bluuebunny/crossref_metadata_2025_split huggingface dataset:
Regulation of Substrate Dissipation via Tunable Linear Elasticity Controls Cell Activity
Authors: Sacco Pasquale , Piazza Francesco , Pizzolitto Chiara , Baj Gabriele , Brun Francesco , Marsich Eleonora , Donati Ivan 
Published: April 2022

AbstractNatural tissues and extracellular matrices (ECMs) are not purely elastic materials but exhibit dissipative properties. Although it has recently emerged as a novel regulator of cellular responses, the contribution of material dissipation to guiding cell‐fate decisions is still in its infancy. Here, a strategy for tuning the dissipation rate of viscoplastic substrates while precisely regulating linear elasticity is reported. Semi‐interpenetrating substrates consisting of a rigid hydrogel network intertwined with a branched biopolymer are described. The release of these weak physical entanglements under loading dissipates the applied stress and leads to the extension of the linear elasticity. These results reveal a crucial link between this material property and cell response in 2D cultures, impacting cell migration mode and speed, vinculin‐dependent focal adhesion geometry and size, F‐actin organization, the transmission of forces, and Yes‐associated protein nuclear translocation. It is shown that cells require joint actomyosin contractility and microtubule tension to probe the substrate and decide whether or not to adhere, revealing a clear correlation between force transmission, substrate dissipation rate, and amount of anchoring points. Overall, these findings introduce linear elasticity as a novel design parameter for assembling tunable dissipative materials to study cell mechanosensing in 2D and possibly also in 3D cultures.
Rear Electrode Materials for Perovskite Solar Cells
Authors: Chen Rui , Zhang Wenjun , Guan Xinyu , Raza Hasan , Zhang Shasha , Zhang Yiqiang , Troshin Pavel A. , Kuklin Sergei A. , Liu Zonghao , Chen Wei 
Published: April 2022

AbstractPerovskite solar cells (PSCs) represent a promising next‐generation photovoltaic technology considering their high efficiency and low cost. At the current stage, resolving the stability bottleneck is extremely urgent to realize PSCs’ commercialization since the efficiencies of these cells are improved to a level comparable to that of crystalline silicon solar cells. Similar to other functional layers, a proper choice of the rear electrode atop the perovskite layer is equally important for achieving the device's long‐term stability. This topic has not been comprehensively reviewed before. Here, recent progress in the development of rear electrodes based on metals, carbon‐based materials, transparent conductive oxides, and conductive polymers is summarized, especially focusing on their different impacts on the device's long‐term stability and associated degradation mechanisms. In the context of practical applications, the impacts of rear electrode materials on the device's overall efficiency and cost‐effectiveness are also discussed.
Functional Encapsulating Structure for Wireless and Immediate Monitoring of the Fluid Penetration
Authors: Lim Daseul , Hong Insic , Park Sang Uk , Chae Jeong Woo , Lee Seunggon , Baac Hyoung Won , Shin Changhwan , Lee Jungheon , Roh Yeonwook , Im Chaewan , Park Yoonseok , Lee Geumbee , Kim Uikyum , Koh Je‐Sung , Kang Daeshik , Han Seungyong , Won Sang Min 
Published: April 2022

AbstractWith the fast‐paced development of biomedical electronics, monitoring physiological processes have become ubiquitous throughout the field of implantable devices. Nevertheless, inherent challenges remain extant when long‐term applications are concerned. For the stable and reliable function of these devices, hermetic and biocompatible encapsulation is of paramount importance; however, extrinsic defects and intrinsic swelling properties of the encapsulating layer present the key limitation to ideal barrier performance. Thus, the ability to monitor biofluid penetration and predict the device's functional lifespan is necessary for safe and stable operation within the body. This paper presents the functional encapsulation structure that quantitatively measures the diffusion of fluids into the encapsulation layer. The hydrolysis of Magnesium (Mg) electrodes underneath the encapsulating material shows the capability to wirelessly monitor the water penetration rate and the presence of defects, such as pinholes and cracks, in the encapsulating material. The experiments conducted throughout this paper analyze the Mg thickness and geometry of the antenna to optimize the device's susceptivity to water penetration when submerged in aqueous environments. The facile fabrication process and the compatibility with prevailing implantable electronics further substantiate the device's usability in diverse applications where chronic implants are necessary for monitoring disease or administering required treatments.
Arginine‐Rich Polymers with Pore‐Forming Capability Enable Efficient Intracellular Delivery via Direct Translocation Across Cell Membrane
Authors: Kang Ziyao , Liu Qi , Zhang Zhanzhan , Zheng Yadan , Wang Chun , Pan Zheng , Li Qiushi , Liu Yang , Shi Linqi 
Published: April 2022

