bluuebunny/crossref_metadata_2025_split huggingface dataset:
Dynamic Assembly of Viscoelastic Networks by Aqueous Liquid–Liquid Phase Separation and Liquid–Solid Phase Separation (AqLL‐LS PS2)
Authors: Cui Huanqing , Zhang Yage , Shen Yinan , Zhu Shipei , Tian Jingxuan , Li Qingchuan , Shen Yi , Liu Sihan , Cao Yang , Shum Ho Cheung 
Published: October 2022

AbstractLiving cells comprise diverse subcellular structures, such as cytoskeletal networks, which can regulate essential cellular activities through dynamic assembly and synergistic interactions with biomolecular condensates. Despite extensive efforts, reproducing viscoelastic networks for modulating biomolecular condensates in synthetic systems remains challenging. Here, a new aqueous two‐phase system (ATPS) is proposed, which consists of poly(N‐isopropylacrylamide) (PNIPAM) and dextran (DEX), to construct viscoelastic networks capable of being assembled and dissociated dynamically to regulate the self‐assembly of condensates on‐demand. Viscoelastic networks are generated using liquid–liquid phase‐separated DEX droplets as templates and the following liquid‐to‐solid transition of the PNIPAM‐rich phase. The resulting networks can dissolve liquid fused in sarcoma (FUS) condensates within 5 min. This work demonstrates rich phase‐separation behaviors in a single ATPS through incorporating stimuli‐responsive polymers. The concept can potentially be applied to other macromolecules through other stimuli to develop materials with rich phase behaviors and hierarchical structures.
Chemical Vapor Deposition of Quaternary 2D BiCuSeO p‐Type Semiconductor with Intrinsic Degeneracy
Authors: Li Jie , Zhang Yan , Zhang Junrong , Chu Junwei , Xie Liu , Yu Wenzhi , Zhao Xinxin , Chen Cheng , Dong Zhuo , Huang Luyi , Yang Liu , Yu Qiang , Ren Zeqian , Wang Junyong , Xu Yijun , Zhang Kai 
Published: October 2022

Abstract2D BiCuSeO is an intrinsic p‐type degenerate semiconductor due to its self‐doping effect, which possesses great potential to fabricate high‐performance 2D–2D tunnel field‐effect transistors (TFETs). However, the controllable synthesis of multinary 2D materials by chemical vapor deposition (CVD) is still a challenge due to the restriction of thermodynamics. Here, the CVD synthesis of quaternary 2D BiCuSeO nanosheets is realized. As‐grown BiCuSeO nanosheets with thickness down to ≈6.1 nm (≈7 layers) and domain size of ≈277 µm show excellent ambient stability. Intrinsic p‐type degeneracy of BiCuSeO, capable of maintaining even in a few layers, is comprehensively unveiled. By varying the thicknesses and temperatures, the carrier concentration of BiCuSeO nanosheets can be adjusted in the range of 1019 to 1021 cm−3, and the Hall mobility of BiCuSeO is ≈191 cm2 V−1 s−1 (at 2 K). Furthermore, taking advantage of the p‐type degeneracy of BiCuSeO, a prototypical BiCuSeO/MoS2 TFET is fabricated. The emergence of the negative differential resistance trend and multifunctional diodes by modulating the gate voltage and temperature reveal the great practical implementation potential of BiCuSeO nanosheets. These results pave way for the CVD synthesis of multinary 2D materials and rational design of high‐performance tunnel devices.
Organic Semiconductor Single‐Crystal Light‐Emitting Transistors
Authors: Qin Zhengsheng , Gao Can , Dong Huanli , Hu Wenping 
Published: October 2022

AbstractOrganic semiconductor single crystals, with the unique advantages of high carrier transport properties, high optical quality, and low defect density, are ideal candidates for constructing high‐performance organic light‐emitting transistors (OLETs) and advancing their related potential applications, including smart displays, micro‐nano light sources, organic electrically pumped lasers, and integrated photonic circuits. Recently, significant progress has been made in organic semiconductor single‐crystal light‐emitting transistors (OSSCLETs), particularly high‐mobility emissive organic semiconductor single crystals, high‐performance light‐emitting transistors, and color‐tunable organic semiconductor single crystals and OLETs. In this review, the exciting advances in OSSCLETs are summarized in terms of advanced organic semiconductor materials, high‐quality organic semiconductor single crystals, advanced device technologies, and high‐performance light‐emitting transistors. Finally, the challenges and prospects of OSSCLETs as well as promising research directions in this field are briefly summarized.
Stable High‐Concentration Monoclonal Antibody Formulations Enabled by an Amphiphilic Copolymer Excipient
Authors: Klich John H. , Kasse Catherine M. , Mann Joseph L. , Huang Yaoqi , d'Aquino Andrea I. , Grosskopf Abigail K. , Baillet Julie , Fuller Gerald G. , Appel Eric A. 
Published: October 2022

