bluuebunny/crossref_metadata_2025_split huggingface dataset:
Bioinspired Simultaneous Changes in Fluorescence Color, Brightness, and Shape of Hydrogels Enabled by AIEgens
Authors: Li Zhao , Liu Pengchao , Ji Xiaofan , Gong Junyi , Hu Yubing , Wu Wenjie , Wang Xinnan , Peng Hui‐Qing , Kwok Ryan T. K. , Lam Jacky W. Y. , Lu Jian , Tang Ben Zhong 
Published: February 2020

AbstractDevelopment of stimuli‐responsive materials with complex practical functions is significant for achieving bioinspired artificial intelligence. It is challenging to fabricate stimuli‐responsive hydrogels showing simultaneous changes in fluorescence color, brightness, and shape in response to a single stimulus. Herein, a bilayer hydrogel strategy is designed by utilizing an aggregation‐induced emission luminogen, tetra‐(4‐pyridylphenyl)ethylene (TPE‐4Py), to fabricate hydrogels with the above capabilities. Bilayer hydrogel actuators with the ionomer of poly(acrylamide‐r‐sodium 4‐styrenesulfonate) (PAS) as a matrix of both active and passive layers and TPE‐4Py as the core function element in the active layer are prepared. At acidic pH, the protonation of TPE‐4Py leads to fluorescence color and brightness changes of the actuators and the electrostatic interactions between the protonated TPE‐4Py and benzenesulfonate groups of the PAS chains in the active layer cause the actuators to deform. The proposed TPE‐4Py/PAS‐based bilayer hydrogel actuators with such responsiveness to stimulus provide insights in the design of intelligent systems and are highly attractive material candidates in the fields of 3D/4D printing, soft robots, and smart wearable devices.
NIR Light‐Driving Barrier‐Free Group Rotation in Nanoparticles with an 88.3% Photothermal Conversion Efficiency for Photothermal Therapy
Authors: Xi Dongmei , Xiao Ming , Cao Jianfang , Zhao Luyang , Xu Ning , Long Saran , Fan Jiangli , Shao Kun , Sun Wen , Yan Xuehai , Peng Xiaojun 
Published: February 2020

AbstractTraditional photothermal therapy requires high‐intensity laser excitation for cancer treatments due to the low photothermal conversion efficiency (PCE) of photothermal agents (PTAs). PTAs with ultra‐high PCEs can decrease the required excited light intensity, which allows safe and efficient therapy in deep tissues. In this work, a PTA is synthesized with high PCE of 88.3% based on a BODIPY scaffold, by introducing a CF3 “barrier‐free” rotor on the meso‐position (tfm‐BDP). In both the ground and excited state, the CF3 moiety in tfm‐BDP has no energy barrier to rotation, allowing it to efficiently dissipate absorbed (NIR) photons as heat. Importantly, the barrier‐free rotation of CF3 can be maintained after encapsulating tfm‐BDP into polymeric nanoparticles (NPs). Thus, laser irradiation with safe intensity (0.3 W cm−2, 808 nm) can lead to complete tumor ablation in tumor‐bearing mice after intravenous injection of tfm‐BDP NPs. This strategy of “barrier‐free rotation” provides a new platform for future design of PTT agents for clinical cancer treatment.
Photoinduced Trap Passivation for Enhanced Photoluminescence in 2D Organic–Inorganic Hybrid Perovskites
Authors: Song Yiling , Liu Weiwei , Qin Yan , Han Xiaobo , Li Wancai , Li Xiaohong , Long Hua , Li Dehui , Wang Kai , Wang Bing , Lu Peixiang 
Published: February 2020

