bluuebunny/crossref_metadata_2025_split huggingface dataset:
Bifunctional Single Atom Catalysts for Rechargeable Zinc–Air Batteries: From Dynamic Mechanism to Rational Design
Authors: Zhang Peng , Chen Kuo , Li Jiaye , Wang Minmin , Li Min , Liu Yunqi , Pan Yuan 
Published: June 2023

AbstractEver‐growing demands for rechargeable zinc–air batteries (ZABs) call for efficient bifunctional electrocatalysts. Among various electrocatalysts, single atom catalysts (SACs) have received increasing attention due to the merits of high atom utilization, structural tunability, and remarkable activity. Rational design of bifunctional SACs relies heavily on an in‐depth understanding of reaction mechanisms, especially dynamic evolution under electrochemical conditions. This requires a systematic study in dynamic mechanisms to replace current trial and error modes. Herein, fundamental understanding of dynamic oxygen reduction reaction and oxygen evolution reaction mechanisms for SACs is first presented combining in situ and/or operando characterizations and theoretical calculations. By highlighting structure–performance relationships, rational regulation strategies are particularly proposed to facilitate the design of efficient bifunctional SACs. Furthermore, future perspectives and challenges are discussed. This review provides a thorough understanding of dynamic mechanisms and regulation strategies for bifunctional SACs, which are expected to pave the avenue for exploring optimum single atom bifunctional oxygen catalysts and effective ZABs.
Perovskite‐Derived Bismuth with I− and Cs+ Dual Modification for High‐Efficiency CO2‐to‐Formate Electrosynthesis and Al‐CO2 Batteries
Authors: Luo Yuqing , Chen Shuhua , Zhang Jie , Ding Xue , Pan Binbin , Wang Liguang , Lu Jun , Cao Muhan , Li Yanguang 
Published: June 2023

AbstractBi‐based materials are one of the most promising candidates for electrochemical CO2 reduction reaction (CO2RR) to formate; however, the majority of them still suffer from low current density and stability that essentially constrain their potential applications at the industrial scale. Surface modification represents an effective approach to modulate the electrode microenvironment and the relative binding strength of key intermediates. Herein, it is demonstrated that the surface comodification with halides and alkali metal ions from the conversion of Bi‐based halide perovskite nanocrystals is a viable strategy to boost the CO2RR performance of Bi for formate electrosynthesis. Cs3Bi2I9 nanocrystals are prepared by a hot‐injection method. The as‐prepared products feature well‐defined hexagonal shape and uniform size distribution. When used as the precatalyst, Cs3Bi2I9 nanocrystals are converted to Cs+ and I− comodified Bi. The resultant catalyst exhibits high formate Faradaic efficiency close to 100%, and remarkable partial current density up to 44 mA cm−2 in an H‐cell and up to 276 mA cm−2 in a flow cell. Moreover, Cs3Bi2I9 is used as the cathode catalyst and paired with an Al anode in an Al‐CO2 battery for simultaneous CO2 valorization and power generation.
Interface Modification for Efficient and Stable Inverted Inorganic Perovskite Solar Cells
Authors: Xu Tianfei , Xiang Wanchun , Yang Junjie , Kubicki Dominik J. , Tress Wolfgang , Chen Tao , Fang Zhimin , Liu Yali , Liu Shengzhong 
Published: June 2023

AbstractDue to their excellent thermal stability and ideal bandgap, metal halide inorganic perovskite based solar cells (PSCs) with inverted structure are considered as an excellent choice for perovskite/silicon tandem solar cells. However, the power conversion efficiency (PCE) of inverted inorganic perovskite solar cells (PSCs) still lags far behind that of conventional n–i–p PSCs due to interfacial energy level mismatch and high nonradiative charge recombination. Herein, the performance of inverted PSCs is significantly improved by interfacial engineering of CsPbI3−xBrx films with 2‐mercapto‐1‐methylimidazole (MMI). It is found that the mercapto group can preferably react with the undercoordinated Pb2+ from perovskite by forming Pb–S bonds, which appreciably reduces the surface trap density. Moreover, MMI modification results in a better energy level alignment with the electron‐transporting material, promoting carrier transfer and reducing voltage deficit. The above combination results in an open‐circuit voltage enhancement by 120 mV, yielding a champion PCE of 20.6% for 0.09 cm2 area and 17.3% for 1 cm2 area. Furthermore, the ambient, operational and heat stabilities of inorganic PSCs with MMI modification are also greatly improved. The work demonstrates a simple but effective approach for fabricating highly efficient and stable inverted inorganic PSCs.
Combining Rigid Cellulose Nanocrystals and Soft Silk Proteins: Revealing Interactions and Alignment in Shear
Authors: Leppänen Ilona , Arola Suvi , King Alistair W. T. , Unger Miriam , Stadler Hartmut , Nissen Gry Sofie , Zborowski Charlotte , Virtanen Tommi , Salmela Juha , Setälä Harri , Lésage Stephanie , Österberg Monika , Tammelin Tekla 
Published: June 2023

