bluuebunny/crossref_metadata_2025_split huggingface dataset:
Dynamic Stimulations with Bioengineered Extracellular Matrix‐Mimicking Hydrogels for Mechano Cell Reprogramming and Therapy
Authors: Shou Yufeng , Teo Xin Yong , Wu Kenny Zhuoran , Bai Bingyu , Kumar Arun R. K. , Low Jessalyn , Le Zhicheng , Tay Andy 
Published: April 2023

AbstractCells interact with their surrounding environment through a combination of static and dynamic mechanical signals that vary over stimulus types, intensity, space, and time. Compared to static mechanical signals such as stiffness, porosity, and topography, the current understanding on the effects of dynamic mechanical stimulations on cells remains limited, attributing to a lack of access to devices, the complexity of experimental set‐up, and data interpretation. Yet, in the pursuit of emerging translational applications (e.g., cell manufacturing for clinical treatment), it is crucial to understand how cells respond to a variety of dynamic forces that are omnipresent in vivo so that they can be exploited to enhance manufacturing and therapeutic outcomes. With a rising appreciation of the extracellular matrix (ECM) as a key regulator of biofunctions, researchers have bioengineered a suite of ECM‐mimicking hydrogels, which can be fine‐tuned with spatiotemporal mechanical cues to model complex static and dynamic mechanical profiles. This review first discusses how mechanical stimuli may impact different cellular components and the various mechanobiology pathways involved. Then, how hydrogels can be designed to incorporate static and dynamic mechanical parameters to influence cell behaviors are described. The Scopus database is also used to analyze the relative strength in evidence, ranging from strong to weak, based on number of published literatures, associated citations, and treatment significance. Additionally, the impacts of static and dynamic mechanical stimulations on clinically relevant cell types including mesenchymal stem cells, fibroblasts, and immune cells, are evaluated. The aim is to draw attention to the paucity of studies on the effects of dynamic mechanical stimuli on cells, as well as to highlight the potential of using a cocktail of various types and intensities of mechanical stimulations to influence cell fates (similar to the concept of biochemical cocktail to direct cell fate). It is envisioned that this progress report will inspire more exciting translational development of mechanoresponsive hydrogels for biomedical applications.
Recent Advances and Perspectives on Supported Catalysts for Heterogeneous Hydrogen Production from Ammonia Borane
Authors: Guan Shuyan , Liu Yanyan , Zhang Huanhuan , Shen Ruofan , Wen Hao , Kang Naixin , Zhou Jingjing , Liu Baozhong , Fan Yanping , Jiang Jianchun , Li Baojun 
Published: April 2023

AbstractAmmonia borane (AB), a liquid hydrogen storage material, has attracted increasing attention for hydrogen utilization because of its high hydrogen content. However, the slow kinetics of AB hydrolysis and the indefinite catalytic mechanism remain significant problems for its large‐scale practical application. Thus, the development of efficient AB hydrolysis catalysts and the determination of their catalytic mechanisms are significant and urgent. A summary of the preparation process and structural characteristics of various supported catalysts is presented in this paper, including graphite, metal‐organic frameworks (MOFs), metal oxides, carbon nitride (CN), molybdenum carbide (MoC), carbon nanotubes (CNTs), boron nitride (h‐BN), zeolites, carbon dots (CDs), and metal carbide and nitride (MXene). In addition, the relationship between the electronic structure and catalytic performance is discussed to ascertain the actual active sites in the catalytic process. The mechanism of AB hydrolysis catalysis is systematically discussed, and possible catalytic paths are summarized to provide theoretical considerations for the designing of efficient AB hydrolysis catalysts. Furthermore, three methods for stimulating AB from dehydrogenation by‐products and the design of possible hydrogen product‐regeneration systems are summarized. Finally, the remaining challenges and future research directions for the effective development of AB catalysts are discussed.
Electrolyte Gated Synaptic Transistor based on an Ultra‐Thin Film of La0.7Sr0.3MnO3
Authors: López Alejandro , Tornos Javier , Peralta Andrea , Barbero Isabel , Fernandez‐Canizares Francisco , Sanchez‐Santolino Gabriel , Varela María , Rivera Alberto , Camarero Julio , León Carlos , Santamaría Jacobo , Romera Miguel 
Published: April 2023

