bluuebunny/crossref_metadata_2025_split huggingface dataset:
Bacteria‐Responsive Self‐Assembly of Antimicrobial Peptide Nanonets for Trap‐and‐Kill of Antibiotic‐Resistant Strains
Authors: Tram Nhan Dai Thien , Xu Jian , Mukherjee Devika , Obanel Antonio Eduardo , Mayandi Venkatesh , Selvarajan Vanitha , Zhu Xiao , Teo Jeanette , Barathi Veluchamy Amutha , Lakshminarayanan Rajamani , Ee Pui Lai Rachel 
Published: November 2022

AbstractBacterial trapping using nanonets is a ubiquitous immune defense mechanism against infectious microbes. These nanonets can entrap microbial cells, effectively arresting their dissemination and rendering them more vulnerable to locally secreted microbicides. Inspired by this evolutionarily conserved anti‐infective strategy, a series of 15 to 16 residue‐long synthetic β‐hairpin peptides is herein constructed with the ability to self‐assemble into nanonets in response to the presence of bacteria, enabling spatiotemporal control over microbial killing. Using amyloid‐specific K114 assay and confocal microscopy, the membrane components lipoteichoic acid and lipopolysaccharide are shown to play a major role in determining the amyloid‐nucleating capacity as triggered by Gram‐positive and Gram‐negative bacteria respectively. These nanonets displayed both trapping and killing functionalities, hence offering a direct improvement from the trap‐only biomimetics in literature. By substituting a single turn residue of the non‐amyloidogenic BTT1 peptide, the nanonet‐forming BTT1‐3A analog is produced with comparable antimicrobial potency. With the same sequence manipulation approach, BTT2‐4A analog modified from BTT2 peptide showed improved antimicrobial potency against colistin‐resistant clinical isolates. The peptide nanonets also demonstrated robust stability against proteolytic degradation, and promising in vivo efficacy and biosafety profile. Overall, these bacteria‐responsive peptide nanonets are promising clinical anti‐infective alternatives for circumventing antibiotic resistance.
Ultra‐Thin Single‐Particle‐Layer Sodium Beta‐Alumina‐Based Composite Polymer Electrolyte Membrane for Sodium‐Metal Batteries
Authors: Fang Ruyi , Li Yutao , Wu Nan , Xu Biyi , Liu Yijie , Manthiram Arumugam , Goodenough John B. 
Published: November 2022

AbstractInorganic/organic composite polymer electrolytes (CPEs) with good flexibility and electrode contact have been pursued for solid−state sodium‐metal batteries. However, the application of CPEs for high energy density solid−state sodium‐metal batteries is still limited by the low Na+ conductivity, large thickness, and low ion transference number. Herein, an ultra‐thin single‐particle‐layer (UTSPL) composite polymer electrolyte membrane with a thickness of ≈20 µm straddled by a sodium beta−alumina ceramic electrolyte (SBACE) is presented. A ceramic Na+‐ion electrolyte that bridges or percolates across an ultra‐thin and flexible polymer membrane provides: 1) the strength and flexibility from the polymer membrane, 2) excellent electrolyte/electrode interfacial contact, and 3) a percolation path for Na+‐ion transfer. Owing to this novel design, the obtained UTSPL‐35SBACE membrane exhibits a high Na+‐ion conductivity of 0.19 mS cm−1 and a transference number of 0.91 at room temperature, contributing to long−term cycling stability of symmetric sodium cells with a small overpotential. The assembled quasi‐solid‐state cell with the as−prepared UTSPL‐35SBACE membrane displays superior cycling performance with a discharge capacity of 105 mAh g−1 at 0.5 °C rate after 100 cycles and excellent rate performance (82 mAh g−1 at 5 °C rate) at room temperature with the potassium manganese hexacyanoferrate (KMHCF)@CNTs/CNFs cathode, where KMHCF refers to potassium manganese hexacyanoferrate.
New Phthalic Anhydride‐Based Room‐Temperature Phosphorescence Emitter with Lifetime Longer Than One Second
Authors: Yin Zheng , Sun Qi , Chen Liangliang , Du Mingxu , Huang Yan‐Ying , Peng Qian , Zhang Guanxin , Zhang Deqing 
Published: November 2022

