bluuebunny/crossref_metadata_2025_split huggingface dataset:
High‐Efficiency Air‐Processed Si‐Based Perovskite Light‐Emitting Devices via PMMA‐TBAPF6 Co‐Doping
Authors: Xu Xiaoxiao , Zhu Ting , Xiao Ke , Zhu Yu , Chen Jiaming , Li Dongke , Xu Ling , Xu Jun , Chen Kunji 
Published: March 2022

AbstractThe preparation of high‐efficiency perovskite light‐emitting devices (PeLEDs) in the air‐ambient has always been a challenge. Herein, the authors propose a Si‐based near‐infrared air‐processed PeLED through the anti‐solvent engineering. Two materials, poly(methyl methacrylate) (PMMA) and tetrabutylammonium hexafluorophosphate (TBAPF6) are co‐doped into the anti‐solvent, the former protects the perovskite from degradation in a high‐humidity atmosphere, and the latter passivates the defects on perovskite surface and increases the conductivity. Through the anti‐solvent engineering, the efficiency of PeLEDs has been significantly enhanced and obtains a maximum external quantum efficiency (EQE) of 10.4%, which is the highest among similar devices. This work shows that it is possible to prepare high‐efficiency near‐infrared PeLEDs in air‐ambient through a simple method.
Promoting Mechanistic Understanding of Lithium Deposition and Solid‐Electrolyte Interphase (SEI) Formation Using Advanced Characterization and Simulation Methods: Recent Progress, Limitations, and Future Perspectives
Authors: Xu Yaolin , Dong Kang , Jie Yulin , Adelhelm Philipp , Chen Yawei , Xu Liang , Yu Peiping , Kim Junghwa , Kochovski Zdravko , Yu Zhilong , Li Wanxia , LeBeau James , Shao‐Horn Yang , Cao Ruiguo , Jiao Shuhong , Cheng Tao , Manke Ingo , Lu Yan 
Published: March 2022

AbstractIn recent years, due to its great promise in boosting the energy density of lithium batteries for future energy storage, research on the Li metal anode, as an alternative to the graphite anode in Li‐ion batteries, has gained significant momentum. However, the practical use of Li metal anodes has been plagued by unstable Li (re)deposition and poor cyclability. Although tremendous efforts have been devoted to the stabilization of Li metal anodes, the mechanisms of electrochemical (re‐)deposition/dissolution of Li and solid‐electrolyte‐interphase (SEI) formation remain elusive. This article highlights the recent mechanistic understandings and observations of Li deposition/dissolution and SEI formation achieved from advanced characterization techniques and simulation methods, and discusses major limitations and open questions in these processes. In particular, the authors provide their perspectives on advanced and emerging/potential methods for obtaining new insights into these questions. In addition, they give an outlook into cutting‐edge interdisciplinary research topics for Li metal anodes. It pushes beyond the current knowledge and is expected to accelerate development toward a more in‐depth and comprehensive understanding, in order to guide future research on Li metal anodes toward practical application.
Synthesis of Chiral Endocyclic Allenes by Palladium‐Catalyzed Asymmetric Annulation Followed by Cope Rearrangement
Authors: Shi Bin , Liu Jia‐Bin , Wang Ze‐Tian , Wang Liang , Lan Yu , Lu Liang‐Qiu , Xiao Wen‐Jing 
Published: March 2022

AbstractCatalytic asymmetric synthesis of chiral endocyclic allenes remains a challenge in allene chemistry owing to unfavored tension and complex chirality. Here, we present a new relay strategy merging Pd‐catalyzed asymmetric [3+2] annulation with enyne‐Cope rearrangement, providing a facile route to chiral 9‐membered endocyclic allenes with high efficiency and enantioselectivity. Moreover, theoretical calculations and experimental studies were performed to illustrate the critical, but unusual Cope rearrangement that allows for the complete central‐to‐axial chirality transfer.
A Bacteria‐Responsive Porphyrin for Adaptable Photodynamic/Photothermal Therapy
Authors: Hu Hao , Wang Hua , Yang Yuchong , Xu Jiang‐Fei , Zhang Xi 
Published: March 2022