AbstractDeveloping electronic devices capable of reproducing synaptic functionality is essential in the context of implementing fast, low‐energy consumption neuromorphic computing systems. Hybrid ionic/electronic three‐terminal synaptic transistors are promising as efficient artificial synapses since they can process information and learn simultaneously. In this work, an electrolyte‐gated synaptic transistor is reported based on an ultra‐thin epitaxial La0.7Sr0.3MnO3 (LSMO) film, a half‐metallic system close to a metal‐insulator transition. The dynamic control of oxygen composition of the manganite ultra‐thin film with voltage pulses applied through the gate terminal allows reversible modulation of its electronic properties in a non‐volatile manner. The conductance modulation can be finely tuned with the amplitude, duration, and number of gating pulses, providing different alternatives to gradually update the synaptic weights. The transistor implements essential synaptic features such as excitatory postsynaptic potential, paired‐pulse facilitation, long‐term potentiation/depression of synaptic weights, and spike‐time‐dependent plasticity. These results constitute an important step toward the development of neuromorphic computing devices leveraging the tunable electronic properties of correlated oxides, and pave the way toward enhancing future device functionalities by exploiting the magnetic (spin) degree of freedom of the half metallic transistor channel.
Largely Reducing the Contact Resistance of Molybdenum Ditelluride by In Situ Potassium Modification
Authors: Cong Xiangna , Shah Muhammad Najeeb Ullah , Zheng Yue , He Wenlong 
Published: April 2023

AbstractSemiconducting molybdenum ditelluride (MoTe2) is widely reported owing to its favorable electronic and optoelectronic properties. The effective modulation of its electrical characteristics has garnered growing attention in regard to building high‐performance MoTe2‐based complementary devices. However, the inherent Schottky barrier (SB) in MoTe2‐based devices severely inhibits the charge‐carrier injection efficiency, leading to a high contact resistance between MoTe2 and contact metals. Here, an efficient method is presented for reducing the SB height of field‐effect transistors (FETs) based on MoTe2 by in situ potassium modification. Interestingly, the electrons transported from K continuously change the electrical characteristics of MoTe2 FET from ambipolar to n‐type with an improvement of electron mobility of over one order of magnitude. Meanwhile, the contact resistance of MoTe2 FET is significantly decreased from 11.5 to 0.4 kΩ µm. By regulating the modification region spatially, it is possible to create a complementary inverter with a high gain of ≈32 at VDD = 3 V. This research demonstrates a relatively simple method for optimizing the contact for MoTe2‐based devices and tuning the electrical properties of MoTe2 for future high‐performance complementary electronics.
Coupling Controlled Dual‐Band Tunable Electromagnetic Extraordinary Transmission in Graphene Hybrid Metasurfaces
Authors: Nan Jiameng , Zhang Yujing , Xie Yu , Li Zhichen , Yang Ruisheng , Xu Jing , Fu Quanhong , Zhang Fuli , Fan Yuancheng 
Published: April 2023

AbstractA metasurface is a kind of ultrathin artificial composite composed of subwavelength elements with unique abilities in manipulating electromagnetic waves. However, the static nature of its conventional metallic/dielectric constituent material has limited its fixed functionality in narrow frequency ranges. The two‐dimensional carbon sheet, i.e., graphene, is a promising platform for effectively tuning the functionality as well as operation frequency band of metasurface. Here, the authors propose and demonstrate a kind of graphene hybrid metasurface for dual‐band extraordinary electromagnetic transmission (EET). The metasurface is composed of two graphene/metal hybrid resonators with EET properties. It is shown that the EET of the graphene hybrid metasurfaces can be tuned by increasing the bias voltage on the graphene from 0 to 3 V. Furthermore, it is found that the transmission amplitude and operating frequency band of EET can be controlled by changing the relative position and thus the coupling of the two graphene hybrid resonators. The proposed design strategy of the hybrid metasurfaces is promising for many applications based on active EM or optical modulations.
Magnetic Measurements Applied to Energy Storage
Authors: Li Xiangkun , Zhang Leqing , Liu Hengjun , Li Qiang , Hou Yanglong 
Published: April 2023

AbstractHow to increase energy storage capability is one of the fundamental questions, it requires a deep understanding of the electronic structure, redox processes, and structural evolution of electrode materials. These thorny problems now usually involve spin–orbit, spin‐related electron configuration, etc., which cannot be probed using conventional testing techniques. Considering the intimate connection between spin and magnetic properties, using electron spin as a probe, magnetic measurements make it possible to analyze energy storage processes from the perspective of spin and magnetism. Owing to the capability of characterizing spin properties and high compatibility with the energy storage field, magnetic measurements are proven to be powerful tools for contributing to the progress of energy storage. In this review, several typical applications of magnetic measurements in alkali metal ion batteries research to emphasize the intimate connection between the magnetic properties and electronic structure, which is associated with the electrochemical performance of the electrode materials, are presented. Finally, the current challenges of magnetic measurements and the prospects for enhanced analysis of energy storage systems are discussed.
Synthesis of Chiral β‐Hydroxy Selenides by Ruthenium‐catalysed Transfer Hydrogenation of α‐Aryl Selenomethyl Ketones
Authors: Liu Qixing , Liu Mengna , Chen Jinbiao , Wang Jinlong , Zhou Haifeng 
Published: April 2023

