paper with pre-printed black letters or complex images via scanning with NIR light. These images can be stably stored for more than 6 months at ambient conditions, which can be even erased and rewritten over 50 times without significant loss in color quality. This environment-friendly SMP-based PC paper with extraordinary properties holds great promise in the fields of next-generation office papers, smart price tags, and anti-counterfeiting labels.
Robust hydrogels offer a candidate for artificial skin of bionic robots, yet few hydrogels have a comprehensive performance comparable to real human skin. Here, we present a general method to convert traditional elastomers into tough hydrogels via a unique radiation-induced penetrating polymerization method. The hydrogel is composed of the original hydrophobic crosslinking network from elastomers and grafted hydrophilic chains, which act as elastic collagen fibers and water-rich substances. Therefore, it successfully combines the advantages of both elastomers and hydrogels and provides similar Young’s modulus and friction coefficients to human skin, as well as better compression and puncture load capacities than double network and polyampholyte hydrogels. Additionally, responsive abilities can be introduced during the preparation process, granting the hybrid hydrogels shape adaptability. With these unique properties, the hybrid hydrogel can be a candidate for artificial skin, fluid flow controller, wound dressing layer and many other bionic application scenarios.
20 August 2018 in Journal of Materials Chemistry A
Microarrays have attracted great interest due to their widespread applications in anti-icing, cell manipulation, and antibioadhesion. However, such arrays are typically fabricated with high-cost and time-consuming lithography techniques. Various kinds of new polymers have been developed to solve this problem. Nevertheless, most of the microarrays fabricated with these materials are usually static, lacking sufficient intelligence and therefore hindering their practical applications. Here, a new strategy is reported that introduces shape memory polymer (SMP) into microarray fabrication. The deformation and recovery of SMP microarrays was investigated, and they show robust controllability and stable surface wettability, as well as a high shape recovery ratio (∼91%) at microscale, even after more than ten cycles of “stretch-recovery” process. In addition, various microarrays with a series of continuously changeable microscales were replicated by using the patterned SMP film as a tunable mold. Specifically, the SMP mold not only shows excellent ability to replicate multiple microarrays with controlled and ordered microstructures via one specific SMP mold, but it also can be applied to various polymers with more than ten replicas. This universal strategy paves an avenue for the broad applications of SMP arrays in cell manipulation, water droplet manipulation and smart dry adhesives.
26 June 2018 in ACS Applied Materials & Interfaces