Abstract2D organic–inorganic hybrid perovskites are promising materials for next‐generation optoelectronic devices. Nevertheless, 2D perovskites still suffer from performance‐limiting trap states and possess fundamental photophysical effects that remain poorly understood. Herein, a photoinduced trap passivation for enhanced photoluminescence (PL) in 2D hybrid perovskites is reported. Under two‐photon excitation, the PL emission of the 2D hybrid perovskites exhibits a gradual increase in intensity and lifetime, due to the photoinduced trap passivation by interacting with oxygen in ambient environment. Interestingly, the PL increase shows distinct features at the surface and in the bulk of the 2D perovskites, which can be well revealed by a photoinduced oxygen‐diffused trap‐passivation model. Moreover, the PL increase and relaxation can recycle for several times, which suggests an excellent repeatability of the photoinduced trap passivation. The photoinduced trap passivation is critical for fundamental study of light–matter interaction in 2D perovskites, and shows great promise for improving the optoelectronic responses for functional devices.
Grain Boundary Enhanced Photoluminescence Anisotropy in Two‐Dimensional Hybrid Perovskite Films
Authors: Wang Min , Tang Ji , Wang Hong , Zhang Chuang , Zhao Yong Sheng , Yao Jiannian 
Published: February 2020

AbstractThe boundaries between crystalline grains in hybrid perovskite films are beneficial for carrier dissociation, and may also serve as recombination centers to alter the photoluminescence property. Herein, it is shown that the grain boundaries can significantly enhance the anisotropy of photoluminescence from two‐dimensional (2D) hybrid perovskite films. The measurement of carrier densities shows that the grain boundaries generate an in‐gap state, which results in an additional red‐shifted photoluminescence band due to its emissive nature. Interestingly, the light emission of the in‐gap state appears only in the direction parallel to the film, corresponding to the in‐plane dipole transition as reveled by the measurement on photoluminescence polarization. These results demonstrate the tunable anisotropic photoluminescence from 2D perovskite materials toward the construction of directionally dependent light sources for advanced display application.
Achieving Highly Efficient Pure Organic Single‐Molecule White‐Light Emitter: The Coenhanced Fluorescence and Phosphorescence Dual Emission by Tailoring Alkoxy Substituents
Authors: Wen Yating , Liu Haichao , Zhang Shitong , Cao Jungang , De Jianbo , Yang Bing 
Published: February 2020

AbstractDeveloping the single‐molecule white‐light emitters (SMWLEs) at room temperature is very challenging for pure organic metal‐free system, and it is even more challenging to achieve the high efficiency of pure organic SMWLE. Here, alkoxy substituents are tailored at 2‐positioned thioxanthone (TX) to finely tune the molecular packing mode and the intermolecular interaction between TX units, and the photoluminescence (PL) efficiency (ΦPL) of SMWLE is improved successfully from 1.5% (TX) to 45.0% (TX‐OCH(CH3)2). This simultaneous enhancement of dual emission between fluorescence and phosphorescence can be ascribed to i) a moderate intersystem crossing (ISC) rate for the equilibrium distribution between singlet and triplet excitons, ii) simultaneously accelerated radiative rates of singlet and triplet excitons due to J‐aggregation of TX units, and iii) effective suppression of nonradiation through strong hydrogen bond interactions by alkoxy chains. As a result, this work provides a novel molecular design strategy to harvest high‐efficiency pure organic SMWLE using a precise manipulation of π–π stacking mode and intermolecular interaction by tailoring alkoxy substituents.
Gut Microbial Signatures Can Discriminate Unipolar from Bipolar Depression
Authors: Zheng Peng , Yang Jian , Li Yifan , Wu Jing , Liang Weiwei , Yin Bangmin , Tan Xunmin , Huang Yu , Chai Tingjia , Zhang Hanping , Duan Jiajia , Zhou Jingjing , Sun Zuoli , Chen Xu , Marwari Subhi , Lai Jianbo , Huang Tingting , Du Yanli , Zhang Peifen , Perry Seth W. , Wong Ma‐Li , Licinio Julio , Hu Shaohua , Xie Peng , Wang Gang 
Published: February 2020