AbstractEfficient delivery of biomacromolecules or drugs across the cell membrane via endocytosis usually encounters inevitable entrapment in endosomes and subsequent degradation in lyso‐endosomes. To address this issue, a series of arginine‐rich cell penetrating polymers is designed and synthesized, which internalize into cells by inducing the formation of pores on the cell membrane, thereby crossing the cell membrane via direct translocation that fundamentally avoids endo/lysosomal entrapment. The structure−activity relationship studies show that PTn‐R2‐C6, which is a type of polymer that has two arginine residues and a flexible hexanoic acid linker in each side chain, exhibits excellent pore‐formation ability on the cell membrane. Further investigations indicate that PTn‐R2‐C6 rapidly transports plasmid DNAs into cytosol through a similar endocytosis‐independent pathway, thereby achieving significantly higher transfection efficiency and lower cytotoxicity than the gold‐standard transfection reagent PEI 25K. These results suggest the great potential of PTn‐R2‐C6 as a safe and efficient gene transfection reagent for wide applications including disease treatments, vaccine development, and biomedical research purposes.
Ultrasensitive Mid‐Infrared Biosensing in Aqueous Solutions with Graphene Plasmons
Authors: Wu Chenchen , Guo Xiangdong , Duan Yu , Lyu Wei , Hu Hai , Hu Debo , Chen Ke , Sun Zhipei , Gao Teng , Yang Xiaoxia , Dai Qing 
Published: April 2022

AbstractIdentifying nanoscale biomolecules in aqueous solutions by Fourier transform infrared spectroscopy (FTIR) provides an in situ and noninvasive method for exploring the structure, reactions, and transport of biologically active molecules. However, this remains a challenge due to the strong and broad IR absorption of water which overwhelms the respective vibrational fingerprints of the biomolecules. In this work, a tunable IR transparent microfluidic system with graphene plasmons is exploited to identify ≈2 nm‐thick proteins in physiological conditions. The acquired in situ tunability makes it possible to eliminate the IR absorption of water outside the graphene plasmonic hotspots by background subtraction. Most importantly, the ultrahigh confinement of graphene plasmons (confined to ≈15 nm) permits the implementation of nanoscale sensitivity. Then, the deuterium effects on monolayer proteins are characterized within an aqueous solution. The tunable graphene‐plasmon‐enhanced FTIR technology provides a novel platform for studying biological processes in an aqueous solution at the nanoscale.
Untangling the Mechanisms of Lattice Distortions in Biogenic Crystals across Scales
Authors: Schoeppler Vanessa , Cook Phil K. , Detlefs Carsten , Demichelis Raffaella , Zlotnikov Igor 
Published: April 2022

AbstractBiomineralized structures are complex functional hierarchical assemblies composed of biomineral building blocks joined together by an organic phase. The formation of individual mineral units is governed by the cellular tissue component that orchestrates the process of biomineral nucleation, growth, and morphogenesis. These processes are imprinted in the structural, compositional, and crystallographic properties of the emerging biominerals on all scales. Measurement of these properties can provide crucial information on the mechanisms that are employed by the organism to form these complex 3D architectures and to unravel principles of their functionality. Nevertheless, so far, this has only been possible at the macroscopic scale, by averaging the properties of the entire composite assembly, or at the mesoscale, by looking at extremely small parts of the entire picture. In this study, the newly developed synchrotron‐based dark‐field X‐ray microscopy method is employed to study the link between 3D crystallographic properties of relatively large calcitic prisms in the shell of the mollusc Pinna nobilis and their local lattice properties with extremely high angular resolution down to 0.001°. Mechanistic links between variations in local lattice parameters and spacing, crystal orientation, chemical composition, and the deposition process of the entire mineral unit are unraveled.
One‐Pot Synthesis of 2,3,6‐Trisubstituted Pyridines by Phosphine‐Catalyzed Annulation of γ‐Vinyl Allenoates with Enamino Esters Followed by DDQ‐Promoted Oxidative Aromatization
Authors: Li Xiaohu , Cai Wei , Huang You 
Published: April 2022

AbstractA one‐pot strategy for constructing trisubstituted pyridine derivatives had been established via phosphine‐catalyzed annulation and DDQ oxidative aromatization reactions. This protocol provides trisubstituted pyridines from γ‐vinyl allenoates and enamino esters under metal‐free conditions.magnified image
Nanoconfinement Effects of Micellar Media in Asymmetric Catalysis
Authors: Lorenzetto Tommaso , Frigatti Davide , Fabris Fabrizio , Scarso Alessandro 
Published: April 2022