AbstractNatural materials, such as silk and cellulose, have an inspiring set of properties, which have evolved over hundreds of millions of years. In this study, cellulose nanocrystals (CNCs) and regenerated silk fibroin (RSF) are combined to evaluate their suitability for filament formation. This is assessed by tuning and characterizing the interactions between these two materials and finally by studying the alignment of the mixtures under shear. To modify the interactions between CNCs and silk, CNCs with varying surface functionalities (sulfate and/or aminosilane groups) are used. The interactions and compatibility of the two components are investigated using quartz crystal microbalance with dissipation monitoring (QCM‐D) and photothermal atomic force microscopy (AFM‐IR), which show that ionic interactions induce sufficient binding between the two components. Then, the alignment of the CNC and silk mixtures is evaluated by shear‐induced polarized light imaging, which indicates that silk can orientate with the CNCs when not covalently bound. Finally, the potential of the materials for filament formation is tentatively demonstrated using an industrial dry‐spinning environment, where CNCs are expected to bring order and alignment, whereas RSF provides soft and more mobile regions to further facilitate the alignment of the final filament structure.
Ultrafast Polarization Sensitive Photodetector Based on MoS2/Ta2Pd3Se8 Hybrid Dimensional Heterostructure
Authors: Ke Shenggang , Zhou Jiayuan , Larionov Konstantin V. , Zhu Ankang , Li Ying , Zhang Hui , Yang Yang , Zhu Xiangde , Li Liang , Sorokin Pavel B. , Tian Mingliang , Gao Wenshuai , Liu Xue 
Published: June 2023

AbstractVan der Waals (vdWs) heterostructures based on low dimensional semiconducting materials offer tremendous opportunities in investigating next generation electronic and optoelectronic devices. Careful design based on combinations of different crystal structures and their band alignment engineering in such architectures are crucial for realizing specialized functionality and preferable performance. Here, a polarized light sensitive photodetector with high efficiency and ultrafast response speed based on hybrid dimensional MoS2/Ta2Pd3Se8 vdWs heterostructure, which is owing to the unilateral depletion region as formed between the n–n junction, is reported. In particular, under ultraviolet light irradiation, the device exhibits a high external quantum efficiency of 970%, and the device shows an ultrafast response speed of 1.3 µs under visible light excitation. Moreover, the 1D Ta2Pd3Se8 crystal introduces a highly anisotropic feature of the heterostructure, so as to realize selective detection to linear polarized light with an anisotropic ratio up to 0.66. This work sheds light on the potential applications of hybrid dimensional vdWs heterostructures, which may provide new insight for exploring high performance photodetectors with advanced functions.
An Injectable Sustained Release Hydrogel of Hyaluronic Acid Loaded with β‐Ecdysterone Ameliorates Cartilage Damage in Osteoarthritis via Activating Autophagy
Authors: Tang Yanghua , Zhou Kun , Mo Yafeng , Xin Dawei , Xiong Zhenfei , Yu Xuezi 
Published: June 2023