AbstractOrganic room‐temperature phosphorescence (RTP) materials have attracted much attention in recent years due to their potential applications. However, the development of organic RTP emitters with a long lifetime and high quantum yield remains a great challenge owing to the weak molecular spin–orbit coupling and high sensitivity to oxygen. In this paper, a new purely organic RTP emitter, 3,3″,4,4″‐diphenylsulfonetetracarboxylic dianhydride (DPS), is reported which shows an excitingly ultralong lifetime up to 1.08 s and high phosphorescence quantum yield of 8%. When anhydride units in DPS are transformed into imides, the RTP performance in terms of lifetime and quantum yield is decreased. The presence of multiple intermolecular interactions is favorable for the restriction of nonradiative decay and the promotion of spin–orbit coupling, which is further corroborated by theoretical calculations. The studies demonstrate that DPS is a promising structural motif for developing high‐performance organic RTP emitters.
Transient Response Mismatch: A Limiting Factor of Perovskite Photodetectors
Authors: Ai Zhenhai , Ma Tianshu , An Yidan , Wang Changlei , Cao Guoyang , Ma Dong , Li Xiaofeng 
Published: November 2022

AbstractDue to the excellent optoelectronic performance, perovskite photodetectors (PDs) have attracted a lot of attention in recent years. However, the response speed of such a device is still relatively low. To overcome this defect, the intrinsic mechanisms within the perovskite PDs have to be uncovered. Here a comprehensive optoelectronic simulation is implemented to examine the transient response of the perovskite PDs, where the dynamics of both carriers (electrons/hoes) and ions (anions/cations) are taken into account. The unmatched temporal responses between the photogenerated electrons and holes are found to severely limit the overall response speed. Unfortunately, solely manipulating the perovskite parameters (e.g., thickness, doping concentration, and ion migration) cannot effectively suppress such a detrimental effect. Further study indicates that the mismatch in temporal response originates from the different electrical properties of the opposite charge transport layers, and can only be alleviated by balancing the corresponding carrier extraction capabilities. A roadmap for improving the response speed of the perovskite PDs is finally proposed, which shows the greatly shortened response time from 118.21 to 7.45 ns.
Axial N Ligand‐Modulated Ultrahigh Activity and Selectivity Hyperoxide Activation over Single‐Atoms Nanozymes
Authors: Zhang Han‐Chao , Cui Pei‐Xin , Xie Dong‐Hua , Wang Yu‐Jun , Wang Peng , Sheng Guo‐Ping 
Published: November 2022

AbstractLearning and studying the structure–activity relationship in the bio‐enzymes is conducive to the design of nanozymes for energy and environmental application. Herein, Fe single‐atom nanozymes (Fe‐SANs) with Fe–N5 site, inspired by the structure of cytochromes P450 (CYPs), are developed and characterized. Similar to the CYPs, the hyperoxide can activate the Fe(III) center of Fe‐SANs to generate Fe(IV)O intermediately, which can transfer oxygen to the substrate with ultrafast speed. Particularly, using the peroxymonosulfate (PMS)‐activated Fe‐SANs to oxidize sulfamethoxazole, a typical antibiotic contaminant, as the model hyperoxides activation reaction, the excellent activity within 284 min−1 g−1(catalyst) mmol−1(PMS) oxidation rate and 91.6% selectivity to the Fe(IV)O intermediate oxidation are demonstrated. More importantly, instead of promoting PMS adsorption, the axial N ligand modulates the electron structure of FeN5 SANs for the lower reaction energy barrier and promotes electron transfer to PMS to produce Fe(IV)O intermediate with high selectivity. The highlight of the axial N coordination in the nanozymes in this work provides deep insight to guide the design and development of nanozymes nearly to the bio‐enzyme with excellent activity and selectivity.
Superimposed mosaicism in cutaneous sarcoidosis: A hypothesis
Authors: Happle Rudolf , Wetzke Martin 
Published: November 2022

AbstractSarcoidosis is a chronic granulomatous disorder affecting the lungs, skin, and many other organs. Twin studies suggest that genetic factors account, to a large degree, for the etiology of the disorder. Hence, theoretically, we could postulate that the phenomenon of superimposed mosaicism in the form of a pronounced segmental involvement, overlaying the disseminated non‐segmental lesions, should also occur in sarcoidosis. Indeed, one case suggesting superimposed mosaicism in cutaneous sarcoidosis was found in the literature and is reassessed here.
The impact of vitamin D deficiency on cortical bone area and porosity at the femoral midsection in children from post‐medieval London
Authors: Swan Karen R. , Humphrey Louise T. , Ives Rachel 
Published: November 2022