AbstractWe report a cationic porphyrin 5,10,15,20‐tetrakis‐(4‐N‐methylpyridyl)‐porphyrin (TMPyP) that can respond to specific bacteria, followed by adaptable photodynamic/photothermal therapy processes. TMPyP could be reduced to phlorin by facultative anaerobes with a strong reducing ability such as E. coli and S. typhimurium in hypoxic environments, possessing strong NIR absorption and remarkable photothermal conversion capacity, thus demonstrating excellent antimicrobial activity (>99 %) by photothermal therapy. While in an aerobic environment with aerobic bacteria, TMPyP functioned as a typical photosensitizer that killed bacteria effectively (>99.9 %) by photodynamic therapy. By forming a host–guest complex with cucurbit[7]uril, the biocompatibility of TMPyP significantly improved. This kind of bacteria‐responsive porphyrin shows specificity and adaptivity in antimicrobial treatment and holds potential in non‐invasive treatments of bacterial infections.
Reducing Energy Disorder for Efficient and Stable Sn−Pb Alloyed Perovskite Solar Cells.
Authors: Peng Cheng , Li Chongwen , Zhu Mingzhe , Zhang Chujun , Jiang Xiafei , Yin Hang , He Benlin , Li Haiyan , Li Ming , So Shu Kong , Zhou Zhongmin 
Published: March 2022

AbstractSn−Pb alloyed perovskites have drawn considerable attention because of their appropriate band gap for both single‐junction and multi‐junction tandem photovoltaics, but the easy‐formation of energy disorder still limits their practical applications. Here, we report that the combination of 1‐bromo‐4‐(methylsulfinyl) benzene (BBMS) and SnF2 greatly reduced the Urbach energy of perovskite films, and largely restrained the oxidation of Sn2+. With the help of density functional theory calculations, we clarified the interactions between BBMS and perovskite were responsible for the improvements. As a result, a high efficiency of >22 % was obtained for the Sn−Pb alloy‐based solar cells treated by BBMS and SnF2. More importantly, the BBMS‐treated devices demonstrated outstanding stability, retaining 98 % of its original efficiency after heating at 60 °C for 2660 h under N2.
Enantioselective Total Synthesis of [3]‐Ladderanol through Late‐Stage Organocatalytic Desymmetrization**
Authors: Ray Sayan , Mondal Subhajit , Mukherjee Santanu 
Published: March 2022

AbstractLadderane phospholipids, with their unusual ladder‐like arrangement of concatenated cyclobutane rings, represent an architecturally unique class of natural products. However, despite their fascinating structure and other necessary impetus, only a few synthetic studies of these molecules have been reported so far. We have now devised a concise total synthesis of [3]‐ladderanol, a component of natural ladderane phospholipids, using an organocatalytic enantioselective desymmetrizing formal C(sp2)−H alkylation. Our synthetic strategy rests on the late‐stage introduction of chirality, thus allowing facile access to both enantiomers of [3]‐ladderanol as well as an analogue. This is the first time a desymmetrization strategy is applied to the synthesis of [3]‐ladderanol. The scope of this desymmetrizing C(sp2)−H alkylation of meso‐cyclobutane‐fused cyclohexenediones is also presented.
Sustained Release of a Synthetic Autoinducing Peptide Mimetic Blocks Bacterial Communication and Virulence In Vivo.
Authors: West Korbin H. J. , Gahan Curran G. , Kierski Patricia R. , Calderon Diego F. , Zhao Ke , Czuprynski Charles J. , McAnulty Jonathan F. , Lynn David M. , Blackwell Helen E. 
Published: March 2022

