bluuebunny/crossref_metadata_2025 huggingface dataset:
The Coiled‐Coil Forming Peptide (KVSALKE)5 Is a Cell Penetrating Peptide that Enhances the Intracellular Delivery of Proteins
Authors: Li Jie , Tuma Jan , Han Hesong , Kim Hansol , Wilson Ross C. , Lee Hye Young , Murthy Niren
Published: December 2021

Protein‐based therapeutics have the potential to treat a variety of diseases, however, safe and effective methods for delivering them into cells need to be developed before their clinical potential can be realized. Peptide fusions have great potential for improving intracellular delivery of proteins. However, very few peptides have been identified that can increase the intracellular delivery of proteins, and new peptides that can enhance intracellular protein delivery are greatly needed. In this report, the authors demonstrate that the coiled‐coil forming peptide (KVSALKE)5 (termed K5) can function as a cell penetrating peptide (CPP), and can also complex other proteins that contain its partner peptide E5. It is shown here that GFP and Cas9 fused to the K5 peptide has dramatically enhanced cell uptake in a variety of cell lines, and is able to edit neurons and astrocytes in the striatum and hippocampus of mice after a direct intracranial injection. Collectively, these studies demonstrate that the coiled‐coil forming peptide (KVSALKE)5 is a new class of multifunctional CPPs that has great potential for improving the delivery of proteins into cells and in vivo.
Metal–Phenolic‐Network‐Coated Dendrimer–Drug Conjugates for Tumor MR Imaging and Chemo/Chemodynamic Therapy via Amplification of Endoplasmic Reticulum Stress
Authors: Wang Zhiqiang , Guo Yunqi , Fan Yu , Chen Jingwen , Wang Han , Shen Mingwu , Shi Xiangyang
Published: December 2021

Amplification of endoplasmic reticulum stress (ERS) to realize enhanced cancer therapy has been considered to be unique in current cancer nanomedicine design. Herein, the design of metal–phenolic‐network‐coated dendrimer–drug conjugates as a novel theranostic nanoplatform based on ERS amplification is reported. In the design, acetylated generation‐5 poly(amidoamine) dendrimers are conjugated with an ERS drug, toyocamycin (Toy), through the attached phenylboronic acid moiety, and coated with an iron (Fe)–tannic acid (TF) network. The generated nanocomplexes with a size of 50.2 nm are stable under the physiological environment, and can rapidly release Toy under the tumor microenvironment due to the pH‐ and reactive‐oxygen‐species‐responsive boronic ester bonds to effectively inhibit the ERS‐mediated cancer cell adaptation. Meanwhile, the coated TF network enables the nanocomplexes to generate cytotoxic hydroxyl radicals through a Fenton reaction, amplifying the ERS for improved chemo/chemodynamic therapy of cancer cells in vitro and a xenografted breast tumor model in vivo. Moreover, the coating of TF also renders the complexes with an eminent r1 relaxivity for in vivo T1‐weighted tumor magnetic resonance imaging. The created intelligent nanocomplexes may represent an advanced nanomedicine formulation uniquely integrated with a metal–phenolic network and dendrimer nanotechnology for imaging‐guided cancer therapy through ERS amplification.
Growth of 2D Materials at the Wafer Scale
Authors: Xu Xiangming , Guo Tianchao , Kim Hyunho , Hota Mrinal K. , Alsaadi Rajeh S. , Lanza Mario , Zhang Xixiang , Alshareef Husam N.
Published: December 2021

Wafer‐scale growth has become a critical bottleneck for scaling up applications of van der Waal (vdW) layered 2D materials in high‐end electronics and optoelectronics. Most vdW 2D materials are initially obtained through top‐down synthesis methods, such as exfoliation, which can only prepare small flakes on a micrometer scale. Bottom‐up growth can enable 2D flake growth over a large area. However, seamless merging of these flakes to form large‐area continuous films with well‐controlled layer thickness and lattice orientation is still a significant challenge. This review briefly introduces several vdW layered 2D materials covering their lattice structures, representative physical properties, and potential roles in large‐scale applications. Then, several methods used to grow vdW layered 2D materials at the wafer scale are reviewed in depth. In particular, three strategies are summarized that enable 2D film growth with a single‐crystalline structure over the whole wafer: growth of an isolated domain, growth of unidirectional domains, and conversion of oriented precursors. After that, the progress in using wafer‐scale 2D materials in integrated devices and advanced epitaxy is reviewed. Finally, future directions in the growth and scaling of vdW layered 2D materials are discussed.
Constructing a Stable Interface Layer by Tailoring Solvation Chemistry in Carbonate Electrolytes for High‐Performance Lithium‐Metal Batteries
Authors: Piao Zhihong , Xiao Peitao , Luo Ripeng , Ma Jiabin , Gao Runhua , Li Chuang , Tan Junyang , Yu Kuang , Zhou Guangmin , Cheng Hui‐Ming
Published: December 2021

Lithium‐metal batteries (LMBs) are considered as promising next‐generation batteries due to their high energy density. However, commercial carbonate electrolytes cannot be used in LMBs due to their poor compatibility with the lithium‐metal anode and detrimental hydrogen fluoride (HF) generation by lithium hexafluorophosphate decomposition. By introducing lithium nitrate additive and a small amount of tetramethylurea as a multifunctional cosolvent to a commercial carbonate electrolyte, NO3−, which is usually insoluble, can be introduced into the solvation structure of Li+ to form a conductive and stable solid electrolyte interface. At the same time, HF generation is suppressed by manipulating the solvation structure and a scavenging effect. As a result, the Coulombic efficiency (CE) of Li||Cu half cells using the designed carbonate electrolyte can reach 98.19% at room temperature and 96.14% at low temperature (−15 °C), and Li||LiFePO4 cells deliver a high capacity retention of 94.9% with a high CE of 99.6% after 550 cycles. This work provides a simple and effective way to extend the use of commercial carbonate electrolytes for next‐generation battery systems.
Anisotropic Carrier Mobility from 2H WSe2
Authors: Chen Ping , Pan Jinbo , Gao Wenchao , Wan Bensong , Kong Xianghua , Cheng Yang , Liu Kaihui , Du Shixuan , Ji Wei , Pan Caofeng , Wang Zhong Lin
Published: December 2021