AbstractMonoclonal antibodies (mAbs) are a staple in modern pharmacotherapy. Unfortunately, these biopharmaceuticals are limited by their tendency to aggregate in formulation, resulting in poor stability and often requiring low concentration drug formulations. Existing excipients designed to stabilize formulations are often limited by their toxicity and tendency to form particles such as micelles. Here, the ability of a simple “drop‐in,” amphiphilic copolymer excipient to enhance the stability of high concentration formulations of clinically relevant mAbs without altering their pharmacokinetics or injectability is demonstrated. Through interfacial rheology and surface tension measurements, it is demonstrated that the copolymer excipient competitively adsorbs to formulation interfaces. Further, through determination of monomeric composition and retained bioactivity after stressed aging, it is shown that this excipient confers a significant stability benefit to high concentration antibody formulations. Finally, it is demonstrated that the excipient behaves as an inactive ingredient, having no significant impact on the pharmacokinetic profile of a clinically relevant antibody in mice. This amphiphilic copolymer excipient demonstrates promise as an additive to create stable, high concentration antibody formulations, thereby enabling improved treatment options such as a route‐of‐administration switch from low concentration intravenous (IV) to high concentration subcutaneous (SC) delivery while reducing dependence on the cold chain.
Energy and Frequency Characteristics of Microseismic Particles in a Complex Geological Model
Authors: Zhou Linli , Jia Baoxin , Zheng Kenan , Chen Hao , Zhao Long 
Published: October 2022

AbstractThis study aims to better understand the energy–frequency characteristics of microseismic wave propagation by monitoring particles in complex geology. Artificial seismic source experiments are conducted using a complex geological model, and variational mode decomposition method is applied to process the microseismic signals, obtain reconstructed microseismic signals and decomposition modes, and calculate the microseismic particle input energy and signal energy at each measurement point. Computations derived from the Sadoff empirical formula are used to evaluate the attenuation of the microseismic particle input energy with the propagation distance. The relationships between microseismic wave center frequency and energy and between the microseismic particle input energy and microseismic signal energy are elucidated. The results show that the microseismic particle input energy follows a power exponential decay trend with increasing propagation distance; the values and distributions of the microseismic particle input energy and signal energy conform to a Gaussian trend in the frequency domain; various geological structures and combinations thereof impose frequency modulation effects on the microseismic wave, where the frequency modulation interval depends on the microseismic waves across the different interfaces; and the linear slope describing the relationship between microseismic particle input energy and signal energy can reflect the microseismic wave propagation state.
Functionalized 3D Covalent Organic Frameworks for High‐Performance CO2 Capture and Separation over N2
Authors: Wei Shuxian , Xin Huili , Wang Maohuai , Xu Shengyu , Zhai Wanru , Liu Sen , Wang Lu , Liu Siyuan , Wang Zhaojie , Lu Xiaoqing 
Published: October 2022

AbstractCovalent organic frameworks (COFs) are emerging adsorbent materials for CO2 capture and separation due to their tunable pore size, periodic permutation, and chemical thermal stability. Herein, four functionalized 3D COF‐300s (COF‐300‐X, X = –SO3H, –NO2, –OH, and –NH2) for CO2 adsorption and separation are studied by using density functional theory and grand canonical Monte Carlo simulation. The results show that four functionalized COF‐300s could create a feasible environment for CO2 adsorption with high accessible surface area, suitable pore size, and high porosity. The CO2 adsorption capacity in COF‐300s could be significantly improved by functionalization. In comparison, the best performing COF‐300‐SO3H shows a superior CO2 adsorption capacity of 6.23 mmol g−1 and a high CO2/N2 selectivity of 393 at 298 K and 100 kPa. The adsorption heat and interaction analyses demonstrate that the CO2 affinity in COF‐300s is enhanced by the introduction of polar functional groups, which renders great CO2 adsorption and separation performances. The gas distribution shows that the adsorption sites are concentrated near the functional groups and the distribution of CO2 in COF‐300‐SO3H has a characteristic of multilayer adsorptions. This work highlights COF‐300‐SO3H as an outperforming adsorbent candidate for CO2 capture and separation.
Spatial distribution characteristics of soil moisture in different slopes on Loess Gully Region
Authors: Shan Yulin , Xie Jiancang , Lei Na 
Published: October 2022