AbstractDiscriminating depressive episodes of bipolar disorder (BD) from major depressive disorder (MDD) is a major clinical challenge. Recently, gut microbiome alterations are implicated in these two mood disorders; however, little is known about the shared and distinct microbial characteristics in MDD versus BD. Here, using 16S ribosomal RNA (rRNA) gene sequencing, the microbial compositions of 165 subjects with MDD are compared with 217 BD, and 217 healthy controls (HCs). It is found that the microbial compositions are different between the three groups. Compared to HCs, MDD is characterized by altered covarying operational taxonomic units (OTUs) assigned to the Bacteroidaceae family, and BD shows disturbed covarying OTUs belonging to Lachnospiraceae, Prevotellaceae, and Ruminococcaceae families. Furthermore, a signature of 26 OTUs is identified that can distinguish patients with MDD from those with BD or HCs, with area under the curve (AUC) values ranging from 0.961 to 0.986 in discovery sets, and 0.702 to 0.741 in validation sets. Moreover, 4 of 26 microbial markers correlate with disease severity in MDD or BD. Together, distinct gut microbial compositions are identified in MDD compared to BD and HCs, and a novel marker panel is provided for distinguishing MDD from BD based on gut microbiome signatures.
Solvent‐Free Synthesis of Thin, Flexible, Nonflammable Garnet‐Based Composite Solid Electrolyte for All‐Solid‐State Lithium Batteries
Authors: Jiang Taoli , He Pingge , Wang Guoxu , Shen Yang , Nan Ce‐Wen , Fan Li‐Zhen 
Published: February 2020

AbstractThin solid‐state electrolytes with nonflammability, high ionic conductivity, low interfacial resistance, and good processability are urgently required for next‐generation safe, high energy density lithium metal batteries. Here, a 3D Li6.75La3Zr1.75Ta0.25O12 (LLZTO) self‐supporting framework interconnected by polytetrafluoroethylene (PTFE) binder is prepared through a simple grinding method without any solvent. Subsequently, a garnet‐based composite electrolyte is achieved through filling the flexible 3D LLZTO framework with a succinonitrile solid electrolyte. Due to the high content of garnet ceramic (80.4 wt%) and high heat‐resistance of the PTFE binder, such a composite electrolyte film with nonflammability and high processability exhibits a wide electrochemical window of 4.8 V versus Li/Li+ and high ionic transference number of 0.53. The continuous Li+ transfer channels between interconnected LLZTO particles and succinonitrile, and the soft electrolyte/electrode interface jointly contribute to a high ambient‐temperature ionic conductivity of 1.2 × 10−4 S cm−1 and excellent long‐term stability of the Li symmetric battery (stable at a current density of 0.1 mA cm−2 for over 500 h). Furthermore, as‐prepared LiFePO4|Li and LiNi0.5Mn0.3Co0.2O2|Li batteries based on the thin composite electrolyte exhibit high discharge specific capacities of 153 and 158 mAh g−1 respectively, and desirable cyclic stabilities at room temperature.
How imidazolium‐based ionic liquids solubilize the poorly soluble ibuprofen? A theoretical study
Authors: Huang Yiping , Ji Yuanhui , Zhang Mao , Ouyang Defang 
Published: February 2020

AbstractMolecular dynamics simulations were performed to study combinations of [AcO]−, [TfO]−, [BF4]−, and [PF6]− anions paired with imidazolium cations of increasing alkyl chain length to elucidate the roles of anions and cations in solvating ibuprofen. Our simulation results revealed that ionic liquids (ILs) with strong ibuprofen solvation capacity should possess strong van der Waals force from cations and strong hydrogen bond (HB) from anions. Accordingly, it was found that ILs containing anions with strong HB acceptability, such as [AcO]− anion, were the best effective solvent for ibuprofen solvation, while the longer alkyl chain in the imidazolium cations decrease the polarity, thus increasing the affinity with ibuprofen. Therefore, it was suggested that the heterocyclic structure of imidazolium cation with moderate polarity and longer alkyl chain is a promising cation candidate, whereas the anions which have a strong HB acceptability and substituents without electron withdrawing groups are beneficial. The obtained results can provide useful information for rational design and selection of new ILs to dissolve insoluble drugs.
Association of saliva 25(OH)D concentration with body composition and proportion among pre‐pubertal and pubertal Polish children
Authors: Pruszkowska‐Przybylska Paulina , Sitek Aneta , Rosset Iwona , Sobalska‐Kwapis Marta , Słomka Marcin , Strapagiel Dominik , Żądzińska Elżbieta , Morling Niels 
Published: February 2020