AbstractObjectivesCortical bone structure undergoes dynamic changes during appositional growth and is highly sensitive to mechanical, hormonal, and nutritional influences. Vitamin D deficiency rickets can significantly disrupt the normal mineralization of newly formed bone leading to compromised bone structure. Here, we document ontogenetic trends in femoral cortical bone area and porosity during early growth and examine how vitamin D deficiency during childhood may impact these parameters in a sample of children from post‐medieval London, UK.Materials and MethodsMicro‐CT scans of the femur were collected from a documented sample of 138 children aged from birth to 8.5 years who were grouped by the presence and stage of rickets. Cross‐sections were extracted at the midsection and area and porosity measurements recorded. A local regression (LOESS) was used to fit curves to the dataset of children without rickets, which were used as comparative baselines for children with active and healed rickets.ResultsCortical bone porosity was elevated in all children with active rickets most likely reflecting delayed mineralization of osteoid and increased resorption due to secondary hyperparathyroidism. Total subperiosteal area and cortical bone area were higher in children with healed rickets than children without rickets reflecting the mineralization of osteoid following recovery from the deficiency.DiscussionThe results demonstrate marked differences in cortical bone structure in children with rickets, which vary according to age and disease stage. This study illustrates the complex interaction between metabolic bone diseases and bone formation and the importance of considering ontogenetic changes in bone structure in the study of disease during childhood.
Design of a Fully Non‐Fused Bulk Heterojunction toward Efficient and Low‐Cost Organic Photovoltaics
Authors: Ma Lijiao , Zhang Shaoqing , Ren Junzhen , Wang Guanlin , Li Jiayao , Chen Zhihao , Yao Huifeng , Hou Jianhui 
Published: November 2022

AbstractTo modulate the miscibility between donor and acceptor materials both possessing fully non‐fused ring structures, a series of electron acceptors (A4T‐16, A4T‐31 and A4T‐32) with different polar functional substituents were synthesized and investigated. The three acceptors show good planarity, high conformational stability, complementary absorption and energy levels with the non‐fused polymer donor (PTVT‐BT). Among them, A4T‐32 possesses the strongest polar functional group and shows the highest surface energy, which facilitates morphological modulation in the bulk heterojunction (BHJ) blend. Benefiting from the proper morphology control method, an impressive power conversion efficiency (PCE) of approaching 16.0 % and a superior fill factor over 0.795 are achieved in the PTVT‐BT : A4T‐32‐based organic photovoltaic cells with superior photoactive materials price advantage, which represent the highest value for the cells based on the non‐fused blend films. Notably, this cell maintains ≈84 % of its initial PCE after nearly 2000 h under the continuous simulated 1‐sun‐illumination. In addition, the flexible PTVT‐BT : A4T‐32‐based cells were fabricated and delivered a decent PCE of 14.6 %. This work provides an effective molecular design strategy for the non‐fused non‐fullerene acceptors (NFAs) from the aspect of bulk morphology control in fully non‐fused BHJ layers, which is crucial for their practical applications.
Blending to Make Nonhealable Polymers Healable: Nanophase Separation Observed by CP/MAS 13C NMR Analysis
Authors: Fujisawa Yuta , Nan Yiling , Asano Atsushi , Yanagisawa Yu , Yano Keiichi , Itoh Yoshimitsu , Aida Takuzo 
Published: November 2022

AbstractCan commodity polymers are made to be healable just by blending with self‐healable polymers? Here we report the first study on the fundamental aspect of this practically challenging issue. Poly(ether thiourea) (PTUEG3; Tg=27 °C) reported in 2018 is extraordinary in that it is mechanically robust but can self‐heal even at 12 °C. In contrast, poly(octamethylene thiourea) (PTUC8; Tg=50 °C), an analogue of PTUEG3, cannot heal below 92 °C. We found that their polymer blend self‐healed in a temperature range above 32 °C even when its PTUEG3 content was only 20 mol %. Unlike PTUEG3 alone, this polymer blend, upon exposure to high humidity, barely plasticized, keeping its excellent mechanical properties due to the non‐hygroscopic nature of the PTUC8 component. CP/MAS 13C NMR analysis revealed that the polymer blend was nanophase‐separated, which possibly accounts for why such a small amount of PTUEG3 provided the polymer blend with humidity‐tolerant self‐healable properties.
A Synthesis of Alstonlarsine A via Alstolucines B and F Demonstrates the Chemical Feasibility of a Proposed Biogenesis
Authors: Barnes Griffin L. , Hong Allen Y. , Vanderwal Christopher D. 
Published: November 2022

