bluuebunny/crossref_metadata_2025_split huggingface dataset:
Towards Translation of PqsR Inverse Agonists: From In Vitro Efficacy Optimization to In Vivo Proof‐of‐Principle
Authors: Hamed Mostafa M. , Abdelsamie Ahmed S. , Rox Katharina , Schütz Christian , Kany Andreas M. , Röhrig Teresa , Schmelz Stefan , Blankenfeldt Wulf , Arce‐Rodriguez Alejandro , Borrero‐de Acuña José Manuel , Jahn Dieter , Rademacher Jessica , Ringshausen Felix C. , Cramer Nina , Tümmler Burkhard , Hirsch Anna K. H. , Hartmann Rolf W. , Empting Martin 
Published: January 2023

AbstractPseudomonas aeruginosa (PA) is an opportunistic human pathogen, which is involved in a wide range of dangerous infections. It develops alarming resistances toward antibiotic treatment. Therefore, alternative strategies, which suppress pathogenicity or synergize with antibiotic treatments are in great need to combat these infections more effectively. One promising approach is to disarm the bacteria by interfering with their quorum sensing (QS) system, which regulates the release of various virulence factors as well as biofilm formation. Herein, this work reports the rational design, optimization, and in‐depth profiling of a new class of Pseudomonas quinolone signaling receptor (PqsR) inverse agonists. The resulting frontrunner compound features a pyrimidine‐based scaffold, high in vitro and in vivo efficacy, favorable pharmacokinetics as well as clean safety pharmacology characteristics, which provide the basis for potential pulmonary as well as systemic routes of administration. An X‐ray crystal structure in complex with PqsR facilitated further structure‐guided lead optimization. The compound demonstrates potent pyocyanin suppression, synergizes with aminoglycoside antibiotic tobramycin against PA biofilms, and is active against a panel of clinical isolates from bronchiectasis patients. Importantly, this in vitro effect translated into in vivo efficacy in a neutropenic thigh infection model in mice providing a proof‐of‐principle for adjunctive treatment scenarios.
A Zinc‐ and Calcium‐Rich Lysosomal Nanoreactor Rescues Monocyte/Macrophage Dysfunction under Sepsis
Authors: Zhao Qin , Gong Zijian , Wang Jiaolong , Fu Liangliang , Zhang Jing , Wang Can , Miron Richard J. , Yuan Quan , Zhang Yufeng 
Published: January 2023

AbstractSepsis is a dysregulation of the immune response to pathogens and has high morbidity and mortality worldwide. However, the unclear mapping and course of dysregulated immune cells currently hinders the development of advanced therapeutic strategies to treat sepsis. Here, evidence is provided using single‐cell RNA sequencing from peripheral blood mononuclear cells in sepsis that pathogens attacking monocytes/macrophages disrupt their immune function. The results reveal an enormous decline in monocytes/macrophages in sepsis and chart the evolution of their impaired phagocytosis (Pha) capabilities. Inspired by these findings, nanoparticles, named “Alpha‐MOFs,” are developed that target dysfunctional monocytes/macrophages to actively (A) lift (L) Pha by the release of lysosome‐sensitive ions from a mineralized metal–organic framework (MOF). Alpha‐MOFs have good stability and biosafety in peripheral blood and efficiently targeted monocytes/macrophages. They also release calcium and zinc ions into monocyte/macrophage lysosomes to promote the Pha and degradation of bacteria. Taken together, these results suggest that Alpha‐MOFs rescue monocytes/macrophages dysfunction and effectively improve their survival rate during sepsis.
A Multifunctional Integrated Metal‐Free MRI Agent for Early Diagnosis of Oxidative Stress in a Mouse Model of Diabetic Cardiomyopathy
Authors: Nie Zhuang , Zhang Kun , Chen Xinyu , Wang Jingxin , Gao Huile , Zheng Bingwen , Wu Qihong , Guo Yingkun , Liu Xiangyang , Wang Xu 
Published: January 2023