AbstractThere is significant interest in approaches to the treatment of bacterial infections that block virulence without creating selective pressures that lead to resistance. Here, we report the development of an “anti‐virulence” strategy that exploits the activity of potent synthetic inhibitors of quorum sensing (QS) in Staphylococcus aureus. We identify peptide‐based inhibitors of QS that are resistant to sequestration or degradation by components of murine tissue and demonstrate that encapsulation of a lead inhibitor in degradable polymer microparticles provides materials that substantially inhibit QS in vitro. Using a murine abscess model, we show that this inhibitor attenuates methicillin‐resistant S. aureus (MRSA) skin infections in vivo, and that sustained release of the inhibitor from microparticles significantly improved outcomes compared to mice that received a single‐dose bolus. Our results present an effective and modular approach to controlling bacterial virulence in vivo and could advance the development of new strategies for skin infection control.
A Strategy Based on Aggregation‐Induced Ratiometric Emission to Differentiate Molecular Weight of Supramolecular Polymers
Authors: Liu Hui , Hu Ziqing , Zhang Hanwei , Li Qingyun , Lou Kai , Ji Xiaofan 
Published: March 2022

AbstractMolecular weight has an important bearing on the properties of supramolecular polymers. However, the intuitive differentiation of the molecular weight of supramolecular polymers remains challenging. Given this situation, establishing a reliable relationship between fluorescence properties and molecular weight may be a promising strategy. Herein, we prepared a supramolecular monomerM1with aggregation‐induced ratiometric emission characteristics. With the increasingM1concentration (0.100–100 mM), the average degree of polymerization (DPDOSY) rose from 1.00 to 293. Meanwhile, the color changed from dark blue to cyan, finally to yellow‐green in the same concentration range. Hence, the intuitive relationship between DPDOSYand fluorescence colors was constructed, allowing the visual differentiation of molecular weight. Moreover, the fluorescence color could be regulated by introducing a competitive molecule to induce the depolymerization of supramolecular polymers.
Heterocyclic Conjugated Polymer Nanoarchitectonics with Synergistic Redox‐Active Sites for High‐Performance Aluminium Organic Batteries
Authors: Peng Xiyue , Xie Yuan , Baktash Ardeshir , Tang Jiayong , Lin Tongen , Huang Xia , Hu Yuxiang , Jia Zhongfan , Searles Debra J. , Yamauchi Yusuke , Wang Lianzhou , Luo Bin 
Published: March 2022

AbstractThe development of cost‐effective and long‐life rechargeable aluminium ion batteries (AIBs) shows promising prospects for sustainable energy storage applications. Here, we report a heteroatom π‐conjugated polymer featuring synergistic C=O and C=N active centres as a new cathode material in AIBs using a low‐cost AlCl3/urea electrolyte. Density functional theory (DFT) calculations reveal the fused C=N sites in the polymer not only benefit good π‐conjugation but also enhance the redox reactivity of C=O sites, which enables the polymer to accommodate four AlCl2(urea)2+ per repeating unit. By integrating the polymer with carbon nanotubes, the hybrid cathode exhibits a high discharge capacity and a long cycle life (295 mAh g−1 at 0.1 A g−1 and 85 mAh g−1 at 1 A g−1 over 4000 cycles). The achieved specific energy density of 413 Wh kg−1 outperforms most Al–organic batteries reported to date. The synergistic redox‐active sites strategy sheds light on the rational design of organic electrode materials.
Direct Amination of Benzene with Molecular Nitrogen Enabled by Plasma‐Liquid Interactions
Authors: Xu Xia , Zhao Xuyang , Tang Jie , Duan Yixiang , Tian Yong‐Hui 
Published: March 2022