Transition metal dichalcogenides (TMDCs) with 2H phase are expected to be building blocks in next‐generation electronics; however, they suffer from electrical anisotropy, which is the basics for multi‐terminal artificial synaptic devices, digital inverters, and anisotropic memtransistors, which are highly desired in neuromorphic computing. Herein, the anisotropic carrier mobility from 2H WSe2 is reported, where the anisotropic degree of carrier mobility spans from 0.16 to 0.95 for various WSe2 field‐effect transistors under a gate voltage of −60 V. Phonon scattering, impurity ions scattering, and defect scattering are excluded for anisotropic mobility. An intrinsic screening layer is proposed and confirmed by Z‐contrast scanning transmission electron microscopy (STEM) imaging to respond to the electrical anisotropy. Seven types of intrinsic screening layers are created and calculated by density functional theory to evaluate the modulated electronic structures, effective masses, and scattering intensities, resulting in anisotropic mobility. The discovery of anisotropic carrier mobility from 2H WSe2 provides a degree of freedom for adjusting the physical properties of 2H TMDCs and fertile ground for exploring and integrating TMDC electronic transistors with better performance along the direction of high mobility.
Unraveling the Mechanism of Electrically Induced Adhesive Debonding: A Spectro‐Microscopic Study
Authors: Anduix‐Canto Clara , Peral Daniel , Pérez‐Padilla Víctor , Diaz‐Rovira Anna Maria , Belmez Lledó Alejandro , Orme Christine A. , Petrash Stanislas , Engels Thomas , Chou Kang Wei
Published: December 2021

The design of new electrically debondable adhesives has been an area of enormous interest for the recycling, repair, and reuse of electrical components for the last decade. However, the complexity of analyzing the debonding process under real conditions is a major obstacle for elucidating the mechanism. Here, a general mechanism for the electrical debonding of ionic acrylic adhesives based on imidazolium ionic liquids is reported. Using synchrotron‐based characterization techniques, in situ experiments mimicking real debonding conditions allowed for the first time the recording of ionic diffusion and chemical reactions during the debonding process. Diffusion of ionic species toward the electrodes triggers the debonding via electrochemical reactions at the adhesive–substrate interfaces. The selection of ionic adhesive chemistry and electrodelamination conditions will eventually determine the type of adhesive failure. A detailed understanding of the mechanism allows the development of new electrically debondable adhesives, which is crucial to promote circular economy and a more sustainable environment.
Bistrifluoroacetamide‐Activated Double‐Layer Composite Solid Electrolyte for Dendrite‐Free Lithium Metal Battery
Authors: Hao Shuai , Ran Qiwen , Xiao Yu , Li Lei , Ji Yuyao , Liu Jintao , Yang Ying Chun , Liu Xingquan
Published: December 2021

The achievement of high ionic conductivity for solid‐state electrolyte and low interface resistance between electrodes and electrolyte are keys to successful solid‐state lithium ion batteries. In this paper, an efficient solid‐state electrolyte with dual‐layer structure for dendrite‐free lithium metal battery is designed. A Li metal‐friendly poly(ethylene oxide) (PEO) can serve as low‐voltage stable polymer electrolyte and ceramic‐dominating poly(vinylidene fluoride)–lithium aluminum titanium phosphate (PVDF–LATP) composite solid electrolyte is able to resist higher voltage facing cathode. More importantly, bistrifluoroacetamide (BTFA), as a polar molecular plasticizer, can simultaneously inhibit polymer crystallization, coordinate the delocalization of negative charges, and facilitate the solvation of lithium salts, providing absorption sites for lithium ion migration. The obtained BTFA‐activated PEO/PVDF–LATP double‐layer solid electrolyte exhibits satisfied ionic conductivity (4.4 × 10−4 S cm−1 at 25 °C), high Li+‐transfer number (0.68), and wide electrochemical stable windows (0–5.092 V vs Li/Li+). Moreover, both the assembled full cells with LiFePO4 and high‐voltage LiNi0.8Co0.1Mn0.1O2 cathodes show high initial discharge capacities (163.3 and 219.5 mAh g−1 at 0.1 C, respectively), excellent cycling, and rate performance.
Highly Efficient Hydrogen Production in the Photoreforming of Lignocellulosic Biomass Catalyzed by Cu,In‐Doped ZnS Derived from ZIF‐8
Authors: Nagakawa Haruki , Nagata Morio
Published: December 2021

Cu,In‐doped ZnS (CIZS) is fabricated from a metal–organic framework (MOF) precursor, namely a Cu,In‐doped zeolitic imidazolate framework (ZIF‐8). The prepared CIZS shows high activity for hydrogen production in the photoreforming reaction of lignocellulosic biomass under simulated sunlight. The activity is 125‐fold greater than that of undoped ZnS produced by the same method. Compared to CIZS synthesized by the conventional solvothermal method for sulfide photocatalysts, the CIZS synthesized via a MOF is characterized by high crystallinity and an 8.9‐fold increase in hydrogen production activity. This catalyst also exhibits better performance than conventional photoreforming catalysts, while it is free from toxic substances, such as Cd, or expensive cocatalysts, like Pt. In addition, the prepared CIZS is stable in photocatalytic reactions and achieves an apparent quantum yield of ≈28% under 360‐nm light irradiation.
Self‐Organization of Remote Reservoirs: Transferring Computation to Spatially Distant Locations
Authors: Tanaka Kazutoshi , Tokudome Yuji , Minami Yuna , Honda Satoko , Nakajima Toshiki , Takei Kuniharu , Nakajima Kohei
Published: December 2021