AbstractThis study uses the knee Osteoarthritis (OA) rat (constructed by the anterior cruciate ligament transection) and the inflammatory chondrocyte (constructed by 20 ng mL−1 tumor necrosis factor‐α (TNF‐α)) to study the improvement effect of injectable β‐ecdysterone (β‐Ec) hydrogel consisting of poly (D, L‐lactic‐co‐glycolic acid)‐hyaluronate (HA‐β‐Ec‐Gel) on cartilage damage. The results show that the HA‐β‐Ec‐Gel improves the three‐dimensional of bone structure. The HA‐β‐Ec‐Gel treatment improves cartilage tissue injury of OA rats. It advances the levels of autophagic factor Beclin1 (Beclin1) and microtubule–associated protein 1 light chain 3 (LC3) in cartilage tissue. The lysyl oxidase like 3 (LOXL3), ras homologue enriched (Rheb), phosphorylated (p)‐V–akt murine thymoma viral oncogene homolog (AKT)/AKT, and p‐mechanistic target of rapamycin (mTOR)/mTOR signal expression are inhibited by HA‐β‐Ec‐Gel intervention. In inflammatory chondrocytes, β‐Ec improves the cell viability, autophagosome numbers, and Beclin1 and LC3 II/I levels, also inhibits apoptotic rate, LOXL3 and Rheb expression levels, and the AKT/mTOR pathway. The 3‐methyladenine addition reverses these effects of β‐Ec. The Rheb or LOXL3 knockdown chondrocytes aren't sensitive to TNF–α‐induced damage. Their autophagy level is high. This study reveals the improvement effects of injectable HA‐β‐Ec‐Gel on OA, which provides a scientific basis and new direction for the development of OA treatment strategies.
Thermoresponsive Polypeptide Fused L‐Asparaginase with Mitigated Immunogenicity and Enhanced Efficacy in Treating Hematologic Malignancies
Authors: Zhang Sanke , Sun Yuanzi , Zhang Longshuai , Zhang Fan , Gao Weiping 
Published: June 2023

AbstractL‐Asparaginase (ASP) is well‐known for its excellent efficacy in treating hematological malignancies. Unfortunately, the intrinsic shortcomings of ASP, namely high immunogenicity, severe toxicity, short half‐life, and poor stability, restrict its clinical usage. Poly(ethylene glycol) conjugation (PEGylation) of ASP is an effective strategy to address these issues, but it is not ideal in clinical applications due to complex chemical synthesis procedures, reduced ASP activity after conjugation, and pre‐existing anti‐PEG antibodies in humans. Herein, the authors genetically engineered an elastin‐like polypeptide (ELP)‐fused ASP (ASP‐ELP), a core‐shell structured tetramer predicted by AlphaFold2, to overcome the limitations of ASP and PEG‐ASP. Notably, the unique thermosensitivity of ASP‐ELP enables the in situ formation of a sustained‐release depot post‐injection with zero‐order release kinetics over a long time. The in vitro and in vivo studies reveal that ASP‐ELP possesses increased activity retention, improved stability, extended half‐life, mitigated immunogenicity, reduced toxicity, and enhanced efficacy compared to ASP and PEG‐ASP. Indeed, ASP‐ELP treatment in leukemia or lymphoma mouse models of cell line‐derived xenograft (CDX) shows potent anti‐cancer effects with significantly prolonged survival. The findings also indicate that artificial intelligence (AI)‐assisted genetic engineering is instructive in designing protein‐polypeptide conjugates and may pave the way to develop next‐generation biologics to enhance cancer treatment.
An All‐In‐One Transient Theranostic Platform for Intelligent Management of Hemorrhage
Authors: Haghniaz Reihaneh , Gangrade Ankit , Montazerian Hossein , Zarei Fahimeh , Ermis Menekse , Li Zijie , Du Yuxuan , Khosravi Safoora , de Barros Natan Roberto , Mandal Kalpana , Rashad Ahmad , Zehtabi Fatemeh , Li Jinghang , Dokmeci Mehmet R. , Kim Han‐Jun , Khademhosseini Ali , Zhu Yangzhi 
Published: June 2023

AbstractDeveloping theranostic devices to detect bleeding and effectively control hemorrhage in the prehospital setting is an unmet medical need. Herein, an all‐in‐one theranostic platform is presented, which is constructed by sandwiching silk fibroin (SF) between two silver nanowire (AgNW) based conductive electrodes to non‐enzymatically diagnose local bleeding and stop the hemorrhage at the wound site. Taking advantage of the hemostatic property of natural SF, the device is composed of a shape‐memory SF sponge, facilitating blood clotting, with ≈82% reduction in hemostatic time in vitro as compared with untreated blood. Furthermore, this sandwiched platform serves as a capacitive sensor that can detect bleeding and differentiate between blood and other body fluids (i.e., serum and water) via capacitance change. In addition, the AgNW electrode endows anti‐infection efficiency against Escherichia coli and Staphylococcus aureus. Also, the device shows excellent biocompatibility and gradually biodegrades in vivo with no major local or systemic inflammatory responses. More importantly, the theranostic platform presents considerable hemostatic efficacy comparable with a commercial hemostat, Dengen, in rat liver bleeding models. The theranostic platform provides an unexplored strategy for the intelligent management of hemorrhage, with the potential to significantly improve patients' well‐being through the integration of diagnostic and therapeutic capabilities.
Electro‐membrane reactor: A powerful tool for green chemical engineering
Authors: Chen Binglun , Zhang Zirui , Jiang Chenxiao , Fu Rong , Yan Junying , Wang Huangying , Li Ruirui , Cao Guangzhong , Wang Yaoming , Xu Tongwen 
Published: June 2023