AbstractNitrogen fixation is industrially realized by mass production of ammonia, the principal intermediate nitrogen source for N‐containing organic molecules. Instead, direct C−N bond formation from dinitrogen (N2) is of great interest but remains a challenge. Here, by virtue of unique plasma–liquid interactions, we developed an environmentally benign one‐pot approach to directly couple benzene and N2, two naturally abundant yet chemically inert molecules, into value‐added arylamines. Under the optimal conditions, an amination yield of 45 % was rapidly achieved, far better than the reported benzene amination efficiency using ammonia. A tentative reaction mechanism was proposed involving the long‐lived N2 (A3
) and N2+ species, as evidenced by the key intermediates detected. With a deeper mechanistic understanding and by further optimizing the plasma reactor, the realization of cost‐effective electrical amination of benzene with N2 could become reality.
Halogen⋅⋅⋅Halogen and Halogen⋅⋅⋅π Interactions Enabled Reversible Photo‐oligomerization of Conjugated Dienones: Visible Light Triggered Single‐Crystal‐to‐Single‐Crystal Transformation
Authors: Naskar Sandip , Moi Rajib , Das Indrajit , Biradha Kumar 
Published: March 2022

AbstractThe synthesis of reversible oligomer/polymers is fascinating both from the perspective of the fundamental understanding as well as their applications, ranging from biomedical to self‐healing smart materials. On the other hand, the reactions that occur in single‐crystal‐to‐single‐crystal (SCSC) fashion offer great details of the structure, geometry and stereochemistry of the product. However, SCSC [2+2] oligomerization is rather difficult and rare. Further, till date there are no reports for a reversible [2+2] oligomerization in SCSC fashion. In this work, four halogen‐substituted acrylic dienone molecules were deliberately designed and their ability to participate in [2+2] cycloaddition reaction in solid state was studied under visible light. Despite of having the required alignment of double bonds of dienes in all four crystal structures, they were found to exhibit variable reactivities given the differences in their weak intermolecular interactions such as halogen⋅⋅⋅halogen, halogen⋅⋅⋅π and C−H⋅⋅⋅O interactions. Notably, one of these materials exhibits reversible oligomerization in a SCSC manner.
Under‐5‐Minute Immunoblot Assays by Vortex Fluidic Device Acceleration
Authors: Sanders Emily C. , Sen Sanjana R. , Gelston Aidan A. , Santos Alicia M. , Luo Xuan , Bhuvan Keertna , Tang Derek Y. , Raston Colin L. , Weiss Gregory A. 
Published: March 2022

AbstractUnlocking the potential of personalized medicine in point‐of‐care settings requires a new generation of biomarker and proteomic assays. Ideally, assays could inexpensively perform hundreds of quantitative protein measurements in parallel at the bedsides of patients. This goal greatly exceeds current capabilities. Furthermore, biomarker assays are often challenging to translate from benchtop to clinic due to difficulties achieving and assessing the necessary selectivity, sensitivity, and reproducibility. To address these challenges, we developed an efficient (<5 min), robust (comparatively lower CVs), and inexpensive (decreasing reagent use and cost by >70 %) immunoassay method. Specifically, the immunoblot membrane is dotted with the sample and then developed in a vortex fluidic device (VFD) reactor. All assay steps—blocking, binding, and washing—leverage the unique thin‐film microfluidics of the VFD. The approach can accelerate direct, indirect, and sandwich immunoblot assays. The applications demonstrated include assays relevant to both the laboratory and the clinic.
Enantioselective Tail‐to‐Head Terpene Cyclizations by Optically Active Hexameric Resorcin[4]arene Capsule Derivatives
Authors: Sokolova Daria , Piccini GiovanniMaria , Tiefenbacher Konrad 
Published: March 2022

AbstractMolecular capsules enable the conversion of substrates inside a closed cavity, mimicking to some extent enzymatic catalysis. Chirality transfer from the molecular capsule onto the encapsulated substrate has been only studied in a few cases. Here we demonstrate that chirality transfer is possible inside a rather large molecular container of approximately 1400 Å3. Specifically, we present 1) the first examples of optically active hexameric resorcin[4]arene capsules, 2) their ability to enantioselectively catalyze tail‐to‐head terpene cyclizations, and 3) the surprisingly high sensitivity of enantioselectivity on the structural modifications.
Enhanced thermally conductive TPU/graphene filaments for 3D printing produced by melt compounding
Authors: Maldonado Mário P. , Pinto Gabriel M. , Costa Lidiane Cristina , Fechine Guilhermino J. M. 
Published: March 2022