Soft materials generate rich and diverse dynamics that can be used as computational resources based on the framework of physical reservoir computing. Herein, a method that exploits the dynamic coupling between soft structures and a water medium to allow for the transfer of computation to spatially distant locations is proposed. This technique is implemented by introducing the concept of remote reservoirs that can autonomously alter their physical constituents in real time rather than using reservoirs with predefined, fixed physical constituents. These remote reservoirs self‐organize by including many ad hoc physical substrates in the environment, making the framework more flexible for soft robotic applications. Using a simple experimental platform consisting of silicone rubber strips containing embedded flexible strain sensors, it is demonstrated that the dynamics of passive silicone rubber strips located at a distance from the actuation point can be successfully exploited for computation through generalized synchronization realized via the medium of water. Future application scenarios are illustrated, in which the proposed technique is applied in emergency situations as a communication tool for transferring a message to a location that humans cannot easily access. For example, the technique could be applied to communicate with people trapped in submerged caves.
Direct C−H Difluoroalkylation of Heteroarenes with Difluoroalkyl Carboxylic Acids
Authors: Guo Chunfang , Han Xuliang , Li Xiangye , Diao Zhengzhen , Li Xinjin , Dong Yunhui
Published: December 2021

A new method for the difluoroalkylation of heteroaromatic compounds has been developed by employing readily available difluoroalkyl carboxylic acids. This silver‐catalyzed reaction proceeds under mild conditions and affords a broad range of difluoroalkylated heteroarenes in moderate to good yields, including pyridines, pyrimidines, pyrazines, quinolines, quinoxalines as well as bioactive compounds.
Association of resting heart rate with cognitive decline and dementia in older adults: A population‐based cohort study
Authors: Imahori Yume , Vetrano Davide L. , Xia Xin , Grande Giulia , Ljungman Petter , Fratiglioni Laura , Qiu Chengxuan
Published: December 2021

Introduction: Resting heart rate (RHR) predicts future risk for cardiovascular disease (CVD). However, longitudinal studies investigating the relationship of RHR with cognitive decline are scarce.

Methods: This population‐based cohort study included 2147 participants (age≥60) in SNAC‐K who were free of dementia and regularly followed from 2001–2004 to 2013–2016. RHR was assessed with electrocardiogram. Dementia was diagnosed following the Diagnostic and Statistical Manual of Mental Disorders 4th Revision criteria. Global cognitive function was assessed using Mini‐Mental State Examination (MMSE). Data were analyzed using Cox and linear mixed‐effects models.

Results: RHR≥80 (vs. 60–69) bpm was associated with a multi‐adjusted hazard ratio of 1.55 (95% confidence interval 1.06−2.27) for dementia. The association remained significant after excluding participants with prevalent and incident CVDs. Similarly, RHR≥80 bpm was associated with a multi‐adjusted β‐coefficient of –0.13 (–0.21 to –0.04) for MMSE score.

Discussion: Higher RHR is associated with increased risk for dementia and faster cognitive decline independent of CVDs in a general population of elderly people.
Optimal Settings for Amplification and Estimation Of Small Effects In Postselected Ensembles
Authors: Rostom Aiham M.
Published: December 2021

To describe the pre‐ and postselected quantum ensembles, a complex quantity called the weak value of an operator is used. The weak value is highly controversial due to the fact that it is not bounded by the possible eigenvalues of the corresponding operator. Nevertheless, the obtaining of the anomalous weak value is regarded as a powerful technique in the quantum interferometry nowadays. Here it is shown that the postselection of a quantum system recovers a completely hidden interference effect in the measurement apparatus. Studying the interference pattern shows the optimal settings for the amplification and the parameter estimation. It also proves that the weak value is not an element of reality. Using single photons, it is investigated how a postselected photon can impart a π phase shift (the peak of the amplification) to a photon interacting weakly with it in a nonlinear optical medium. The increasing of the degree of the entanglement lies behind the effectiveness of the postselection in the parameter estimation. In particular, arranging to postselect on pure entangled states can optimize the signal‐to‐noise ratio, allowing to achieve high‐sensitive measurements using low input power.
Vernetzte Polypeptide durch RAFT‐vermittelte Polymerisation zum kontinuierlichen Aufbau von Polymerfilmen
Authors: Chan Nicholas J. , Lentz Sarah , Gurr Paul A. , Tan Shereen , Scheibel Thomas , Qiao Greg G.
Published: December 2021