AbstractThe spatiotemporal changes of soil moistures under different rainfall events and slope positions in the loess hilly and gully area were assessed in this study using the positioning monitoring method. According to the three positions with different distances from the top of the slope, set the three treatments of “top of the slope” (TS), “middle of the slope” (MS), and “bottom of the slope” (BS). The results demonstrated a certain degree of influence of rainfall and slope position on the vertical change of soil moisture at different soil depths in the study area. Before intense rainfall, soil moisture at different slope positions revealed a vertical distribution pattern and increased with increasing soil depth. In addition, soil moisture contents below the 60‐cm depth at different sites were significantly higher than those observed above the 60‐cm depth (p < .05), while soil moisture contents below the 120‐cm depth were extremely significantly higher than those observed above the 120‐cm depth (p < .01). On the other hand, no significant variation in soil moisture content was observed between different depths after intense rainfall events (p > .05). The above studies show that soil moisture in the loess hilly and gully area has a certain hysteresis effect. The hysteresis of soil flow allows us to effectively collect and use soil moisture, which can provide a theoretical basis for the intensive and economical use of soil moisture in this area.
Impact of alternating overnight housing conditions on welfare measures in a bachelor group of western lowland gorillas (Gorilla gorilla gorilla)
Authors: Gartland Kylen N. , Bovee Emily , Fuller Grace 
Published: October 2022

AbstractSpatial parameters and design of overnight housing spaces can have significant influences on both nocturnal and diurnal behaviors of western lowland gorillas (Gorilla gorilla gorilla) in captivity. This is especially true for bachelor groups, as adult males have demonstrated a greater tendency to separate from conspecifics overnight. Additionally, previous studies have suggested that the social needs of individuals in bachelor units may shift over time. The bachelor unit at the Detroit Zoo is managed in a unique hybrid strategy in which the group is housed socially for three nights (either indoors or indoors with outdoor access), then separately on the fourth. A 2016 study of this group (n = 3) suggested that individuals had better welfare following social overnight housing as compared to solitary overnight housing. We aimed to reassess how overnight housing conditions affect individual welfare several years later. We revised a previously developed qualitative behavioral assessment tool that included 13 behavioral items spanning both positive and negative indicators of welfare. Animal care staff completed the assessment and collected a fecal sample every day for each gorilla for a period of 3 months. We used Kruskal–Wallis tests to analyze variation in behavioral items and FGMs between conditions. We then used generalized linear mixed models to identify whether overnight housing condition or other potentially confounding variables were driving observed variation in welfare indicators. We found significant variation demonstrating significantly better welfare indicators after being housed separately as compared to being socially housed indoors overnight. Although separate housing appears to be the ideal condition for this group at this point in time, if seasonality permits, social housing with outdoor access may be a feasible alternative to consistent overnight separation for these gorillas.
Pre‐diagnostic cognitive and functional impairment in multiple sporadic neurodegenerative diseases
Authors: Swaddiwudhipong Nol , Whiteside David J. , Hezemans Frank H. , Street Duncan , Rowe James B. , Rittman Timothy 
Published: October 2022

AbstractIntroductionThe pathophysiological processes of neurodegenerative diseases begin years before diagnosis. However, pre‐diagnostic changes in cognition and physical function are poorly understood, especially in sporadic neurodegenerative disease.MethodsUK Biobank data were extracted. Cognitive and functional measures in individuals who subsequently developed Alzheimer's disease (AD), Parkinson disease, frontotemporal dementia, progressive supranuclear palsy, dementia with Lewy bodies, or multiple system atrophy were compared against individuals without neurodegenerative diagnoses. The same measures were regressed against time to diagnosis, after adjusting for the effects of age.ResultsThere was evidence for pre‐diagnostic cognitive impairment and decline with time, particularly in AD. Pre‐diagnostic functional impairment and decline were observed in multiple diseases.DiscussionThe scale and longitudinal follow‐up of UK Biobank participants provides evidence for cognitive and functional decline years before symptoms become obvious in multiple neurodegenerative diseases. Identifying pre‐diagnostic functional and cognitive changes could improve selection for preventive and early disease‐modifying treatment trials.
Modelling Conformational Flexibility in a Spectrally Addressable Molecular Multi‐Qubit Model System
Authors: Rogers Ciarán J. , Asthana Deepak , Brookfield Adam , Chiesa Alessandro , Timco Grigore A. , Collison David , Natrajan Louise S. , Carretta Stefano , Winpenny Richard E. P. , Bowen Alice M. 
Published: October 2022