AbstractA highly efficient transfer hydrogenation of α‐aryl selenomethyl ketones, using readily available chiral diamine‐derived ruthenium complex as a catalyst and a mixture of formic acid and triethylamine as a hydrogen source in dichloromethane under ambient conditions, is described. A wide range of chiral β‐hydroxy selenides was obtained in 90–99% ee values and moderate to good yields. The practicability is also demonstrated by a gram‐scale synthesis and downstream derivatization.
Tuning Local Charge Distribution in Multicomponent Covalent Organic Frameworks for Dramatically Enhanced Photocatalytic Uranium Extraction
Authors: Yang Hui , Hao Mengjie , Xie Yinghui , Liu Xiaolu , Liu Yanfang , Chen Zhongshan , Wang Xiangke , Waterhouse Geoffrey I. N. , Ma Shengqian 
Published: April 2023

AbstractOptimizing the electronic structure of covalent organic framework (COF) photocatalysts is essential for maximizing photocatalytic activity. Herein, we report an isoreticular family of multivariate COFs containing chromenoquinoline rings in the COF structure and electron‐donating or withdrawing groups in the pores. Intramolecular donor‐acceptor (D‐A) interactions in the COFs allowed tuning of local charge distributions and charge carrier separation under visible light irradiation, resulting in enhanced photocatalytic performance. By optimizing the optoelectronic properties of the COFs, a photocatalytic uranium extraction efficiency of 8.02 mg/g/day was achieved using a nitro‐functionalized multicomponent COF in natural seawater, exceeding the performance of all COFs reported to date. Results demonstrate an effective design strategy towards high‐activity COF photocatalysts with intramolecular D‐A structures not easily accessible using traditional synthetic approaches.
Enhancing Electrochemical Nitrate Reduction to Ammonia over Cu Nanosheets via Facet Tandem Catalysis
Authors: Fu Yunfan , Wang Shuo , Wang Yi , Wei Pengfei , Shao Jiaqi , Liu Tianfu , Wang Guoxiong , Bao Xinhe 
Published: April 2023

AbstractElectrochemical conversion of nitrate (NO3−) into ammonia (NH3) represents a potential way for achieving carbon‐free NH3 production while balancing the nitrogen cycle. Herein we report a high‐performance Cu nanosheets catalyst which delivers a NH3 partial current density of 665 mA cm−2 and NH3 yield rate of 1.41 mmol h−1 cm−2 in a flow cell at −0.59 V vs. reversible hydrogen electrode. The catalyst showed a high stability for 700 h with NH3 Faradaic efficiency of ≈88 % at 365 mA cm−2. In situ spectroscopy results verify that Cu nanosheets are in situ derived from the as‐prepared CuO nanosheets under electrochemical NO3− reduction reaction conditions. Electrochemical measurements and density functional theory calculations indicate that the high performance is attributed to the tandem interaction of Cu(100) and Cu(111) facets. The NO2− generated on the Cu(100) facets is subsequently hydrogenated on the Cu(111) facets, thus the tandem catalysis promotes the crucial hydrogenation of *NO to *NOH for NH3 production.
Construction of Thioamide Peptides from Chiral Amino Acids
Authors: Liao Yanyan , Zhang Shunmin , Jiang Xuefeng 
Published: April 2023

AbstractThioamide peptides were synthesized in a straightforward one‐pot process via the linkage of diverse natural amino acids in the presence of thiolphosphonate and trichlorosilane, wherein carbonyl groups were replaced with thiono compounds with minimal racemization. Experimental and computational mechanistic studies demonstrated that the trichlorosilane enables the activation of carboxylic acids via intense interactions with the Si−O bond, followed by coupling of the carboxylic acids with thiolphosphonate to obtain the key intermediate S‐acyl dithiophosphate. Silyl‐activated quadrangular metathesis transition states afforded the thioamide peptides. The potential applications of these thioamide peptides were further highlighted via late‐stage linkages of diverse natural products and pharmaceutical drugs and the thioamide moiety.
Prussian Blue Analogues with Optimized Crystal Plane Orientation and Low Crystal Defects toward 450 Wh kg−1 Alkali‐Ion Batteries
Authors: Zhang Hang , Gao Yun , Peng Jian , Fan Yameng , Zhao Lingfei , Li Li , Xiao Yao , Pang Wei Kong , Wang Jiazhao , Chou Shu‐Lei 
Published: April 2023