Polypeptidbeschichtungen spielen aufgrund ihres großen biologischen Potentials eine wichtige Rolle in der Oberflächenmodifizierung von Materialien. Da ihre Eigenschaften durch ihren strukturellen Aufbau mitbestimmt werden, ist eine Kontrolle der Struktur durch entsprechende Herstellungsstrategien notwendig. In diesem Artikel berichten wir über eine einfache Methode zur präzisen Herstellung von dicht vernetzten Polypeptidfilmen mit ungewöhnlich hoher β‐Faltblatt – und Zufallsknäuel Konformation durch eine kontinuierliche Assemblierungspolymerisation (CAP, continuous assembly polymerization) mittels reversibler Addtitions‐Fragmentierungs‐Kettenübertragungspolymerisation (RAFT Polymerisation, reversible‐addition‐fragmentation chain‐transfer polymerization), kurz CAP‐RAFT. CAP‐RAFT wurde bereits grundlegend mit methacryliertem Poly‐l‐Lysin (PLLMA) und methacrylierter Poly‐l‐Glutaminsäure (PLGMA) untersucht. Eine sorgfältige Anpassung der Methode führte hier zu Filmen mit einer Schichtdicke von bis zu 36.1±1.1 nm, die durch mehrfache Anwendung dieser Strategie auf 94.9±8.2 nm erhöht werden konnte. PLLMA‐ und PLGMA‐Filme wiesen überraschenderweise bis zu 30–50 % Zufallsknäuel Konformation auf. Durch den enzymatischen Abbau mit einem Protease‐Mix, der Proteasen im Wundheilungsmileu repräsentiert, konnte das Potential diesen Strukturen für Anwendungen im Wirkstofftransport und in der Gewebezüchtung gezeigt werden.
Coordinated Anionic Inorganic Module—An Efficient Approach Towards Highly Efficient Blue‐Emitting Copper Halide Ionic Hybrid Structures
Authors: Li Haibo , Lv Yi , Zhou Zhennan , Tong Hua , Liu Wei , Ouyang Gangfeng
Published: December 2021

Copper halide based organic–inorganic hybrid semiconductors exhibit great potential as light‐emitting materials with excellent structural variety and optical tunability. Among them, copper halide hybrid molecular compounds with discrete inorganic modules are particularly interesting due to their high quantum efficiency. However, synthesizing highly efficient blue‐emitting molecular clusters remains challenging. Here, we report a novel and facile strategy for the design and synthesis of highly luminescent copper halide hybrid structures by fabricating coordinated anionic inorganic modules in these ionic species. By using this approach, a family of strongly blue‐emitting copper halide hybrid ionic structures has been prepared with high internal quantum yields up to 98 %. Strong luminescence from the combination of ionic and covalent bonds in these compounds make them ideal candidates as alternative, rare‐earth‐element free light‐emitting materials for possible use in optoelectronic devices.
Crosslinked Polypeptide Films via RAFT‐Mediated Continuous Assembly of Polymers
Authors: Chan Nicholas J. , Lentz Sarah , Gurr Paul A. , Tan Shereen , Scheibel Thomas , Qiao Greg G.
Published: December 2021

Polypeptide coatings are a cornerstone in the field of surface modification due to their widespread biological potential. As their properties are dictated by their structural features, subsequent control thereof using unique fabrication strategies is important. Herein, we report a facile method of precisely creating densely crosslinked polypeptide films with unusually high random coil content through continuous assembly polymerization via reversible addition–fragmentation chain transfer (CAP‐RAFT). CAP‐RAFT was fundamentally investigated using methacrylated poly‐l‐lysine (PLLMA) and methacrylated poly‐l‐glutamic acid (PLGMA). Careful technique refinement resulted in films up to 36.1±1.1 nm thick which could be increased to 94.9±8.2 nm after using this strategy multiple times. PLLMA and PLGMA films were found to have 30–50 % random coil conformations. Degradation by enzymes present during wound healing reveals potential for applications in drug delivery and tissue engineering.
Pd‐catalyzed decarboxylative [3 + 2] cycloaddition: Assembly of highly functionalized spirooxindoles bearing two quaternary centers
Authors: Li Tiantian , Zhu Xinju , Jiang Hui , Wang Yanong , Zheng Nan , Peng Tian , Gao Rui , Shi Linlin , Hao Xin‐Qi , Song Mao‐Ping
Published: December 2021

An efficient method for the practical formation of functionalized spirooxindoles, which was accompanied by generating a sterically congested spiroketal system and bearing two quaternary stereocenters via a sequential palladium, catalyzed decarboxylative [3 + 2] cycloaddition of vinylethylene carbonates (VECs) and isatins. Importantly, the redox‐neutral catalytic system possesses the characteristics of operational convenience, good functional group tolerance, and good regioselectivity and diastereoselectivity, which enables a diastereoselective synthesis of spiroketal oxindole skeletons in an excellent yield.
Ring size enlargement in an ortho‐cycloalkyl‐substituted bis(imino)pyridine‐cobalt ethylene polymerization catalyst and its impact on performance and polymer properties
Authors: Han Mingyang , Oleynik Ivan I. , Liu Ming , Ma Yanping , Oleynik Irina V. , Solan Gregory A. , Liang Tongling , Sun Wen‐Hua
Published: December 2021

Four unsymmetrical examples of bis(arylimino)pyridines that each possess an ortho‐cycloalkyl substituent of unique ring size, 2‐{CMeN(2,4,6‐Me3C6H2)}‐6‐{CMeN(2,4‐(CHPh2)2‐6‐RC6H2)}C5H3N (R = cyclopentyl L1, cyclohexyl L2, cyclooctyl L3, cyclododecyl L4), have been prepared and employed as reactants in the formation of the corresponding cobaltous chloride complexes, (N,N,N′)CoCl2 (Co1–Co4). Structural characterization of Co2 and Co3 spotlights the five‐coordinate geometry and the steric disparity imposed on the metal center by the inequivalent N‐mesityl and N‐2,4‐dibenzyhydryl‐6‐cycloalkylphenyl groups. Co1–Co4 all proved productive precatalysts for ethylene polymerization achieving optimal performance at a temperature of 60°C on activation with either MAO or MMAO. Cyclopentyl‐containing Co1 displayed the highest level (up to 10.3 × 106 g PE per mol [Co] per h), whereas its cyclododecyl counterpart Co4 the lowest (down to 0.14 × 106 g PE per mol [Co] per h). Strictly linear polyethylenes were produced with molecular weights spanning the range 22.0–36.0 kg per mol for Co1–Co4/MAO and 22.6–33.6 kg per mol for Co1–Co4/MMAO, with cyclohexyl Co2 producing the highest values with either activator. With the exception of the polymer produced using Co4, all catalysts afforded narrow unimodal distributions (Mw/Mn range: 1.7–2.2) for the polyethylenes in line with single site active species. By contrast, Co4 bearing the largest and conformationally flexible cycloalkyl group formed polyethylenes that were distinctly bimodal, which would imply the presence of two active species. End‐group analysis of lower molecular weight polymer samples identified vinyl groups congruent with a termination step involving β‐H elimination.
Various coordination modes of new coumarin Schiff bases toward Cobalt (III) ion: Synthesis, spectral characterization, in vitro cytotoxic activity, and investigation of apoptosis
Authors: Giriraj Kalaiarasi , Mohamed Kasim Mohamed Subarkhan , Balasubramaniam Keerthana , Thangavel Sathiya Kamatchi , Venkatesan Janani , Suresh Sharmila , Shanmugam Pritha , Karri Chiranjeevi
Published: December 2021

