Pore Environment Control and Enhanced Performance of Enzymes Infiltrated in Covalent Organic FrameworksQi Sun, Chung‐Wei Fu, Briana Aguila et al.|Journal of the American Chemical Society|2017 In the drive toward green and sustainable methodologies for chemicals manufacturing, biocatalysts are predicted to have much to offer in the years to come. That being said, their practical applications are often hampered by a lack of long-term operational stability, limited operating range, and a low recyclability for the enzymes utilized. Herein, we show how covalent organic frameworks (COFs) possess all the necessary requirements needed to serve as ideal host materials for enzymes. The resultant biocomposites of this study have shown the ability boost the stability and robustness of the enzyme in question, namely lipase PS, while also displaying activities far outperforming the free enzyme and biocomposites made from other types of porous materials, such as mesoporous silica and metal-organic frameworks, exemplified in the kinetic resolution of the alcohol assays performed. The ability to easily tune the pore environment of a COF using monomers bearing specific functional groups can improve its compatibility with a given enzyme. As a result, the orientation of the enzyme active site can be modulated through designed interactions between both components, thus improving the enzymatic activity of the biocomposites. Moreover, in comparison with their amorphous analogues, the well-defined COF pore channels not only make the accommodated enzymes more accessible to the reagents but also serve as stronger shields to safeguard the enzymes from deactivation, as evidenced by superior activities and tolerance to harsh environments. The amenability of COFs, along with our increasing understanding of the design rules for stabilizing enzymes in an accessible fashion, gives great promise for providing "off the shelf" biocatalysts for synthetic transformations.
Lightweight Polypropylene/Stainless-Steel Fiber Composite Foams with Low Percolation for Efficient Electromagnetic Interference ShieldingA. Ameli, Mohammadreza Nofar, Sai Wang et al.|ACS Applied Materials & Interfaces|2014 Lightweight polypropylene/stainless-steel fiber (PP-SSF) composites with 15-35% density reduction were fabricated using foam injection molding. The electrical percolation threshold, through-plane electrical conductivity, and electromagnetic interference (EMI) shielding effectiveness (SE) of the PP-SSF composite foams were characterized and compared against the solid counterparts. With 3 wt % CO2 dissolved in PP as a temporary plasticizer and lubricant, the fiber breakage was significantly decreased during injection molding, and well-dispersed fibers with unprecedentedly large aspect ratios of over 100 were achieved. The percolation threshold was dramatically decreased from 0.85 to 0.21 vol %, accounting for 75% reduction, which is highly superior, compared to 28% reduction of the previous PP-carbon fiber composite foam.1 Unlike the case of carbon fiber,1 SSFs were much longer than the cell size, and the percolation threshold reduction of PP-SSF composite foams was thus primarily governed by the decreased fiber breakage instead of fiber orientation. The specific EMI SE was also significantly enhanced. A maximum specific EMI SE of 75 dB·g(-1)·cm(3) was achieved in PP-1.1 vol % SSF composite foams, which was much higher than that of the solid counterpart. Also, the relationships between the microstructure and properties were discussed. The mechanism of EMI shielding enhancement was also studied.
Fabrication of Circularly Polarized MR‐TADF Emitters with Asymmetrical Peripheral‐Lock Enhancing Helical B/N‐Doped NanographenesXiugang Wu, Jingwei Huang, Bo‐Kang Su et al.|Advanced Materials|2021 Abstract Circularly polarized thermally activated delayed fluorescence (CP‐TADF) and multiple‐resonance thermally activated delayed fluorescence (MR‐TADF), which exhibit novel circularly polarized luminescence and excellent color fidelity, respectively, have gained immense popularity. In this study, integrated CP‐TADF and MR‐TADF (CPMR‐TADF) are prepared by strategic design and synthesis of asymmetrical peripherally locked enantiomers, which are separated and denoted as ( P , P ″, P ″)‐/( M , M ″, M ″)‐ BN4 and ( P , P ″, P ″)‐/( M , M ″, M ″)‐ BN5 and exhibit TADF and circularly polarized light (CPL) properties. As the entire molecular frame participates in the frontier molecular orbitals, the resulting helical chirality of (+)/(−)‐ BN4 ‐ and (+)/(−)‐ BN5 ‐based solution‐processed organic light‐emitting diodes (OLEDs) helps in achieving a narrow full width at half maximum (FWHM) of 49/49 and 48/48 nm and a high maximum external quantum efficiency (EQE) of 20.6%/19.0% and 22.0%/26.5%, respectively. Importantly, unambiguous circularly polarized electroluminescence signals with dissymmetry factors ( g EL ) of +3.7 × 10 −3 /−3.1 × 10 −3 ( BN4 ) and +1.9 × 10 −3 /−1.6 × 10 −3 ( BN5 ) are obtained. The results indicate successful exploitation of CPMR‐TADF‐emitter‐based OLEDs to exhibit three characteristics: high efficiency, color purity, and circularly polarized light.
Transformation of Rusty Stainless‐Steel Meshes into Stable, Low‐Cost, and Binder‐Free Cathodes for High‐Performance Potassium‐Ion BatteriesYunhai Zhu, Yanbin Yin, Xu Yang et al.|Angewandte Chemie International Edition|2017 Abstract To recycle rusty stainless‐steel meshes (RSSM) and meet the urgent requirement of developing high‐performance cathodes for potassium‐ion batteries (KIB), we demonstrate a new strategy to fabricate flexible binder‐free KIB electrodes via transformation of the corrosion layer of RSSM into compact stack‐layers of Prussian blue (PB) nanocubes (PB@SSM). When further coated with reduced graphite oxide (RGO) to enhance electric conductivity and structural stability, the low‐cost, stable, and binder‐free RGO@PB@SSM cathode exhibits excellent electrochemical performances for KIB, including high capacity (96.8 mAh g −1 ), high discharge voltage (3.3 V), high rate capability (1000 mA g −1 ; 42 % capacity retention), and outstanding cycle stability (305 cycles; 75.1 % capacity retention).
Warm/cool-tone switchable thermochromic material for smart windows by orthogonally integrating properties of pillar[6]arene and ferroceneSai Wang, Zuqiang Xu, Tingting Wang et al.|Nature Communications|2018 Functional materials play a vital role in the fabrication of smart windows, which can provide a more comfortable indoor environment for humans to enjoy a better lifestyle. Traditional materials for smart windows tend to possess only a single functionality with the purpose of regulating the input of solar energy. However, different color tones also have great influences on human emotions. Herein, a strategy for orthogonal integration of different properties is proposed, namely the thermo-responsiveness of ethylene glycol-modified pillar[6]arene (EGP6) and the redox-induced reversible color switching of ferrocene/ferrocenium groups are orthogonally integrated into one system. This gives rise to a material with cooperative and non-interfering dual functions, featuring both thermochromism and warm/cool tone-switchability. Consequently, the obtained bifunctional material for fabricating smart windows can not only regulate the input of solar energy but also can provide a more comfortable color tone to improve the feelings and emotions of people in indoor environments.