AbstractDipolar coupled multi‐spin systems have the potential to be used as molecular qubits. Herein we report the synthesis of a molecular multi‐qubit model system with three individually addressable, weakly interacting, spin
centres of differing g‐values. We use pulsed Electron Paramagnetic Resonance (EPR) techniques to characterise and separately address the individual electron spin qubits; CuII, Cr7Ni ring and a nitroxide, to determine the strength of the inter‐qubit dipolar interaction. Orientation selective Relaxation‐Induced Dipolar Modulation Enhancement (os‐RIDME) detecting across the CuII spectrum revealed a strongly correlated CuII‐Cr7Ni ring relationship; detecting on the nitroxide resonance measured both the nitroxide and CuII or nitroxide and Cr7Ni ring correlations, with switchability of the interaction based on differing relaxation dynamics, indicating a handle for implementing EPR‐based quantum information processing (QIP) algorithms.
Excited‐State Intramolecular Proton Transfer Parent Core Engineering for Six‐Level System Lasing Toward 900 nm
Authors: Yan Chang‐Cun , Liu Yan‐Ping , Yang Wan‐Ying , Wu Jun‐Jie , Wang Xue‐Dong , Liao Liang‐Sheng 
Published: October 2022

AbstractOrganic molecules which can undergo excited‐state intramolecular proton transfer (ESIPT) process have been considered as ideal gain materials for near‐infrared organic lasers owing to their effective four‐level systems. However, extending lasing wavelength beyond 800 nm with present ESIPT‐active gain materials is still in challenge. Herein, we established a molecular design strategy that operates via extending the π‐conjugated system of the ESIPT parent core to enhance the cascaded double ESIPT process and thus to achieve the red‐shifted six‐level system lasing. Concretely, a model molecule with 1,9‐dihydroxyanthracene as the ESIPT parent core was designed and synthesized, which was proved to undergo twice cascaded ESIPT processes while the 1,8‐dihydroxynaphthalene‐based analogue can only undergo once ESIPT process based on DFT calculations and ultrafast dynamics analyses. Finally, a six‐level system lasing toward 900 nm was achieved with a low threshold of 27.4 μJ cm−2.
Fluorine‐18 Labeling of Difluoromethyl and Trifluoromethyl Groups via Monoselective C−F Bond Activation
Authors: Khanapur Shivashankar , Lye Kenneth , Mandal Dipendu , Jie Wee Xin , Robins Edward G. , Young Rowan D. 
Published: October 2022

AbstractWe report a general method for the labeling of both CF3 and CF2H groups in a broad range of chemical settings (aryl, oxide, sulfide). The method utilizes frustrated Lewis pair mediated selective C−F activation to formally substitute fluorine‐19 with fluorine‐18 in a two‐step defluorination/radiofluorination process, and as such can utilize the target compounds as starting materials. The radiotracer precursors can be isolated as stable salts prior to radiofluorination. The method delivers good radiochemical yields and molar activities (up to 35.2±6.5 % non‐decay corrected isolated activity yields and 12.0±1.7 GBq μmol−1 molar activities) and is shown to be applicable to biologically relevant compounds. The ability to utilize the target compound as the starting material and the synthetic simplicity of the method coupled with the ever‐increasing use of CF3 and CF2H groups in pharmaceuticals makes this method attractive for drug and radiotracer development.
Dotierungs‐/Legierungswege zu bleifreien Halogenid‐Perowskiten mit ultimativen Photolumineszenz‐Quantenausbeuten
Authors: Stroyuk Oleksandr , Raievska Oleksandra , Hauch Jens , Brabec Christoph J. 
Published: October 2022

AbstractMaßgeschneiderte Modifizierungen bleifreier Halogenid‐Perowskite (BHP) durch Dotierung/Legierung mit Metallkationen gelten als vielversprechender Weg zu hocheffizienten anorganischen Leuchtstoffen mit Photolumineszenz (PL)‐Quantenausbeuten von bis zu 100 %. Solche Materialien weisen typischerweise eine selektive Empfindlichkeit gegen UV‐Licht, einen breiten PL‐Bereich, lange PL‐Lebensdauern und eine einzigartige Variabilität und Stabilität der Zusammensetzung auf – eine ideale Kombination für viele Lichtsammelanwendungen. Dieser Kurzaufsatz stellt den Stand der Technik bei dotierten BHPs vor, mit dem Schwerpunkt auf Berichten aus den letzten 2–3 Jahren. Wir diskutieren die Faktoren, die die Effizienz und die spektralen Parameter der Breitband‐PL von dotierten BHP abhängig von Dotierstoff und Wirtsmatrix im mikro‐ wie auch im nanokristallinen Zustand bestimmen, gehen auf die wichtigsten Herausforderungen in diesem sich rasch entwickelnden Forschungsbereich ein und skizzieren die vielversprechendsten Konzepte, um weitere Fortschritte in diesem Bereich zu erzielen.
Atroposelective Synthesis of N‐Arylated Quinoids by Organocatalytic Tandem N‐Arylation/Oxidation
Authors: Guo Chang‐Qiu , Lu Chuan‐Jun , Zhan Li‐Wen , Zhang Peng , Xu Qi , Feng Jia , Liu Ren‐Rong 
Published: October 2022