AbstractReplacement of organic solvents, in particular chlorinated, aromatic, and polar aprotic ones, is an emerging issue that can find a solution in the development of catalytic reactions in water. Nature performs a multitude of chemical transformations in water under mild conditions mediated by enzymes. In particular the nanoconfinement effects of the enzymes ensure high activity and impressive stereoselectivities. Micellar catalysis is nowadays a real alternative approach to catalysis in traditional organic media, enabling good activity under mild conditions, with the advantage of possible catalyst and micellar medium recycling. Micellar media emerged also as good nano‐environments for stereoselective reactions, with many examples of chemical transformations mediated by metal and organo‐catalysts for which improvements of stereoselectivity were observed with respect to the same reaction under homogeneous conditions in traditional organic solvents. More specifically, both the catalytically active site and the micelles provided by the surfactant can contribute to the asymmetric induction, partially resembling what known in terms of stereoselectivity imparted by the active site of enzymes and metallo‐enzymes.magnified image
Single‐Cell RNA Sequencing Reveals Heterogeneity of Myf5‐Derived Cells and Altered Myogenic Fate in the Absence of SRSF2
Authors: Guo Ruochen , You Xue , Meng Kai , Sha Rula , Wang Zhenzhen , Yuan Ningyang , Peng Qian , Li Zhigang , Xie Zhiqin , Chen Ruijiao , Feng Ying 
Published: April 2022

AbstractSplicing factor SRSF2 acts as a critical regulator for cell survival, however, it remains unknown whether SRSF2 is involved in myoblast proliferation and myogenesis. Here, knockdown of SRSF2 in myoblasts causes high rates of apoptosis and defective differentiation. Combined conditional knockout and lineage tracing approaches show that Myf5‐cre mice lacking SRSF2 die immediately at birth and exhibit a complete absence of mature myofibers. Mutant Myf5‐derived cells (tdtomato‐positive cells) are randomly scattered in the myogenic and non‐myogenic regions, indicating loss of the community effect required for skeletal muscle differentiation. Single‐cell RNA‐sequencing reveals high heterogeneity of myf5‐derived cells and non‐myogenic cells are significantly increased at the expense of skeletal muscle cells in the absence of SRSF2, reflecting altered cell fate. SRSF2 is demonstrated to regulate the entry of Myf5 cells into the myogenic program and ensures their survival by preventing precocious differentiation and apoptosis. In summary, SRSF2 functions as an essential regulator for Myf5‐derived cells to respond correctly to positional cues and to adopt their myogenic fate.
High Open Circuit Voltage Over 1 V Achieved in Tin‐Based Perovskite Solar Cells with a 2D/3D Vertical Heterojunction
Authors: Wang Tianyue , Loi Hok‐Leung , Cao Jiupeng , Qin Zhaotong , Guan Zhiqiang , Xu Yang , Cheng Haiyang , Li Mitch Guijun , Lee Chun‐Sing , Lu Xinhui , Yan Feng 
Published: April 2022

Abstract2D–3D mixed tin halide perovskites are outstanding candidate materials for lead‐free perovskite solar cells (PSCs) due to their improved stability and decreased trap density in comparison with their pure 3D counterparts. However, the mixture of multiple phases may lead to poor charge transfer across the films and limit the device efficiency. Here, a stacked quasi‐2D (down)–3D (top) double‐layered structure in perovskite films prepared via vacuum treatment is demonstrated, which can result in a planar bilayer heterojunction. In addition, it is found that the introduction of guanidinium thiocyanate (GuaSCN) additive can improve the crystallinity and carrier mobility in the 2D perovskite layer and passivate defects in the whole film, leading to a long carrier lifetime (>140 ns) in photoluminescence measurements. As a result, the PSCs show a high open circuit voltage (VOC) up to 1.01 V with a voltage loss of only 0.39 V, which represents the record values ever reported for tin‐based PSCs. The champion device exhibits a power conversion efficiency (PCE) of 13.79% with decent stability, retaining 90% of the initial PCE for 1200 h storage in N2‐filled glovebox.
Virtual Screening for Organic Solar Cells and Light Emitting Diodes
Authors: Forero‐Martinez Nancy C. , Lin Kun‐Han , Kremer Kurt , Andrienko Denis 
Published: April 2022