AbstractElectro‐membrane reactors use electro‐membranes for preferentially diffusive/electrophoretic migration or electroosmotic separation of in‐situ reactive products, thereby maximizing the reaction rate and transport efficiencies of the products. These reactors are widely employed in the chemical engineering sectors such as green chemical synthesis, biorefining, electrocatalytic reduction/oxidation, and water treatment. In this review article, we provide an overview of the recent advances in three categories of electro‐membrane reactors in chemical engineering sectors from three categories: (1) Electro‐membrane reactors based on stacked ion‐exchange membranes for resources recovery; (2) Electro‐membrane reactors via Faraday reactions on functional anodes/cathodes for substance transformation; and (3) Closed‐loop chemical reactions and substance separation via coupling of Faraday reactions and stacked membranes. The increasing demand for low‐carbon economy has accelerated the advancement of environmentally friendly chemical engineering and sustainable processes and necessitates the use of electro‐membrane processes. The macro perspective provides a timely reference for researchers and engineers.
Plasma metabolomics identifies metabolic alterations associated with the growth and development of cat
Authors: Liu Shuaiyang , Chen Yun , Wang Xiaoming , Wang Shuang , Bai Lan , Cheng Xu , Wan Juan , Hu Yufeng , Ding Yi , Zhang Xin , Ding Mingxing , Li Hongliang , Hu Manli 
Published: June 2023

AbstractBackgroundThe purpose of our study was to study the composition and content of the feline plasma metabolome revealing the critical metabolites and metabolic pathways associated with age during growth and development.MethodsBlood samples were collected from juvenile and adult groups for blood routine tests and serum biochemistry tests. Non‐targeted metabolomics analyses of plasma were also performed to investigate changes in metabolites and metabolic pathways.ResultsIn this study, we found that the red blood cell counts, liver function indexes (albumin and gamma‐glutamyl transpeptidase), and the concentration of triglyceride and glucose changed significant with growth and development. The metabolomics results revealed that 1427 metabolites were identified in the plasma of young and adult cats. Most of these metabolites belong to major classes of lipids and lipid‐like molecules. The most obvious age‐related metabolites include reduced levels of chenodeoxycholate, taurocholate, cholate, and taurochenodeoxycholate but increased levels of L‐cysteine and taurocyamine in the adult cat's serum. These metabolites are mainly involved in the primary bile acid biosynthesis pathway, the bile secretion pathway, and the taurine and hypotaurine metabolism pathway.ConclusionThis study revealed many age‐related metabolite alterations in the feline plasma. These age‐varying metabolites, especially in the bile acid biosynthesis and secretion metabolism pathways, indicate that the regulation of these pathways is involved in the growth and development of cats. This study promotes our understanding of the mechanism of feline growth and provides new insights into nutrition and medicine for cats of different ages.
Variations in Intracellular Organometallic Reaction Frequency Captured by Single‐Molecule Fluorescence Microscopy
Authors: Nguyen Dat , Yan Guangjie , Chen Tai‐Yen , Do Loi H. 
Published: June 2023

AbstractStudies of organometallic reactions in living cells commonly rely on ensemble‐averaged measurements, which can obscure the detection of reaction dynamics or location‐specific behavior. This information is necessary to guide the design of bioorthogonal catalysts with improved biocompatibility, activity, and selectivity. By leveraging the high spatial and temporal resolution of single‐molecule fluorescence microscopy, we have successfully captured single‐molecule events promoted by Ru complexes inside live A549 human lung cells. By observing individual allylcarbamate cleavage reactions in real‐time, our results revealed that they occur with greater frequency inside the mitochondria than in the non‐mitochondria regions. The estimated turnover frequency of the Ru complexes was at least 3‐fold higher in the former than the latter. These results suggest that organelle specificity is a critical factor to consider in intracellular catalyst design, such as in developing metallodrugs for therapeutic applications.
Regulation of Redox Molecular Junctions in Covalent Organic Frameworks for H2O2 Photosynthesis Coupled with Biomass Valorization
Authors: Chang Jia‐Nan , Shi Jing‐Wen , Li Qi , Li Shan , Wang Yi‐Rong , Chen Yifa , Yu Fei , Li Shun‐Li , Lan Ya‐Qian 
Published: June 2023