AbstractReactive oxygen species (ROS) are closely associated with the progression of diabetic cardiomyopathy (DCM) and can be regarded as one of its early biomarkers. Magnetic resonance imaging (MRI) is emerging as a powerful tool for the detection of cardiac abnormalities, but the sensitive and direct ROS‐response MRI probe remains to be developed. This restricts the early diagnosis of DCM and prevents timely clinical interventions, resulting in serious and irreversible pathophysiological abnormalities. Herein, a novel ROS‐response contrast‐enhanced MRI nanoprobe (RCMN) is developed by multi‐functionalizing fluorinated carbon nanosheets (FCNs) with multi‐hydroxyl and 2,2,6,6‐tetramethylpiperidin‐1‐oxyl groups. RCMNs capture ROS and then gather in the heart provisionally, which triggers MRI signal changes to realize the in vivo detection of ROS. In contrast to the clinical MRI agents, the cardiac abnormalities of disease mice is detected 8 weeks in advance with the assistance of RCMNs, which greatly advances the diagnostic window of DCM. To the best of the knowledge, this is the first ROS‐response metal‐free T2‐weighted MRI probe for the early diagnosis of DCM mice model. Furthermore, RCMNs can timely scavenge excessively produced ROS to alleviate oxidative stress.
Impact of Charge Carrier Injection/Extraction Performances in Low‐Dimension PEDOT:PSS Organic Electrochemical Transistors
Authors: Sych Galyna , Rannou Patrice , Jullien‐Palletier Maxime , Sadki Saïd , Bonnassieux Yvan , Sanaur Sébastien 
Published: January 2023

AbstractOrganic electrochemical transistors (OECT) are gaining momentum in future applications of biosensors and bioelectronics. Nonetheless, contact (or series) resistances (RS/D) remain underexplored, even though physical processes between the source/drain electrodes and organic mixed ionic‐electron conductors (OMIECs) drive a substantial part of their performances. To address this shortcoming, in this study, low‐dimension OECTs featuring 2 µm‐long poly(3,4‐ethylenedioxythiophene) and polystyrene sulfonate acid (PEDOT:PSS) channel are explored. Normalized contact resistances (RS/D⋅W) values as low as 1.4 W cm are obtained. It is observed that channel PEDOT:PSS thickness is not detrimental to RS/D but is impacting the cut‐off frequency. A figure‐of‐merit (h) expressing the charge‐carrier injection (or extraction, respectively) efficiency shows that planar depletion‐mode OECTs are not contact‐limited up to L = 30 µm channel length. Finally, an unprecedented approach that highlight the importance of optimizing the micro‐fabrication technologies is shown, by decreasing the contact overlap length, according to OMIECs physicochemical contact properties. Indeed, a transfer‐length method coupled to a current‐crowding model allow to fully understand the behavior of low‐dimension PEDOT:PSS OECTs and next, to optimize its circuits design. This is paving the way toward the development of OECTs‐based integrated circuits with faster switching speed, broadening further their scopes and future use as advanced bioelectronics platforms.
The imperative to support Black youths in resisting low and limiting expectations
Authors: Debrosse Régine , Touré Kapo Leslie , Métayer Karen 
Published: January 2023

AbstractHarmful narratives circulate about Black youths in North America. Deficit narratives portray them, their culture, and their communities as problems, narratives about policing encourage their control and punishment, color‐evasive narratives ignore how race shapes their experiences, and essentialist narratives erase their distinct and often intersectional experiences by presenting them as monolithic. Community psychology and allied fields do not escape these trends, which in turn infuse practice, research, and teaching involving Black youths. The present paper highlights four principles that community psychology and allied fields can adopt to support Black youths in resisting these negative and narrow narratives. They are: (1) emphasizing Black youths' and Black communities' strengths, (2) supporting their agency, (3) adopting culturally relevant practices, and (4) developing critical consciousness through reflections on and deconstruction of these narratives. We hope that the reflections shared in this paper will expand the perspectives infused by researchers and practitioners in community psychology, social work, urban studies, and allied fields who work with Black youths.
Atrophy of the Cholinergic Basal Forebrain can Detect Presynaptic Cholinergic Loss in Parkinson's Disease
Authors: Ray Nicola J. , Kanel Prabesh , Bohnen Nicolaas I. 
Published: January 2023