AbstractThe field of organic semiconductors is multifaceted and the potentially suitable molecular compounds are very diverse. Representative examples include discotic liquid crystals, dye‐sensitized solar cells, conjugated polymers, and graphene‐based low‐dimensional materials. This huge variety not only represents enormous challenges for synthesis but also for theory, which aims at a comprehensive understanding and structuring of the plethora of possible compounds. Eventually computational methods should point to new, better materials, which have not yet been synthesized. In this perspective, it is shown that the answer to this question rests upon the delicate balance between computational efficiency and accuracy of the methods used in the virtual screening. To illustrate the fundamentals of virtual screening, chemical design of non‐fullerene acceptors, thermally activated delayed fluorescence emitters, and nanographenes are discussed.
Synthesis of Ni/NiO@MoO3−x Composite Nanoarrays for High Current Density Hydrogen Evolution Reaction
Authors: Zhang Jun‐Ye , Liang Jiayu , Mei Bingbao , Lan Kun , Zu Lianhai , Zhao Tiancong , Ma Yuzhu , Chen Yan , Lv Zirui , Yang Yi , Yu Chuanghui , Xu Zhe , Xia Bao Yu , Li Wei , Yuan Qinghong , Zhao Dongyuan 
Published: April 2022

AbstractHigh current density hydrogen evolution reaction (HER) in alkaline water electrolysis plays crucial role in renewable and sustainable energy systems, while posing a great challenge to the highly‐efficient electrocatalysts. Here, the synthesis of Ni/NiO@MoO3−x composite nanoarrays is reported by a moderate reduction strategy, combining Ni/NiO nanoparticles (≈20 nm) with amorphous MoO3−x nanoarrays. The Ni/NiO@MoO3−x composite nanoarrays possess enhanced hydrophilicity, optimize reaction energy barriers, accelerate reactant diffusion/bubble detachment, and therefore display an ultrahigh alkaline HER activity with a low η10 overpotential of 7 mV as well as Tafel slope of 34 mV dec−1. More significantly, the Ni/NiO@MoO3−x nanoarrays only demand low overpotentials of 75 and 112 mV to deliver 100 and 200 mA cm−2 hydrogen production current, and can steadily work at 100 mA cm−2 for 40 h, which is more efficient and stable than the Pt/C catalyst.
P and Mo Dual Doped Ru Ultrasmall Nanoclusters Embedded in P‐Doped Porous Carbon toward Efficient Hydrogen Evolution Reaction
Authors: Li Chuang , Jang Haeseong , Liu Shangguo , Kim Min Gyu , Hou Liqiang , Liu Xien , Cho Jaephil 
Published: April 2022

AbstractRational design of efficient hydrogen evolution reaction (HER) electrocatalysts for mass production of hydrogen via electrochemical water splitting is a challenging but pressing task. Herein, an in situ dual doping engineering from phosphomolybdic acid encapsulated within the bimetallic metal‐organic‐frameworks strategy to synthesize P,Mo dual doped Ru ultrasmall nanoparticles embedded in P‐doped porous carbon (P,Mo‐Ru@PC) for efficient HER is proposed. As a result, P,Mo‐Ru@PC achieves a low overpotential of 21 at 10 mA cm−2, low Tafel slopes of 21.7 mV dec−1, and a mass activity about 22 times greater than that of commercial 20 wt% Pt/C in alkaline media. First principle calculations demonstrate that introducing Mo and P atoms into Ru lattices triggers the in situ electron donation from Ru to Mo and P and consequently reduces the energy barrier for the HER.
Over 30% Efficient Indoor Organic Photovoltaics Enabled by Morphological Modification Using Two Compatible Non‐Fullerene Acceptors
Authors: Lee Chihyung , Lee Jung‐Hyun , Lee Hyun Hwi , Nam Minwoo , Ko Doo‐Hyun 
Published: April 2022

AbstractTo meet the requirements for indoor organic photovoltaic (OPV) applications, it is imperative to minimize charge recombination loss and enhance photovoltaic performance toward commercially compelling levels. Here, morphological modification in non‐fullerene blends is demonstrated to boost the efficiency and stability of indoor OPVs. For morphological modification, a ternary blend is devised by utilizing two well‐miscible non‐fullerene acceptors, which improve morphological features in the photoactive layer and suppress charge recombination loss. Morphological modification enhances OPV performance, particularly under low‐intensity indoor irradiation conditions, at which trap‐assisted recombination mainly governs the photovoltaic performance. The optimum ternary OPV shows a new record power conversion efficiency of 30.11% at a 500 lux light‐emitting diode, accompanied by excellent morphological durability under thermal stress, despite the use of “existing” photovoltaic materials designed for AM 1.5 G operation. This study elucidates the effects of morphology on OPV performance under low‐light conditions and suggests an ideal morphology for non‐fullerene OPVs with enhanced performance for indoor applications.
Protonic Conduction in La2NiO4+δ and La2‐xAxNiO4+δ (A = Ca, Sr, Ba) Ruddlesden–Popper Type Oxides
Authors: Zhong Peng , Toyoura Kazuaki , Jiang Lulu , Chen Lubing , Ismail Sara Adeeba , Hatada Naoyuki , Norby Truls , Han Donglin 
Published: April 2022