AbstractDiarylamines and related scaffolds are ubiquitous atropisomeric chemotypes in biologically active natural products. However, the catalytic asymmetric synthesis of these axially chiral compounds remains largely unexplored. Herein, we report that a BINOL‐derived chiral phosphoric acid (CPA) successfully catalyzed the atroposelective coupling of quinone esters and anilines through direct C−N bond formation to afford N‐aryl quinone atropisomers with an unprecedented intramolecular N−H−O hydrogen bond within a six‐membered ring in good yields and enantioselectivities with the quinone ester as both the electrophile and the oxidant. A gram‐scale experiment demonstrated the utility of this synthetic protocol. Moreover, this methodology provides a platform for the synthesis of structurally diverse secondary amine atropisomers by nucleophilic addition.
The Dynamic Formation from Metal‐Organic Frameworks of High‐Density Platinum Single‐Atom Catalysts with Metal‐Metal Interactions
Authors: Shan Jieqiong , Liao Jiangwen , Ye Chao , Dong Juncai , Zheng Yao , Qiao Shi‐Zhang 
Published: October 2022

AbstractSingle‐atom catalysts (SACs) hold great promise for highly efficient heterogeneous catalysis, yet the practical applications require the development of high‐density active sites with flexible geometric structures. The lack of understanding in the dynamic formation process of single atoms in the host framework has been plaguing the controllable synthesis of next generation SACs. Here using Co‐based metal‐organic frameworks (MOFs) as a starting substrate, we fully elucidated the formation of high‐density Pt single atoms with inter‐site interactions in derived Co3O4 host. The cation exchange process and dynamic evolution of Pt−Pt interactions, organic ligand cleavage and Pt‐oxygen coordination formation during the pyrolysis process have been unambiguously interpreted by a series of in situ/ex situ spectroscopic measurements and theoretical computation. These findings would direct the synthesis of high‐density SACs with metal‐metal interactions, which demonstrate significantly enhanced structural flexibility and catalytic properties.
Singlet‐Triplet Energy Gap as a Critical Molecular Descriptor for Predicting Organic Photovoltaic Efficiency
Authors: Han Guangchao , Yi Yuanping 
Published: October 2022

AbstractIn contrast to the inorganic and perovskite solar cells, organic photovoltaics (OPV) depend on a series of charge generation and recombination processes, which complicates molecular design to improve the power conversion efficiencies (PCEs). Herein, we first propose the singlet‐triplet energy gap (ΔEST) as a critical molecular descriptor for predicting the PCE considering that minimizing ΔEST is beneficial to simultaneously reduce voltage loss and triplet recombination. Remarkably, the results from data‐driven machine learning verify that the prediction accuracy of the ΔEST (Pearson's correlation coefficient r=0.72) is apparently superior to that of two commonly used molecular descriptors in OPV, i.e., the optical gap (r=0.65) and the driving force (r=0.53). Moreover, an impressive prediction accuracy of r=0.81 is achieved just by combining the three descriptors. This work paves the way toward rapid and precise screening of efficient OPV materials.
A Sterically Tuned Directing Auxiliary Promotes Catalytic 1,2‐Carbofluorination of Alkenyl Carbonyl Compounds**
Authors: Liu Zhonglin , Oxtoby Lucas J. , Sun Juntao , Li Zi‐Qi , Kim Nana , Davies Geraint H. M. , Engle Keary M. 
Published: October 2022

AbstractThe site‐selective palladium‐catalyzed three‐component coupling of unactivated alkenyl carbonyl compounds, aryl‐ or alkenylboronic acids, and N‐fluorobenzenesulfonimide is described herein. Tuning of the steric environment on the bidentate directing auxiliary enhances regioselectivity and facilitates challenging C(sp3)−F reductive elimination from a PdIV intermediate to afford 1,2‐carbofluorination products in moderate to good yields.