Four Co (III) complexes containing substituted acetyl coumarin Schiff bases have been synthesized and structurally characterized using IR, UV–visible, 1H nuclear magnetic resonance (NMR), and mass spectroscopic techniques, which suggested that the complexes Co1 and Co3 have a similar type of coordination behavior with the binding of the ligands through ring carbonyl oxygen, azomethine nitrogen and enolate oxygen atoms. In complexes Co2 and Co4, the coordination was through ring carbonyl oxygen, azomethine nitrogen, and thiolate sulfur atoms and the complexes are of ML2 type. The anticancer potential of the synthesized complexes has been analyzed against cancerous cells such as human breast cancer cells (MCF‐7), human lung cancer cells (A549), and non‐cancerous Human Umbilical Vein Endothelial Cells (HUVEC). The activity of the complexes exceeded that of the ligands and the standard drug cisplatin, and the order of activity observed was Co4 > Co3 > Co2 > Co1 > cisplatin > ligands. The IC50 values of the complexes were less than 5 μM in both the cancer cells and greater than 200 μM for non‐cancerous cells indicating the specificity of the complexes toward cancer cells. The morphological changes of the MCF‐7 and A549 cells with the complexes Co1‐Co4 have been studied by AO‐EB (Acridine Orange‐Ethidium Bromide) and Hoechst 33258 staining methods, and these results revealed that the complexes induce cell death only through apoptosis. Further the mode of cell death induced by the complexes has been confirmed by flow cytometric analysis. Complex Co4 showed better activity due to the electron‐donating hydroxyl group present in the seventh position of the coumarin ring. These results highlight the strong possibility of developing highly active cobalt coumarin complexes as anticancer agents.
Recent progress of biomass based self‐healing polymers
Authors: Bei Yu , Ma Yufeng , Song Fei , Kou Zhimin , Hu Lihong , Bo Caiying , Jia Puyou , Zhou Yonghong
Published: December 2021

Self‐healing polymer materials have been developed rapidly over the past 20 years, which can replace thermosetting materials to a certain extent, repair damage without manual intervention, prolong service life, and compress usage cost. The self‐healing polymer materials derived from biomass resources can reduce the dependence on traditional non‐renewable resources such as petroleum. The structures and properties of biomass based self‐healing polymer materials are of great significance for their processing, recycling and self‐healing. In this paper, the research progress of bio‐based self‐healing polymer materials based on dynamic non‐covalent bonds and dynamic covalent bonds including hydroxyl ester, Schiff base, disulfide bond, and hydroxyl urethane derived from vegetable oil, lignin, cellulose, vanillin and natural rubber were reviewed, and the dynamic non‐covalent bonds and dynamic covalent bonds were also introduced. The applications of various dynamic covalent bonds and dynamic non‐covalent bonds in the design and construction of polymer materials were reviewed, and the future development of dynamic covalent polymer materials was prospected.
Data‐driven methodology to realize strong and broadband microwave absorption properties of polymer‐fly ash cenosphere composite
Authors: Bora Pritom J. , Mahanta Bibhusita , Kishore  , Ramamurthy Praveen C.
Published: December 2021

A very efficient microwave absorption characteristic of conducting polymer (polyaniline or PANI) incorporated fly ash cenosphere (FAC), which is a waste of thermal power plant, is revealed in this work with materials data‐driven approach. The different loading (wt%) of PANI‐FAC hybrids to a polymer such as polyvinyl butyral (PVB) results in different reflection loss (RL). However, RL performances do not improve by simply increasing the PANI‐FAC hybrid loading (wt%) to PVB. Herein, PANI‐FAC loading to PVB is optimized through the electromagnetic data‐driven methodology. A remarkable RL ≤ − 40 dB with entire X‐band (8.2–12.4 GHz) absorption bandwidth (RL ≤ −10 dB, RL value −10 dB corresponds to 90% absorption) is predicted for 8.5 wt% PANI‐FAC hybrid loaded PVB‐PANI‐FAC composite. The predicted RL matched with experimental data (minimum RL value −44.5 dB with X‐band absorption bandwidth), confirming the proposed proof of concept of data‐driven methodology to obtain broadband and robust microwave absorption characteristics of polymer‐FAC composites.
Investigation of self‐cleaning and bouncing properties of superhydrophobic aluminum nitride/silicone rubber
Authors: Zhou Wei , Ma Yongwei , He Qiang
Published: December 2021