AbstractA significant hydration and protonic conduction in La2NiO4+δ‐based Ruddlesden–Popper (RP) oxides will enable their use as positrode materials in proton ceramic electrochemical cells (PCECs). Unlike perovskite electrolytes and positrode materials, where protons reside and jump on regular oxide ions, RP oxides such as La2NiO4+δ may contain oxygen interstitials and offer the possibility that protons locate on and migrate by help of these, suggesting a mechanism by which positrodes may operate by triple conduction. Here, theoretical calculations that support proton migration between interstitial oxide ions in the rock‐salt layer via unshared oxide ions in the perovskite layer are reported. Furthermore, water contents of pristine La2NiO4+δ and La2‐xAxNiO4+δ (A = Ca, Sr, Ba) are reported, showing that hydration increases with the level and basicity of the dopant. Hebb‐Wagner blocking electrode measurements show significant partial protonic conductivity in all samples. The effects of doping on hydration and of on the p‐type conductivity suggest that protons reside primarily on structural oxide ion, but a role of interstitial oxide ions for dissolution and migration of protons cannot be ruled out in cases with oxygen excess. The results are instructive for further studies and optimization of RP oxides as potential positrode materials for PCECs.
Strain Engineering of Layered Heterogeneous Structure via Self‐Evolution Confinement for Ultrahigh‐Rate Cyclic Sodium Storage
Authors: Wang Chunhui , Li Guanwu , Qin Haozhe , Xiao Zhiming , Wang Dong , Zhang Bao , Ou Xing , Wu Yingpeng 
Published: April 2022

AbstractTo get a robust architecture for rapid and permanent ion insertion/extraction, various frameworks are constructed, attempting to enhance the high‐rate lifespan. However, uncontrollable structural evolution always results in the structural failure derived from the continuous increasing inner strain during the cycling. Herein, inspired by the nest structure, a stable framework with wave‐like surface morphology and cross‐linked inner configuration is fabricated, which possesses fast ion migration channel and stable structure. Most importantly, the concept of synchronous self‐evolution confinement is proposed for high‐capacity conversion‐type anode materials, which can control the aggregated inner strain and alleviate the inescapable electrode pulverization, thus ensuring the electrode stability and boosting the structure integrity during the repeated cycling. When serving as an anode for sodium ion batteries, the initial nest‐like (SnFe)S2 heterogeneous mildly evolves into a stable architecture with exceptional performance, expressing a prominent rate property (389.4 mA h g−1 at 30 A g−1) and stable durability (627.41 mA h g−1 at 10 A g−1 for 800 cycles). Significantly, this route of strain engineering sheds significant light on solving large volume‐expansion‐type materials for high reversible capacity, especially in the exploration of electrochemical energy storages.
Giant Thermoelectric Properties of Ionogels with Cationic Doping
Authors: Liu Zhuo , Cheng Hanlin , Le Qiujian , Chen Rui , Li Jianbo , Ouyang Jianyong 
Published: April 2022

AbstractAlthough ionic thermoelectric (iTE) materials can have very high thermopower, it is of great significance to develop novel methods to further improve the ionic thermopower and figure of merit (ZTi). Here, significant improvement in the thermopower and thus the ZTi value of an ionogel by cationic doping, is reported. Doping sodium dicyanamide (Na:DCA) into the ionogels of poly(vinylidene fluoride‐co‐hexafluoropropylene) (PVDF‐HFP) and 1‐ethyl‐3‐methylimidazolium dicyanamide (EMIM:DCA) that is an ionic liquid can greatly enhance the thermopower. This is attributed to the interactions between the doped Na+ cations and DCA– anions, thereby increasing the difference in the mobilities of EMIM+ cations and DCA– anions. Moreover, through the combination with the solid networks engineering by an anti‐solvent to PVDF‐HFP, the PVDF‐HFP/EMIM:DCA ionogel doped with 0.5 mol% Na+ with respect to EMIM+ exhibits an ionic thermopower of 43.8 ± 1.0 mV K–1, ionic conductivity of 19.4 ± 0.3 mS cm–1 and thermal conductivity of 0.183 W m–1 K–1 at the relative humidity of 85% and room temperature. The corresponding ZTi value thus reaches 6.1 ± 0.4, much higher than the previous ZTi records of iTE materials. These ionogels can be used in the iTE capacitors for the thermoelectric conversion.