AbstractConducting polymers are a potential solution to the issue of wide‐range manufacture of flexible electronics, since many polymers are suitable to advanced fabrication methods, such as fused deposition modeling (FDM) 3D printing. Therefore, it is proposed in this work a ductile thermoplastic polyurethane (TPU)/graphene nanocomposite with enhanced thermal conductivity that would be suitable for additive manufacturing processes. The nanocomposites were produced by melt compounding technique, which does not require the use of toxic solvents and is characteristic of being used by the thermoplastic industry. The filaments were then analyzed in terms of graphene dispersion, microstructural changes, mechanical behavior, and thermal conductivity. It was verified that graphene does not have a good interaction with the TPU matrix, presenting voids at the interface and forming agglomerates at higher contents. However, it was able to affect the TPU's hard segments organization, leading to a more ordered structure up to 1.0 wt%. Consequently, the thermal conductivity was enhanced up to the graphene concentration by about 14% in relation to neat TPU. Additionally, even though the system presented a poor interface, no mechanical properties were lost, that is, the composite remained ductile even after graphene insertion, which is extremely interesting for additive manufacturing processes.
Abundance and effect of health status on apparent survival of Guiana dolphins,Sotalia guianensis, in an open embayment in north‐eastern Brazil
Authors: de Meirelles Ana Carolina Oliveira , Choi‐Lima Katherine Fiedler , Vila Nova Thaís Moura Campos , Monteiro‐Filho Emygdio Leite de Araujo , Lotufo Tito Monteiro da Cruz 
Published: March 2022

AbstractGuiana dolphins (Sotalia guianensis) inhabit shallow waters of the tropical western Atlantic, an area that is now mostly occupied by cities and harbours. Demographic studies have been concentrated in sheltered areas of south/south‐eastern Brazil.This study investigated site fidelity and estimated population abundance and apparent survival of Guiana dolphins in Mucuripe Embayment (ME), on the north‐eastern Brazilian coast, through photo‐identification surveys and closed and open population mark–recapture models, from October 2009 to September 2011.Forty‐six Guiana dolphin groups were recorded (in groups of between one and eight dolphins, with a mean ± SD of 3.49 ± 2.33) in 27 out of 40 surveys. Twenty‐five animals were photo‐identified, with eight considered to have a ‘poor health’ status. The standardized site fidelity index (SSFI) was low (0.25).Using the programcapture, the time and heterogeneity model (Mth) resulted in a total abundance estimate of 39, with a Coefficient of Variation (CV) of 21% (95% CI 35–80%). Inprogram mark, model averaging resulted in a total abundance estimate of 33 (CV 32%, 95% CI 30–100%). Using a CV of 21%, the power to detect a decline of 50% during the study period was 0.44 and the power to detect a decline of 5% a year was 0.11. To detect these declines with a 0.90 power, 12 years of monitoring would be necessary.The annual adult apparent survival rate was low (0.71; CV 19%; 95% CI 0.40–0.90), and differed for dolphins in ‘good’ (0.64; CV 28%, 95% CI 0.27–0.89) and ‘poor’ (0.85; CV 22%; 95% CI: 0.23–0.99) health.The low abundance of Guiana dolphins in ME indicates that conservation actions should start immediately, such as creating a marine protected area, continuing awareness campaigns, using by‐catch reduction technologies, developing new regulations, and promoting law enforcement. Monitoring studies must continue with increased effort to reduce uncertainty in estimates and to improve the power to detect trends of decline.
Synergistic effect of compounds directed to triosephosphate isomerase, a combination to develop drug against trichomoniasis
Authors: Benítez‐Cardoza Claudia G. , Brieba Luis G. , Arroyo Rossana , Rojo‐Domínguez Arturo , Vique‐Sánchez José L. 
Published: March 2022