AbstractWe offer a new biogenetic proposal for the origin of the complex alkaloid alstonlarsine A, through rearrangement of the Strychnos alkaloids alstolucines B and F. Further, we provide evidence of the chemical feasibility of this proposal in the facile conversion of synthetic alstolucines into alstonlarsine A through a short, efficient sequence of N‐methylation, β‐elimination, and a cascade 1,7‐hydride shift/Mannich cyclization. We believe that this is the first biogenetic proposal involving the “tert‐amino effect”, a hydride‐shift‐based internal redox trigger of a Mannich cyclization. A further interesting feature of the cascade is that its stereochemical outcome most likely originates in conformational preferences during the hydride shift.
Multifunctional Helicene‐Based Ytterbium Coordination Polymer Displaying Circularly Polarized Luminescence, Slow Magnetic Relaxation and Room Temperature Magneto‐Chiral Dichroism**
Authors: Dhbaibi Kais , Grasser Maxime , Douib Haiet , Dorcet Vincent , Cador Olivier , Vanthuyne Nicolas , Riobé François , Maury Olivier , Guy Stéphan , Bensalah‐Ledoux Amina , Baguenard Bruno , Rikken Geert L. J. A. , Train Cyrille , Le Guennic Boris , Atzori Matteo , Pointillart Fabrice , Crassous Jeanne 
Published: November 2022

AbstractThe combination of physical properties sensitive to molecular chirality in a single system allows the observation of fascinating phenomena such as magneto‐chiral dichroism (MChD) and circularly polarized luminescence (CPL) having potential applications for optical data readout and display technology. Homochiral monodimensional coordination polymers of YbIIIwere designed from a 2,15‐bis‐ethynyl‐hexahelicenic scaffold decorated with two terminal 4‐pyridyl units. Thanks to the coordination of the chiral organic chromophore to Yb(hfac)3units (hfac−=1,1,1,5,5,5‐hexafluoroacetylaconate), efficient NIR‐CPL activity is observed. Moreover, the specific crystal field around the YbIIIinduces a strong magnetic anisotropy which leads to a single‐molecule magnet (SMM) behaviour and a remarkable room temperature MChD. The MChD‐structural correlation is supported by computational investigations.
The Eschenmoser's Salt as a Formylation Agent for the Synthesis of Indolizinecarbaldehydes and Their Use for Colorimetric Nitrite Detection
Authors: Antón‐Cánovas Teresa , Alonso Francisco 
Published: November 2022

AbstractC−H bond formylation is the most immediate way to incorporate the versatile formyl group into (hetero)aromatics. However, the type of reagents and severe conditions involved in the classical formylation methods often curtail their application, especially in the presence of other functional groups. Herein, we present the Eschenmoser's salt, a commercially available (dimethylamino)methylating chemical, as a useful reagent for the C−H formylation of indolizines and other compounds. The method is straightforward and mild, furnishing indolizinecarbaldehydes in modest‐to‐good yields with exclusive and remote regioselectivity. Furthermore, these compounds can be easily transformed into push‐pull dyes and are highly selective in the colorimetric detection of nitrite, a substance extensively employed as preservative in the food industry, the concentration of which is crucial to control to prevent harmful effects in living organisms. The assay is simple, allowing the naked‐eye detection of nitrite in solution or on a cotton swab for a wide range of concentrations.
Strong Anchoring of Hydrogels through Superwetting‐Assisted High‐Density Interfacial Grafting
Authors: Hao Dezhao , Wang Zhao , Liu Mingjie , Guo Xinglin , Wang Shutao , Jiang Lei 
Published: November 2022

AbstractStrong adhesion of hydrogels on solids plays an important role in stable working for various practical applications. However, current hydrogel adhesion suffers from poor interfacial bonding with solid surfaces. Here, we propose a general superwetting‐assisted interfacial polymerization (SAIP) strategy to robustly anchor hydrogels onto solids by forming high‐density interfacial covalent bonds. The key of our strategy is to make the initiator fully contact solid surfaces via a superwetting way for enhancing the interfacial grafting efficiency. The designed anchored hydrogels show strong bulk failure with a high breaking strength of ≈1.37 MPa, different from weak interfacial failure that occurs in traditional strategies. The strong interfacial adhesion greatly enhances the stability of hydrogels against swelling destruction. This work opens up new inspirations for designing strongly anchored hydrogels from an interfacial chemistry perspective.
Electrochemically‐Switched 2nd Order Non‐Linear Optical Response in an Arylimido‐Polyoxometalate with High Contrast and Cyclability
Authors: Hood Bethany R. , de Coene Yovan , Torre Do Vale Froes Afonso V. , Jones Claire F. , Beaujean Pierre , Liégeois Vincent , MacMillan Fraser , Champagne Benoît , Clays Koen , Fielden John 
Published: November 2022