AbstractObjectivesDue to increasing problems with obesity and vitamin D deficiency among children, studies that tackle both problems together are needed.MethodsData were collected from 182 randomly selected children aged 6‐13 years in primary schools in central Poland. Measures included anthropometric dimensions, body composition, questionnaires completed by participants' parents, and saliva samples. The level of 25(OH)D was assessed from the saliva samples using an enzyme‐linked immunosorbent assay kit. The children were divided into two groups: pre‐pubertal (girls below 10 years and boys below 11 years) and pubertal individuals (girls above 10 years and boys above 11 years).ResultsThe 25(OH)D concentrations were higher in late spring (June) among pre‐pubertal children than in the autumn (November‐December) among pubertal children. The level of 25(OH)D was positively correlated with body cell mass (BCM,%) among all children (pubertal: R = 0.20, P = .044; pre‐pubertal: R = 0.23, P = .041) and inversely associated with waist‐to‐hip ratio (WHR) among pubertal children of both sexes (R = ‑0.25; P = .031). The stepwise regression analysis revealed that investigation in spring (June) and breastfeeding was associated with increased muscle mass (MM, %) (beta = 0.253, P = .003 and beta = 0.225, P = .005, respectively) and total body water (TBW, %) (beta = 0.276, P = .004 and beta = 0.246, P = .011, respectively) and was associated with decreased body mass index (BMI; beta = −0.222, P = .024 and beta = −0.269, P = .009, respectively) and fat mass (%) (beta = −0.288, P = .003 and beta = −0.266, P = .005, respectively).ConclusionsSeason of salivary sampling and breastfeeding status were more strongly associated with body components, BMI and WHR, than 25(OH)D concentrations.
Why is low body fat rarely seen in large‐sized male athletes?
Authors: Abe Takashi , Bell Zachary W. , Wong Vickie , Spitz Robert W. , Loenneke Jeremy P. 
Published: February 2020

AbstractObjectivesIt is unknown why low body fat is rarely seen in large‐sized athletes (>100 kg body mass). The aim of this review was to examine the relationship between body mass and body composition (fat mass and fat‐free mass) in elite male athletes, and to discuss the possible reasons why low body fat is rarely seen in large‐sized male athletes.MethodsA search using two electronic databases was conducted. Eighteen studies estimated body composition in elite athletes by dual‐energy X‐ray absorptiometry, totaling 2249 elite male athletes and 72 data points.ResultsOur results indicated that low body fat (eg, less than 10% body fat) was rarely seen in large‐sized male athletes over 100 kg body mass. The larger the body mass, the higher the fat‐free mass, with fat‐free mass leveling off when body mass exceeds approximately 120 kg.ConclusionPossible reasons for this are unknown but we provide some ideas for why this might occur. The two different stages to consider with respect to skeletal muscle growth: the amount of growth during development and the amount of growth as a result of long‐term resistance training. In certain sporting events, a large body mass may be favored. However, the large‐sized athletes have to balance any potential positive influence of body mass on sports performance with the potential negative factors associated with body fat accumulation. Further research is warranted, as there is currently limited evidence on this topic.
A phenotypically severe, biochemically “silent” case of HIBCH deficiency in a newborn diagnosed by rapid whole exome sequencing and enzymatic testing
Authors: D'Gama Alissa M. , Brucker William J. , Zhang Tian , Gubbels Cynthia S. , Ferdinandusse Sacha , Shi Jiahai , Grant Patricia Ellen , VanNoy Grace , Genetti Casie A. , Juusola Jane , Yu Timothy W. , Kritzer Amy , Agrawal Pankaj B. 
Published: February 2020