ObjectivesStructural imaging of the cholinergic basal forebrain may provide a biomarker for cholinergic system integrity that can be used in motor and non‐motor outcome studies in Parkinson's disease. However, no prior studies have validated these structural metrics with cholinergic nerve terminal in vivo imaging in Parkinson's disease. Here, we correlate cholinergic basal forebrain morphometry with the topography of vesicular acetylcholine transporter in a large Parkinson's sample.Methods[18F]‐Fluoroethoxybenzovesamicol vesicular acetylcholine transporter positron emission tomography was carried out in 101 non‐demented people with Parkinson's (76.24% male, mean age 67.6 ± 7.72 years, disease duration 5.7 ± 4.4 years). Subregional cholinergic basal forebrain volumes were measured using magnetic resonance imaging morphometry. Relationships were assessed via volume‐of‐interest based correlation analysis.ResultsSubregional volumes of the cholinergic basal forebrain predicted cholinergic nerve terminal loss, with most robust correlations occurring between the posterior cholinergic basal forebrain and temporofrontal, insula, cingulum, and hippocampal regions, and with modest correlations in parieto‐occipital regions. Hippocampal correlations were not limited to the cholinergic basal forebrain subregion Ch1‐2. Correlations were also observed in the striatum, thalamus, and brainstem.InterpretationCholinergic basal forebrain morphometry is a robust predictor of regional cerebral vesicular acetylcholine transporter bindings, especially in the anterior brain. The relative lack of correlation between parieto‐occipital binding and basal forebrain volumes may reflect the presence of more diffuse synaptopathy in the posterior cortex due to etiologies that extend well beyond the cholinergic system. ANN NEUROL 2023;93:991–998
Stepwise Engineering the Pore Aperture of a Cage‐like MOF for the Efficient Separation of Isomeric C4 Paraffins under Humid Conditions
Authors: Wang Lu , Xue Wenjuan , Zhu Hejin , Guo Xiangyu , Huang Hongliang , Zhong Chongli 
Published: January 2023

AbstractThe separation of isomeric C4 paraffins is an important task in the petrochemical industry, while current adsorbents undergo a trade‐off relationship between selectivity and adsorption capacity. In this work, the pore aperture of a cage‐like Zn‐bzc (bzc=pyrazole‐4‐carboxylic acid) is tuned by the stepwise installation methyl groups on its narrow aperture to achieve both molecular‐sieving separation and high n‐C4H10 uptake. Notably, the resulting Zn‐bzc‐2CH3 (bzc‐2CH3=3,5‐dimethylpyrazole‐4‐carboxylic acid) can sensitively capture n‐C4H10 and exclude iso‐C4H10, affording molecular‐sieving for n‐C4H10/iso‐C4H10 separation and high n‐C4H10 adsorption capacity (54.3 cm3 g−1). Breakthrough tests prove n‐C4H10/iso‐C4H10 can be efficiently separated and high‐purity iso‐C4H10 (99.99 %) can be collected. Importantly, the hydrophobic microenvironment created by the introduced methyl groups greatly improves the stability of Zn‐bzc and significantly eliminates the negative effect of water vapor on gas separation under humid conditions, indicating Zn‐bzc‐2CH3 is a new benchmark adsorbent for n‐C4H10/iso‐C4H10 separation.
Electrochemical Reactivation of Dead Li2S for Li−S Batteries in Non‐Solvating Electrolytes
Authors: Qi Xiaoqun , Yang Fengyi , Sang Pengfei , Zhu Zhenglu , Jin Xiaoyu , Pan Yujun , Ji Jie , Jiang Ruining , Du Haoran , Ji Yongsheng , Fu Yongzhu , Qie Long , Huang Yunhui 
Published: January 2023