AbstractThe development of new drugs is continuous in the world; currently, saving resources (both economic ones and time) and preventing secondary effects have become a necessity for drug developers. Trichomoniasis is the most common nonviral sexually transmitted infection affecting more than 270 million people around the world. In our research group, we focussed on developing a selective and more effective drug againstTrichomonas vaginalis, and we previously reported on a compound, calledA4, which had a trichomonacidal effect. Later, we determined another compound, calledD4, which also had a trichomonacidal effect together with favorable toxicity results. BothA4andD4are directed at the enzyme triosephosphate isomerase. Thus, we made combinations between the two compounds, in which we determined a synergistic effect againstT. vaginalis, determining the IC50and the toxicity of the best relationship to obtain the trichomonacidal effect. With these results, we can propose a combination of compounds that represents a promising alternative for the development of a new therapeutic strategy against trichomoniasis.
Small Molecule Inhibitors of Nuclear Export and the Amelioration of Lupus by Modulation of Plasma Cell Generation and Survival
Authors: Rangel‐Moreno Javier , Garcia‐Hernandez Maria de la Luz , Owen Teresa , Barnard Jennifer , Becerril‐Villanueva Enrique , Kashyap Trinayan , Argueta Christian , Gamboa‐Dominguez Armando , Tamir Sharon , Landesman Yosef , Goldman Bruce I. , Ritchlin Christopher T. , Anolik Jennifer H. 
Published: March 2022

ObjectiveTo investigate the hypothesis that selective inhibitors of nuclear export (SINE compounds), recently approved for treatment of refractory plasma cell (PC) malignancy, may have potential in the treatment of lupus.MethodsFemale NZB/NZW mice were treated with the SINE compound KPT‐350 or vehicle control. Tissue specimens were harvested and analyzed by flow cytometry, using standard markers. Nephritis was monitored by determining the proteinuria score and by histologic analysis of kidney specimens. Serum anti–double‐stranded DNA (anti‐dsDNA) levels were measured by enzyme‐linked immunosorbent assay, and total numbers of IgG‐secreting and dsDNA‐specific antibody‐secreting cells were assessed by enzyme‐linked immunospot assay.ResultsKPT‐350 abrogated murine lupus nephritis at both early and late stages of the disease and rapidly impaired generation of autoreactive PCs in germinal centers (GCs). SINE compounds inhibited the production of NF‐κB–driven homeostatic chemokines by stromal cells, altering splenic B and T cell strategic positioning and significantly reducing follicular helper T cell, GC B cell, and autoreactive PC counts. KPT‐350 also decreased levels of cytokines and chemokines involved in PC survival and recruitment in the kidney of lupus‐prone mice. Exportin 1, the target of SINE compounds, was detected in GCs of human tonsils, splenic B cells of lupus patients, and multiple B cell subsets in the kidneys of patients with lupus nephritis.ConclusionCollectively, our results provide support for the therapeutic potential of SINE compounds, via their targeting of several molecular and cellular pathways critical in lupus pathogenesis, including autoantibody production by plasma cells.
GKC‐CI: A unifying framework for contextual norms and information governance
Authors: Shvartzshnaider Yan , Sanfilippo Madelyn Rose , Apthorpe Noah 
Published: March 2022

AbstractPrivacy‐enhancing technologies that incorporate a socially meaningful conception of privacy, one that meets people's expectations and is ethically defensible, need to factor in contextual privacy norms and information governance as part of their design. This involves understanding what information handling practices users deem acceptable, what factors influence users' perceptions and behaviors, and how informational norms evolve. In this paper, we present GKC‐CI, a unifying framework for examining contextual privacy norms and information governance in a given context to help structure research inquiries around these questions.