AbstractElectrochemically switched 2nd order non‐linear optical responses have been demonstrated for the first time in polyoxometalates (POMs), with an arylimido‐derivative showing a leading combination of high on/off contrast (94 %), high visible transparency, and cyclability. Spectro‐electrochemical and TD‐DFT studies indicate that the switch‐off results from weakened charge transfer (CT) character of the electronic transitions in the reduced state. This represents the first study of an imido‐POM reduced state, and demonstrates the potential of POM hybrids as electrochemically activated molecular switches.
Design and preparation of durable anti‐icing polysilazane coatings with abrasion and UV resistance
Authors: Kuang Jian , An Xiaowei , Huang Congshu , Chen Hongfei , Wei Chunyang 
Published: November 2022

AbstractThis work developed a method to enhance the durability of anti‐icing performance of a coating to endure abrasion and UV exposure, through grafting functional polydimethylsiloxane (PDMS) to TiO2 particles and further reacting with polysilazane (PSZ) pre‐polymer. This method remarkably improved the anti‐icing properties of PSZ‐based coatings evaluated by freezing delay time and ice removal shear strength. After either surface abrasion for 50 cycles or UV exposure for 100 h, the modified coatings exhibited ice shear strength increase by only 10.44 and 6.44 kPa respectively, significantly lower comparing to that of the coatings containing 30% TiO2 with no PDMS modification (29.69 and 11.88 kPa, respectively). Such strengthened durability of anti‐icing performance is attributed to the PDMS molecules bridging PSZ rigid segments and TiO2 compositions, which formed a hydrophobic cross‐linking network structure. The durable anti‐icing technique developed herein shall appeal to many outdoor applications of facilities and infrastructures.
Synergistic effects of silicon based material with intumescent flame retardant in thermoplastic polyurethane: Pre‐polymerization and dynamic vulcanization based facile approach
Authors: Cui Yongyin , Pan Hongwei , Xu Zhengshuai , Li Yongxu , Cao Lan 
Published: November 2022

AbstractA flame retardant thermoplastic polyurethane (TPU) was prepared using the silicon based (Si)‐intumescent (IFR) synergistic flame‐retardant system, which combined the advantages of additive and reactive types. Silicone rubber was introduced into the matrix of hydroxybutanyl terminated polydimethylsiloxane (PDMS) block TPU via dynamic vulcanization, which enabled the combination of silicon based material and TPU. Then, the IFR system was used to supplement the defects of single Si based flame retardancy, which realized the synergistic flame retardancy of Si‐IFR. Under the Si‐IFR system, when IFR uses 15%, the TPU reached the V‐0 flame retardant level and the limiting oxygen index was 29.6. Moreover, the toughness of the Si‐IFR flame‐retardant TPU was better than PDMS block TPU. The silicon based material improved the matrix and cooperated with IFR to form a composite carbon layer, which protected the inner material, enhanced the strength of the carbon layer and eliminated dropping.
Preparation and properties of expandable epoxy foam prepreg for sandwich composites prepared via thermal expansion molding process
Authors: Min Wei , Qi Liangliang , Zhao Xinxing , Xiao Jie , Wan YuJia , Yu Muhuo , Sun Zeyu 
Published: November 2022

AbstractThermal expansion molding process (TEMP) is a new technology for integrated molding sandwich composites. However, the development of high‐performance expandable foam prepreg limits the scale applications of this technology. In this study, epoxy foam prepreg (M‐1) with expandable function was used to prepare foams with different expansion ratios via restricted foaming. Three suitable expansion ratios were determined to prepare foam sandwich composites by analyzing the density, bubble sizes, compressive strength, and expansion pressures of expandable foam. The maximum expansion pressure produced by four, six, and eight times of foam expansion were 251, 160, and 115 kPa, respectively. Tensile test and digital imaging computer technology confirmed that with the increase of foam expansion ratio, the strength decreased, but the plastic deformation ability increased. Failure modes such as foam matrix fracture, glass fiber mat fracture, and mutual‐slipping between the foam matrix and glass fiber mat occur during the stretching process. Finally, the PMI/M‐1 foam hybrid sandwich composites with three structures were prepared via the TEMP technology, which verified the feasibility of this technology in forming sandwich composites.