AbstractThe use of non‐solvating, or as‐called sparingly‐solvating, electrolytes (NSEs), is regarded as one of the most promising solutions to the obstacles to the practical applications of Li−S batteries. However, it remains a puzzle that long‐life Li−S batteries have rarely, if not never, been reported with NSEs, despite their good compatibility with Li anode. Here, we find the capacity decay of Li−S batteries in NSEs is mainly due to the accumulation of the dead Li2S at the cathode side, rather than the degradation of the anodes or electrolytes. Based on this understanding, we propose an electrochemical strategy to reactivate the accumulated Li2S and revive the dead Li−S batteries in NSEs. With such a facile approach, Li−S batteries with significantly improved cycling stability and accelerated dynamics are achieved with diglyme‐, acetonitrile‐ and 1,2‐dimethoxyethane‐based NSEs. Our finding may rebuild the confidence in exploiting non‐solvating Li−S batteries with practical competitiveness.
Isolation of an Annulated 1,4‐Distibabenzene Diradicaloid
Authors: Steffenfauseweh Henric , Rottschäfer Dennis , Vishnevskiy Yury V. , Neumann Beate , Stammler Hans‐Georg , Szczepanik Dariusz W. , Ghadwal Rajendra S. 
Published: January 2023

AbstractThe first 1,4‐distibabenzene‐1,4‐diide compound [(ADC)Sb]2 (5) based on an anionic dicarbene (ADC) (ADC=PhC{N(Dipp)C}2, Dipp=2,6‐iPr2C6H3) is reported as a bordeaux‐red solid. Compound 5, featuring a central six‐membered C4Sb2 ring with formally SbI atoms may be regarded as a base‐stabilized cyclic bis‐stibinidene in which each of the Sb atoms bears two lone‐pairs of electrons. 5 undergoes 2 e‐oxidation with Ph3C[B(C6F5)4] to afford [(ADC)Sb]2[B(C6F5)4]2 (6) as a brick‐red solid. Each of the Sb atoms of 6 has an unpaired electron and a lone‐pair. The broken‐symmetry open‐shell singlet diradical solution for (6)2+ is calculated to be 2.13 kcal mol−1 more stable than the closed‐shell singlet. The diradical character of (6)2+ according to SS‐CASSCF (state‐specific complete active space self‐consistent field) and UHF (unrestricted Hartree‐Fock) methods amounts to 36 % and 39 %, respectively. Treatments of 6 with (PhE)2 yield [(ADC)Sb(EPh)]2[B(C6F5)4]2 (7‐E) (E=S or Se). Reaction of 5 with (cod)Mo(CO)4 affords [(ADC)Sb]2Mo(CO)4 (8).
Transient and Dissipative Host–Guest Hydrogels Regulated by Consumption of a Reactive Chemical Fuel
Authors: Su Bo , Chi Teng , Ye Zhou , Xiang Yuanhui , Dong Ping , Liu Dongping , Addonizio Christopher J. , Webber Matthew J. 
Published: January 2023

AbstractThe transient self‐assembly of molecules under the direction of a consumable fuel source is fundamental to biological processes such as cellular organization and motility. Such biomolecular assemblies exist in an out‐of‐equilibrium state, requiring continuous consumption of high energy molecules. At the same time, the creation of bioinspired supramolecular hydrogels has traditionally focused on associations occurring at the thermodynamic equilibrium state. Here, hydrogels are prepared from cucurbit[7]uril host–guest supramolecular interactions through transient physical crosslinking driven by the consumption of a reactive chemical fuel. Upon action from this fuel, the affinity and dynamics of CB[7]–guest recognition are altered. In this way, the lifetime of transient hydrogel formation and the dynamic modulus obtained are governed by fuel consumption, rather than being directed by equilibrium complex formation.
Optimized Sieving Effect for Ethanol/Water Separation by Ultramicroporous MOFs
Authors: Zheng Xiaoqing , Chen Liangji , Zhang Hao , Yao Zizhu , Yang Yisi , Xiang Fahui , Li Yunbin , Xiang  Shengchang , Zhang Zhangjing , Chen Banglin 
Published: January 2023