In order to investigate the effect of aluminum nitride (AlN) on the self‐cleaning and bouncing properties of room temperature vulcanized (RTV) silicone rubber, a superhydrophobic AlN/RTV composite with micro‐nano structure was prepared by powder scattering technology. The method combines the characteristics of RTV curing at room temperature, and has the advantages of simple operation, low cost and easy realization. Bouncing experiments, with different droplet sizes, different tilting angles and different temperatures, and self‐cleaning experiments were designed. The micro‐morphology of superhydrophobic surface was analyzed by Raman spectroscopy, scanning electron microscope, energy dispersive spectrometer, and interferometric 3D profilometer. The results show that the static contact angle and the rolling angle of AlN/RTV are 157.7 ± 0. 9° and 4.2 ± 0.7°, respectively. Many micro‐roughness structures were formed on the RTV surface by AlN, which reduced the contact area between droplets and the sample surface, so the samples had outstanding self‐cleaning and bouncing properties.
Effects of heat stress on virus transmission and virus‐mediated apoptosis in whitefly Bemisia tabaci
Authors: Wang Xin‐Ru , Shao Yue , Wang Chao , Liu Yin‐Quan
Published: December 2021

Tomato yellow leaf curl virus (TYLCV), a plant DNA virus of the genus Begomovirus, is transmitted by whiteflies of the Bemisia tabaci species complex in a persistent manner. Our previous study indicated that activation of the apoptosis pathway in whiteflies could facilitate TYLCV accumulation and transmission. Considering that temperature change can influence the spread of insect‐borne plant viruses, we focused on plant virus induced‐apoptosis to investigate the underlying mechanism of temperature regulation on plant virus transmission via an insect vector. We found that heat stress (40°C) on whiteflies could facilitate TYLCV accumulation and increase transmission to tomato plants. Despite upregulation of caspase‐1 and caspase‐3 gene expression, heat stress failed to induce an increase in the activation of cleaved caspase‐3 and DNA fragmentation in TYLCV‐infected whiteflies. However, our data failed to determine the role of heat stress in apoptosis modulation of insect–plant virus interplay while still providing clues to understand insect vectors and their transmitted plant viruses.
Perceptions, satisfactions, and performance of undergraduate students during Covid‐19 emergency remote teaching
Authors: Wilhelm Jessica , Mattingly Spencer , Gonzalez Victor H.
Published: December 2021

Due to the Covid‐19 pandemic, the education system worldwide faced sudden and unforeseen challenges. Many academic institutions closed their doors, forcing both educators and students to transition to Emergency Remote Teaching (ERT) for the remainder of the semester. This transition eliminated hands‐on experiences, increased workload, and altered curricula. However, these aspects, as well as students' perceptions, study habits, and performance in response to ERT remain poorly documented. This contribution describes changes in the curriculum of an undergraduate cadaver‐based laboratory, and explores students' performance, self‐perceived learning, and overall satisfaction during this educational crisis. Online content delivery for this course included both asynchronous instruction and synchronous discussion sessions. While formative assessments remained the same, online spotter examinations included short answer, multiple choice, multiple answer, ordering, and true and false questions. Despite examination grades improving 20% during ERT, students reported lower levels of learning, confidence, and engagement with the course materials when compared to the face‐to‐face portion of the class. The most prevalent challenges identified by students were those related to the loss of access to cadaver‐based learning, including difficulty identifying and visualizing structures in three dimensions, and the loss of context and sensorial cues. Flexibility in taking examinations and learning the material at their own pace were recognized as positive outcomes of the ERT transition. While the resulting student perceptions and performances are unsurprising, they offer insight into the challenges of fostering a productive learning environment in a future threatened by epidemic outbreak and economic uncertainty.
The autonomy‐validity dilemma in mechanical prediction procedures: The quest for a compromise
Authors: Neumann Marvin , Niessen A. Susan M. , Tendeiro Jorge N. , Meijer Rob R.
Published: December 2021

A robust finding in psychological research is that combining information with a mechanical rule results in more valid predictions than combining information holistically in the mind. Nevertheless, information is typically combined holistically in practice, resulting in suboptimal predictions and decisions. Earlier research showed that decision makers are more likely to use mechanical prediction procedures when they retain autonomy in the decision‐making process. However, it remains largely unknown how different autonomy‐enhancing features affect predictive validity. Therefore, in two preregistered studies (total N = 342), we investigated if and how prediction procedures can be designed such that they satisfy decision makers' autonomy needs and acceptance without reducing predictive validity. Based on archival application data from a university admission procedure, participants predicted applicants' first‐year grade point average and chance of dropout. The results of Bayesian analyses showed that participants preferred prediction procedures in which they retained autonomy by choosing consistent predictor weights of a mechanical rule or by holistically adjusting the predictions of an optimal regression model. In general, these prediction procedures resulted in slightly higher predictive validity compared with fully holistic prediction. Providing participants with predictor validity information slightly increased predictive validity when participants could choose predictor weights but not when making holistic predictions or adjusting optimal model predictions. Giving decision makers a role in designing mechanical rules through choosing weights based on explicit predictive validity information could help promote the implementation and validity of mechanical prediction in practice.
Concomitant genetic defects potentiate the adverse impact of prenatal alcohol exposure on cardiac outflow tract maturation
Authors: Harvey Drayton C. , De Zoysa Prashan , Toubat Omar , Choi Jongkyu , Kishore Jahnavi , Tsukamoto Hidekazu , Kumar S. Ram
Published: December 2021

Background

Prenatal alcohol exposure (PAE) is associated with an increased incidence of congenital heart defects (CHD), in particular outflow tract (OFT) defects. However, the variability in the incidence of CHD following PAE has not been fully explored. We hypothesize that a concomitant, relevant genetic defect would potentiate the adverse effect of PAE and partially explain the variability of PAE‐induced CHD incidence.

Methods

The OFT is formed by the second heart field (SHF). Our PAE model consisted of two intraperitoneal injections (3 g/kg, separated by 6 hr) of 30% ethanol on E6.5 during SHF specification. The impact of genetic defects was studied by SHF‐specific loss of Delta‐like ligand 4 (Dll4), fibroblast growth factor 8 (Fgf8) and Islet1.