AbstractH2O2 photosynthesis coupled with biomass valorization can not only maximize the energy utilization but also realize the production of value‐added products. Here, a series of COFs (i.e. Cu3‐BT‐COF, Cu3‐pT‐COF and TFP‐BT‐COF) with regulated redox molecular junctions have been prepared to study H2O2 photosynthesis coupled with furfuryl alcohol (FFA) photo‐oxidation to furoic acid (FA). The FA generation efficiency of Cu3‐BT‐COF was found to be 575 mM g−1 (conversion ≈100 % and selectivity >99 %) and the H2O2 production rate can reach up to 187 000 μM g−1, which is much higher than Cu3‐pT‐COF, TFP‐BT‐COF and its monomers. As shown by theoretical calculations, the covalent coupling of the Cu cluster and the thiazole group can promote charge transfer, substrate activation and FFA dehydrogenation, thus boosting both the kinetics of H2O2 production and FFA photo‐oxidation to increase the efficiency. This is the first report about COFs for H2O2 photosynthesis coupled with biomass valorization, which might facilitate the exploration of porous‐crystalline catalysts in this field.
Rational Design and Expedient Synthesis of Heparan Sulfate Mimetics from Natural Aminoglycosides for Structure and Activity Relationship Studies
Authors: Wakpal Joseph , Pathiranage Vishaka , Walker Alice R. , Nguyen Hien M. 
Published: June 2023

AbstractHeparan sulfate (HS) contains variably repeating disaccharide units organized into high‐ and low‐sulfated domains. This rich structural diversity enables HS to interact with many proteins and regulate key signaling pathways. Efforts to understand structure‐function relationships and harness the therapeutic potential of HS are hindered by the inability to synthesize an extensive library of well‐defined HS structures. We herein report a rational and expedient approach to access a library of 27 oligosaccharides from natural aminoglycosides as HS mimetics in 7–12 steps. This strategy significantly reduces the number of steps as compared to the traditional synthesis of HS oligosaccharides from monosaccharide building blocks. Combined with computational insight, we identify a new class of four trisaccharide compounds derived from the aminoglycoside tobramycin that mimic natural HS and have a strong binding to heparanase but a low affinity for off‐target platelet factor‐4 protein.
Organopotassium‐Catalyzed Silylation of Benzylic C(sp3)−H Bonds
Authors: Neil Baptiste , Saadi Lamine , Fensterbank Louis , Chauvier Clément 
Published: June 2023

AbstractBenzylsilanes have found increasing applications in organic synthesis as bench‐stable synthetic intermediates, yet are mostly produced by stoichiometric procedures. Catalytic alternatives based on the atom‐economical silylation of benzylic C(sp3)−H bonds remain scarcely available as specialized directing groups and catalytic systems are needed to outcompete the kinetically‐favored silylation of C(sp2)−H bonds. Herein, we describe the first general and catalytic‐in‐metal undirected silylation of benzylic C(sp3)−H bonds under ambient, transition metal‐free conditions using stable tert‐butyl‐substituted silyldiazenes (tBu−N=N−SiR3) as silicon source. The high activity and selectivity of the catalytic system, exemplified by the preparation of various mono‐ or gem‐bis benzyl(di)silanes, originates from the facile generation of organopotassium reagents, including tert‐butylpotassium.
Joint intention understanding in children with autism spectrum disorder
Authors: Hou Wenwen , Li Xue , Yang Yunmei , Li Jing 
Published: June 2023

AbstractThis study examined the ability of children with autism spectrum disorder (ASD) to generate joint intention‐based action prediction in a joint action task. Children were presented with a series of videos in which two actors either played with blocks based on joint intention (social condition) or played with blocks independently (nonsocial condition). In the familiarization stage, two actors demonstrated how they played with blocks three times. In the test stage, one actor left the scene, and another actor grasped a block and asked where she should place it. Children's gaze behavior was assessed by an eye tracker. After watching videos, children were asked to answer two questions: an action prediction question and an intention understanding question. The results showed that in the implicit eye movement task, children with ASD and typically developing (TD) children exhibited location‐based anticipatory gaze under both conditions. However, in terms of explicit behavioral responses, TD children showed higher accuracy in response to action prediction questions and intention understanding questions than children with ASD in the social condition, while no significant group difference was found in the nonsocial condition. These results indicate that children with ASD have difficulty understanding joint intention and that their action prediction is primarily driven by bottom‐up sensory inputs.