Abstract3‐Hydroxyisobutyryl‐CoA dehydrogenase (HIBCH) deficiency is a rare error in valine catabolism associated with a Leigh syndrome‐like phenotype, mitochondrial dysfunction, and increased C4‐OH. We report the most severe case to date in a full‐term female who presented with poor feeding and nystagmus on day of life (DOL) 1. Although initial neuroimaging findings were concerning for metabolic disease, further metabolic testing was nondiagnostic and she was discharged on DOL 18. She was readmitted on DOL 22 after severe apneic episodes requiring intubation, with EEG demonstrating multifocal seizures and MRI/MRS demonstrating worsening findings. Care was withdrawn DOL 27 and she expired. Rapid whole exome sequencing (WES) demonstrated compound heterozygous variants in HIBCH with a paternal pathogenic variant (c.852delA, p.L284FfsX10) and a maternal likely pathogenic variant (c.488G>T, p.C163F). Fibroblast enzymatic testing demonstrated marked reduction in HIBCH levels. This case demonstrates the importance of rapid WES and follow‐up functional testing in establishing a diagnosis when metabolic disease is suspected but lacks an expected biochemical signature.
Unexpected effects of systemic steroids on the CRSwNP proteome: is protein upregulation more important than inhibition?
Authors: Workman Alan D. , Miyake Michelle M. , Nocera Angela L. , Mueller Sarina K. , Finn Kristen , Otu Hasan H. , Libermann Towia A. , Bleier Benjamin S. 
Published: February 2020

BackgroundOral steroids, traditionally thought of as immunosuppressive agents that are broad in their immunomodulatory effects, are a mainstay of treatment to reduce disease burden in chronic rhinosinusitis with nasal polyps (CRSwNP). The purpose of this study was to determine how differentially expressed proteins in CRSwNP are affected by oral steroid therapy.MethodsMatched exosomal proteomic arrays were quantified using aptamer‐based methods in systemic steroid‐naive CRSwNP patients before and after a standardized oral prednisone course (n = 12). Previously identified differentially expressed proteins in CRSwNP patients were compared to determine the effect of steroids on expression. Fisher's exact test and t test were applied to normalized protein expression profiles to determine significance.ResultsOf 18 proteins previously identified to be highly underexpressed in CRSwNP, 16 (89%) had an average increase after systemic steroid treatment (p < 0.05). Lactoperoxidase, initially present at 9‐fold lower concentrations in CRSwNP subjects, increased by 209% after steroid treatment. A similar trend was observed with other proteins of interest, including platelet factor 4 and C‐C motif ligand 28. The converse of this steroid effect was not true; of the 53 proteins that are highly overexpressed in CRSwNP, only 22 (42%) decreased in quantity with steroid use.ConclusionProteomic analysis of differentially expressed proteins in CRSwNP demonstrates that systemic steroids cause almost uniform upregulation of transcriptionally decreased proteins, whereas the effects of steroids on transcriptionally increased proteins are more heterogeneous. Thus, proteomic analysis may be an effective tool to understand specific therapeutic benefits of steroid use in polyp disease and to create more targeted treatments.
General Strategy for Synthesis of Ordered Pt3M Intermetallics with Ultrasmall Particle Size
Authors: Zhang Bentian , Fu Gengtao , Li Yutao , Liang Lecheng , Grundish Nicholas S. , Tang Yawen , Goodenough John B. , Cui Zhiming 
Published: February 2020