Results

Acute PAE alone significantly increased CHD incidence (4% vs. 26%, p = .015) with a particular increase in OFT alignment defects, viz., double outlet right ventricle (0 vs. 9%, p = .02). In embryos with a SHF genetic defect, acute PAE significantly increased CHD incidence (14 vs. 63%, p < .001), including double outlet right ventricle (6 vs. 50%, p < .001) compared to controls. PAE (p = .01) and heterozygous loss of Dll4 (p = .04) were found to independently contribute to CHD incidence, while neither Islet1 nor Fgf8 defects were found to be significant.

Conclusions

Our model recapitulates the increased incidence of OFT alignment defects seen in the clinic due to PAE. The presence of a concomitant SHF genetic mutation increases the incidence of PAE‐related OFT defects. An apparent synergistic interaction between PAE and the loss of DLL4‐mediated Notch signaling in OFT alignment requires further analysis.
Magnetic frequency mixing technological advances for the practical improvement of point‐of‐care testing
Authors: Li Tangan , Wang Kan , Zheng Chujun , Zheng Wei , Cheng Yuemeng , Ning Qihong , Xu Hao , Cui Daxiang
Published: December 2021

Nanomaterials, especially superparamagnetic nanomaterials, have recently played essential roles in point‐of‐care testing due to their intrinsic magnetic, electrochemical, and optical properties. The inherent superparamagnetism of magnetic nanoparticles makes them highly sensitive for quantitative detection. Among the various magnetic detection technologies, frequency mixing technology (FMT) technology is an emerging detection technique in the nanomedical field. FMT sensors have high potential for development in the field of biomedical quantitative detection due to their simple structure, and they are not limited to the materials used. In particular, they can be applied for large‐scale disease screening, early tumor marker detection, and low‐dose drug detection. This review summarizes the principles of FMT and recent advances in the fields of immunoadsorption, lateral flow assay detection, magnetic imaging, and magnetic nanoparticles recognition. The advantages and limitations of FMT sensors for robust, ultrasensitive biosensing are highlighted. Finally, the future requirements and challenges in the development of this technology are described. This review provides further insights for researchers to inspire the future development of FMT by integration into biosensing and devices with a broad field of applications in analytical sensing and clinical usage.
Fibrin‐specific poly(N‐isopropylacrylamide) nanogels for targeted delivery of tissue‐type plasminogen activator to treat thrombotic complications are well tolerated in vivo
Authors: Mihalko Emily P. , Nellenbach Kimberly , Krishnakumar Manasi , Moiseiwitsch Nina , Sollinger Jennifer , Cooley Brian C. , Brown Ashley C.
Published: December 2021

Targeted drug delivery for maintaining blood fluidity can reduce the risks associated with systemic anticoagulants that can lead to off‐target bleeding. Recently, there has been much interest in targeted delivery of tissue‐type plasminogen activator (tPA) for treating thrombotic complications. The work presented here characterizes a fibrin‐specific nanogel (FSN) design for targeted delivery of tPA to treat thrombotic complications. Fibrin binding and clot degradation were characterized in vitro, and animal models of thrombosis were used to examine nanogel effects on coagulation parameters. In vitro assays showed tPA‐FSNs attach to fibrin in a dose‐dependent manner independent of tPA loading. In animal models of thrombosis, including an electrolytic injury to monitor clot properties in real time, and a lipopolysaccharide‐induced disseminated intravascular coagulation (DIC) animal model, tPA‐FSNs modulated fibrin/fibrinogen and platelet incorporation into clots and at optimized dosing could recover consumptive coagulopathy in DIC. Distribution of unloaded and tPA‐loaded FSNs showed potential clearance of tPA‐FSNs after 24 h, although unloaded FSNs may be retained at sites of fibrin deposits. Maximum tolerated dose studies showed tPA‐FSNs have minimal toxicity up to 20 times the optimized therapeutic dose. Overall, these studies demonstrate the therapeutic efficacy of targeted fibrinolysis for systemic microthrombi and begin to evaluate key translational parameters for tPA‐FSN therapeutics, including optimal tPA‐FSN dosage in a DIC rodent model and safety of intravenous tPA‐FSN therapeutics.
Vibsane‐Type Diterpenoids: Structures, Derivatives, Bioactivities, and Synthesis
Authors: Li Meng , Zhou Zhi‐Ping , Yuan Zai‐Feng , Zhao Qin‐Shi
Published: December 2021

Vibsane‐type diterpenoids isolated from the genus Viburnum, are rare 6–11 membered ring polysubstituted macrocyclic diterpenoids. Since the first report of vibsane‐type diterpenoids from V. odoratissimum in 1980, they have attracted the attention of scientists due to their complex structures, excellent biological activities, and great synthetic challenges. Recently, there are some notable research achievements on the discovery, synthesis, structural modification, and pharmacological mechanism of vibsane‐type diterpenoids. Therefore, we will focus on these aspects to review important achievements of vibsane diterpenoids between 1980–2021.
Synthesis of Chiral Amines via a Bi‐Enzymatic Cascade Using an Ene‐Reductase and Amine Dehydrogenase
Authors: Jongkind Ewald P. J. , Fossey‐Jouenne Aurélie , Mayol Ombeline , Zaparucha Anne , Vergne‐Vaxelaire Carine , Paul Caroline E.
Published: December 2021