AbstractHigh‐purity ethanol is a promising renewable energy resource, however separating ethanol from trace amount of water is extremely challenging. Herein, two ultramicroporous MOFs (UTSA‐280 and Co‐squarate) were used as adsorbents. A prominent water adsorption and a negligible ethanol adsorption identify perfect sieving effect on both MOFs. Co‐squarate exhibits a surprising water adsorption capacity at low pressure that surpassing the reported MOFs. Single crystal X‐ray diffraction and theoretical calculations reveal that such prominent performance of Co‐squarate derives from the optimized sieving effect through pore structure adjustment. Co‐squarate with larger rhombohedral channel is suitable for zigzag water location, resulting in reinforced guest‐guest and guest‐framework interactions. Ultrapure ethanol (99.9 %) can be obtained directly by ethanol/water mixed vapor breaking through the columns packed with Co‐squarate, contributing to a potential for fuel‐grade ethanol purification.
Synthesis and characterization of new bio‐based nonmigrating poly(vinyl chloride) plasticizers
Authors: Nosal‐Kovalenko Hanna , Krasuska Agata , Warzała Marek , Robaszkiewicz Andrzej , Ledniowska Kerstin , Stańczyk Dorota , Hordyjewicz‐Baran Zofia , Bartoszewicz Maria , Semeniuk Izabela , Zarębska Magdalena 
Published: January 2023

AbstractThis study describes the synthesis of new nonmigrating PVC plasticizers based on oleic acid as the main raw material. Their structures and production routes were planned to ensure that the resulting synthesis by‐products could also act as PVC plasticizers. All received Esters 1, 2, and 3 revealed plasticizing effect on PVC. Achieved results of elongation at break (260%) for PVC composites with Ester 2 (C11) and Ester 3 (C14) were comparable to those recorded for diisononyl phthalate (DINP) and dioctyl terephthalate (DOTP) (C2 and C5), and only 15% lower for Ester 1 (C8). As intended, the developed plasticizers showed high resistance to migration. The Ester 3 proved to be an extremely migration‐resistant bio‐based plasticizer, due to its high oxirane ring content and large molecule size. After 28 days of survey, the loss of this plasticizer from the PVC sample with 50 PHR of plasticizer was 4.7%, which is nearly 80% lower compared to DINP. Ester 2 was slightly less resistant to migration—with 14.1% mass loss observed after 28 days, which can be attributed to the smaller size of its molecules. Additionally, PVC composites containing Esters 1, 2, and 3 exhibited higher thermal stability compared to composites with DINP or DOTP. T10% for PVC composites with 60 PHR of Esters 1, 2, and 3 was recorded at 286.2°C, 282.8°C, and 286.4°C, respectively. Thus, the developed esters can act not only as PVC plasticizers, but also as thermal stabilizers.
Unique graphene‐carbon black hybrid nanofiller by a micromechanical cleavage technique as a reinforcing agent in elastomers: Fundamental and experimental studies
Authors: Roy Amrita , Kar Saptarshi , Ghosal Ranjan , Mukhopadhyay Rabindra , Naskar Kinsuk , Bhowmick Anil K. 
Published: January 2023