AbstractControllable synthesis of atomically ordered intermetallic nanoparticles (NPs) is crucial to obtain superior electrocatalytic performance for fuel cell reactions, but still remains arduous. Herein, we demonstrate a novel and general hydrogel‐freeze drying strategy for the synthesis of reduced graphene oxide (rGO) supported Pt3M (M=Mn, Cr, Fe, Co, etc.) intermetallic NPs (Pt3M/rGO‐HF) with ultrasmall particle size (about 3 nm) and dramatic monodispersity. The formation of hydrogel prevents the aggregation of graphene oxide and significantly promotes their excellent dispersion, while a freeze‐drying can retain the hydrogel derived three‐dimensionally (3D) porous structure and immobilize the metal precursors with defined atomic ratio on GO support during solvent sublimation, which is not afforded by traditional oven drying. The subsequent annealing process produces rGO supported ultrasmall ordered Pt3M intermetallic NPs (≈3 nm) due to confinement effect of 3D porous structure. Such Pt3M intermetallic NPs exhibit the smallest particle size among the reported ordered Pt‐based intermetallic catalysts. A detailed study of the synthesis of ordered intermetallic Pt3Mn/rGO catalyst is provided as an example of a generally applicable method. This study provides an economical and scalable route for the controlled synthesis of Pt‐based intermetallic catalysts, which can pave a way for the commercialization of fuel cell technologies.
Heterologous Expression and Engineering of the Nitrogenase Cofactor Biosynthesis Scaffold NifEN
Authors: Solomon Joseph B. , Lee Chi Chung , Jasniewski Andrew J. , Rasekh Mahtab F. , Ribbe Markus W. , Hu Yilin 
Published: February 2020

AbstractNifEN plays a crucial role in the biosynthesis of nitrogenase, catalyzing the final step of cofactor maturation prior to delivering the cofactor to NifDK, the catalytic component of nitrogenase. The difficulty in expressing NifEN, a complex, heteromultimeric metalloprotein sharing structural/functional homology with NifDK, is a major challenge in the heterologous expression of nitrogenase. Herein, we report the expression and engineering of Azotobacter vinelandii NifEN in Escherichia coli. Biochemical and spectroscopic analyses demonstrate the integrity of the heterologously expressed NifEN in composition and functionality and, additionally, the ability of an engineered NifEN variant to mimic NifDK in retaining the matured cofactor at an analogous cofactor‐binding site. This is an important step toward piecing together a viable pathway for the heterologous expression of nitrogenase and identifying variants for the mechanistic investigation of this enzyme.
Semisynthetic and Enzyme‐Mediated Conjugate Preparations Illuminate the Ubiquitination‐Dependent Aggregation of Tau Protein
Authors: Munari Francesca , Barracchia Carlo G. , Franchin Cinzia , Parolini Francesca , Capaldi Stefano , Romeo Alessandro , Bubacco Luigi , Assfalg Michael , Arrigoni Giorgio , D'Onofrio Mariapina 
Published: February 2020

AbstractIn the brain of individuals with Alzheimer's disease, the regulatory protein ubiquitin is found conjugated to different lysine residues of tau protein assembled into pathological paired helical filaments. To shed light on the hitherto unexplored ubiquitination‐linked conformational transitions of tau, the availability of in vitro ubiquitin conjugation methods is of primary importance. In our work, we focused on the four‐repeat domain of tau and assembled an enzymatic machinery formed by UBE1, Ubc13, and CHIP enzymes. The enzymatic reaction resulted in monoubiquitination at multiple sites, reminiscent of the ubiquitination pattern observed in vivo. We further exploited chemoselective disulfide coupling reactions to construct three tau regioisomers with site‐specific monoubiquitination. Protein aggregation experiments revealed that the multiple enzyme‐derived products were unable to convert into amyloid fibrils, while the semisynthetic conjugates exhibited diverse capability to form filaments. This study contributes novel insight into the effects of a key post‐translational modification on aberrant protein self‐assembly.