Access to chiral amines with more than one stereocentre remains challenging, although an increasing number of methods are emerging. Here we developed a proof‐of‐concept bi‐enzymatic cascade, consisting of an ene reductase and amine dehydrogenase (AmDH), to afford chiral diastereomerically enriched amines in one pot. The asymmetric reduction of unsaturated ketones and aldehydes by ene reductases from the Old Yellow Enzyme family (OYE) was adapted to reaction conditions for the reductive amination by amine dehydrogenases. By studying the substrate profiles of both reported biocatalysts, thirteen unsaturated carbonyl substrates were assayed against the best duo OYE/AmDH. Low (5 %) to high (97 %) conversion rates were obtained with enantiomeric and diastereomeric excess of up to 99 %. We expect our established bi‐enzymatic cascade to allow access to chiral amines with both high enantiomeric and diastereomeric excess from varying alkene substrates depending on the combination of enzymes.
Co‐Feeding of Ethene, Propene, and 1‐Butene to Co‐Mn‐Catalyzed Fischer‐Tropsch Synthesis
Authors: Reul Andreas , Thiessen Johannes , Jess Andreas , Scholz Judith , Heykamp Angela
Published: December 2021

In Fischer‐Tropsch synthesis (FTS), a variety of hydrocarbons with different chain lengths are formed. The selectivities depend on the catalyst and the reaction conditions. Co‐feeding olefins allows changing the selectivity even outside the rules of the Anderson‐Schulz‐Flory distribution. In this work, ethene, propene, and 1‐butene were co‐fed to Co‐Mn‐catalyzed FTS to increase the olefin selectivity in the C3‐ to C8‐fraction. An increase of the CO reaction rate and oxygenate selectivity indicates that besides FTS also hydroformylation takes place. While the predominant reaction is the unwanted hydrogenation of the co‐fed olefins, this could in case of ethene be reduced by lowering the H2 pressure.
On properties of EFA plots
Authors: Neymeyr Klaus , Beese Martina , Sawall Mathias
Published: December 2021

The evolving factor analysis (EFA) facilitates the detection of the emergence or loss of chemical species during a chemical reaction, a chromatographic process, a spectroelectrochemical analysis, and other experiments. To this end, EFA monitors the singular values of sequences of spectral data matrices with increasing dimensions. This paper studies the growth behavior of these singular values. It investigates properties of the EFA techniques, analyzes the general shape of the singular value curves, and gives practical remarks for an improved extraction of chemical information from EFA plots.
CO2‐Philic Mixed‐Matrix Membranes Based on Ultra‐Stable Porous‐Framework Zirconium Phosphate
Authors: Ji Taotao , Liu Liangliang , Wang Lingyi , Li Yanshuo , Liu Yi
Published: December 2021

The practical application of membrane separation, such as CO2 recovery from flue gas, is usually accompanied by harsh operating conditions of high temperature and pressure as well as acidic and humid feed properties, which poses a great challenge to the stability of membrane materials. In this work, zirconium phosphate material with highly stable porous‐framework structure was synthesized by ionothermal method, and then, its incorporation into the polymer matrix to prepare ZrPOF‐Pebax mixed‐matrix membranes (MMMs) was pioneered. Benefiting from their 4.0 × 3.0 Å 7‐ring windows and CO2‐philic framework, the optimal MMMs with a 5 wt % ZrPOF content exhibited enhanced CO2/N2 selectivity of 29.6, with a decent CO2 permeability of 286.3 Barrer, which raised by 79.4 and 67.5% compared to the neat Pebax 2533 membranes, respectively. Furthermore, owing to their excellent thermal, water, and chemical stability, obtained MMMs maintained excellent performances under harsh operating conditions.
Recent Advances of Monolithic All‐Perovskite Tandem Solar Cells: From Materials to Devices
Authors: Jiang Shan , Bai Yiming , Ma Zongwen , Jin Shengli , Zou Chao , Tan Zhao'ao
Published: December 2021

Comprehensive Summary

Organic–inorganic metal‐halide perovskite solar cells (PerSCs) have achieved significant progresses due to their outstanding optoelectronic characteristics, and the power conversion efficiency (PCE) of single‐junction PerSCs has been boosted from 3.8% to a certified 25.2%. However, the efficiency of single‐junction cells is governed by the Shockley–Queisser (S–Q) radiative limit, and fabricating all‐perovskite tandem solar cells is a particularly attractive method to break the S–Q limit. Since the bandgap of lead (Pb)–based mixed halide perovskite can be tuned from 1.55 eV to 2.3 eV, and the mixed tin (Sn)–Pb perovskites have bandgap of ~1.2 eV, these perovskites become the best candidates for the front and rear subcells of all‐perovskite tandem device, respectively. In this review, we firstly summarize the current development progresses of two‐terminal (2‐T) all‐perovskite tandem solar cells. For further optimizing the device performance, the wide bandgap mixed halide perovskites for front subcell, mixed Sn–Pb narrow bandgap perovskites for rear subcell, and the interconnection layer (ICL) of 2‐T tandem device are then discussed. This review aims to open a pathway to realize highly efficient all‐perovskite tandem solar cells.
Revealing the Solution Structure of Pd(OAc)2 with Halide Additives
Authors: Wang Liwei , Yang Dali , Alhumade Hesham , Yi Hong , Qi Xiaotian , Lei Aiwen
Published: December 2021

Comprehensive Summary

Mechanistic studies of the palladium catalyst activation with halide additives are of great importance to palladium catalysis. In this work, XAFS spectroscopy and cyclic voltammetry were utilized to study real structures of Pd(OAc)2 in solution with different inorganic halogen additives. XAFS results demonstrate that Pd maintained +2 in the presence of excessive LiCl, LiBr, ZnCl2, ZnBr2, and NaI. Fitting results of EXAFS spectra revealed that the Pd's first shell is replaced by halogen partially or completely depending on the halogen species. DFT calculations were conducted to identify the most reliable solvated structures. The combined experimental and computational studies elucidate the critical role of inorganic halide additives in Pd chemistry.