AbstractIn this work, a synthetic technique was developed which effected delamination of graphite into graphene with simultaneous disaggregation of carbon black clusters and formation of secondary attachment between the two. Styrene butadiene rubber nanocomposite with this hybrid filler exhibited substantial reinforcement in the mechanical properties, wear resistance and rubber‐filler interactions. The hybrid nanofiller was superior to conventional carbon black, imparting 57% increase in tensile strength of the nanocomposite. The composite with the hybrid filler also exhibited improved modulus and traction. A detailed analysis of mechanism of reinforcement by the hybrid filler is proposed by the computation of root mean square end‐to‐end network chain distance and the lateral tube dimension employing the entangled‐bound‐rubber‐tube (EBT) model. This neoteric hybrid nanofiller overcame the so‐called dispersibility issues and could be exploited as a part of replacement of carbon black, a synthetic material from fossil fuel by sustainable natural filler.
The improved low‐field electro‐actuation of dielectric elastomer composites regulated by entirely‐inorganicBaTiO3@TiO2core‐shell construction
Authors: Wei Xiuping , Zhao Hang , Yin Lei , Miao Zhiying , Ding Xiaoyu , Wang Qian , Bai Jinbo 
Published: January 2023

AbstractDielectric elastomer (DE) as an important electro‐active polymer (EAP), is capable of providing a large elastic deformation under an external electric field. However, the excellent electro‐actuated performance is usually obtained under high electric fields, which greatly limits the practical application range of DE, especially in the field of in vivo organisms. Thus, it is essential to make a reasonable structural regulation to achieve an effectively improved electro‐actuation of DE materials under low driving electric fields. Herein, a typical BaTiO3@TiO2entirely‐inorganic core‐shell construction was prepared through the micro‐emulsion method. Meanwhile, a series of polydimethylsiloxane (PDMS)‐based DE composites incorporated with different fractions of BaTiO3@TiO2were synthesized by solution blending and compression molding. The BaTiO3@TiO2core‐shell construction endows DE composites with an enlarged heterogeneous interface and enhanced interfacial polarization synchronously, which is also benefit to maintain the flexibility of DE materials. The buffer effect offered by TiO2shell is helpful to alleviate the local electric field concentration at the fillers‐matrix interface in DE when being withstood an exponentially‐growing electric field. Specifically, the maximum electro‐actuated strain of 21% under a low electric field (40 V·μm−1) is obtained from the DE composite filled with 4 wt% BaTiO3@TiO2, which is 290% higher than that of pristine PDMS (5.38% at 40 V·μm−1). It is shown that the well‐designed inorganic core‐shell construction can effectively improve the electromechanical conversion capability of DE composites. This study provides a promising approach to obtain an optimized electro‐actuation under low electric fields.
Synergetic improvement of the thermal conductivity and interlaminar fracture toughness of carbon fiber/epoxy composites by interleaving BN@ZnO particles
Authors: Gu Guohua , Zhang Yuqi , Dong Shuhua , Wei Chuncheng , Lin Zhitao , Shen Hongwang , Meng Fantao 
Published: January 2023

AbstractSynergetic improvement of the thermal conductivity and interlaminar fracture toughness of carbon fiber/epoxy resin composites (CF/EP) is a challenging research job. In this work, hexagonal boron nitride coated ZnO (BN@ZnO) particles were firstly prepared by sol–gel method and BN@ZnO composite laminates were manufactured by mold pressing process. X‐ray diffraction, x‐ray electron spectroscopy and scanning electron microscopy were used to analyze the structure, chemical components and morphology of the BN@ZnO and composite laminates. The effects of BN@ZnO on the impact strength, model II interlaminar fracture toughness (GIIC) and thermal conductivity of composite laminates are investigated. The results show that the interlaminar fracture toughness and thermal conductivity of composite laminates are synergistically enhanced owing to the introduction of hybrid fillers with different dimensions and morphology. The thermal conductivity of the 10 wt% BN@ZnO coated composite laminates is increased by 78% and 90% at 25 and 100°C, respectively. The mechanical properties of composite laminates are enhanced. The model II interlaminar fracture toughness of 2 wt% BN@ZnO composite laminates is 15.4% higher than pure laminate. This work is of significance to realize the structural and functional integration of composite materials.