AbstractPrussian blue analogues (PBAs) have been regarded as promising cathode materials for alkali‐ion batteries owing to their high theoretical energy density and low cost. However, the high water and vacancy content of PBAs lower their energy density and bring safety issues, impeding their large‐scale application. Herein, a facile “potassium‐ions assisted” strategy is proposed to synthesize highly crystallized PBAs. By manipulating the dominant crystal plane and suppressing vacancies, the as‐prepared PBAs exhibit increased redox potential resulting in high energy density up to ≈450 Wh kg−1, which is at the same level of the well‐known LiFePO4 cathodes for lithium‐ion batteries. Remarkably, unconventional highly‐reversible phase evolution and redox‐active pairs were identified by multiple in situ techniques for the first time. The preferred guest‐ion storage sites and migration mechanism were systematically analysed through theoretical calculations. We believe these results could inspire the design of safe with high energy density.
Multi‐Resonance Building‐Block‐Based Electroluminescent Material: Lengthening Emission Maximum and Shortening Delayed Fluorescence Lifetime
Authors: Cai Xinliang , Pu Yexuan , Li Chenglong , Wang Zhiheng , Wang Yue 
Published: April 2023

AbstractMulti‐resonance thermally activated delayed fluorescence (MR‐TADF) materials are considered a class of organic materials with exceptional electronic and optical properties, which make them promising for the applications in organic light‐emitting diodes (OLEDs). In this study, we improved, synthesized, and characterized a multiple‐resonance type emitter based on the assembly of MR‐building blocks (MR‐BBs). By optimizing the geometric arrangement of MR‐BBs, we were able to generate narrowband emission in the longer wavelength region and shorten the delayed excited‐state lifetime, resulting in improved emission efficiency compared to the parent molecule. Our proof‐of‐concept molecule, m‐DBCz, exhibited narrowband yellowish‐green TADF emission with a full width at half‐maximum of 32 nm and a small singlet‐triplet energy gap of 0.04 eV. The OLED developed using m‐DBCz as the emitter demonstrated electroluminescence at 548 nm and achieved a high external quantum efficiency (EQE) of 34.9 %. Further optimization of the device resulted in a high external quantum efficiency of 36.3 % and extremely low efficiency roll‐off, with EQE values of 30.1 % and 27.7 % obtained even at high luminance levels of 50 000 and 100 000 cd m−2. These results demonstrate the full potential of MR‐TADF materials for applications on ultrahigh‐luminance OLEDs.
Layered Zeolite for Assembly of Two‐Dimensional Separation Membranes for Hydrogen Purification
Authors: Wang Jilong , Fan Yaqi , Jiang Jingang , Wan Zheng , Pang Shuyue , Guan Yejun , Xu Hao , He Xiao , Ma Yanhang , Huang Aisheng , Wu Peng 
Published: April 2023

AbstractMembrane separation is an energy‐efficient and environmentally friendly process. Two‐dimensional (2D) molecular sieving membranes featuring unique nanopores and low transport resistance have the potential to achieve highly permeable and selective mixture separation with low energy consumption. High‐aspect‐ratio zeolite nanosheets with intrinsic molecular‐sieving pores perpendicular to the layers are desirable building blocks for fabricating high‐performance 2D zeolite membrane. However, a wider application of 2D zeolitic membranes is restricted by the limited number of recognized zeolite nanosheets. Herein, we report a swollen layered zeolite, ECNU‐28, with SZR topology and eight‐member ring (8‐MR, 3.0 Å×4.8 Å) pores normal to the nanosheets. It can be easily exfoliated to construct 2D membrane, which shows a high hydrogen selectivity up to 130 from natural gas and is promising for hydrogen purification and greenhouse gas capture.
Selective Functionalisation of 5‐Methylcytosine by Organic Photoredox Catalysis
Authors: Simpson Mathew M. , Lam Ching Ching , Goodman Jonathan M. , Balasubramanian Shankar 
Published: April 2023

AbstractThe epigenetic modification 5‐methylcytosine plays a vital role in development, cell specific gene expression and disease states. The selective chemical modification of the 5‐methylcytosine methyl group is challenging. Currently, no such chemistry exists. Direct functionalisation of 5‐methylcytosine would improve the detection and study of this epigenetic feature. We report a xanthone‐photosensitised process that introduces a 4‐pyridine modification at a C(sp3)−H bond in the methyl group of 5‐methylcytosine. We propose a reaction mechanism for this type of reaction based on density functional calculations and apply transition state analysis to rationalise differences in observed reaction efficiencies between cyanopyridine derivatives. The reaction is initiated by single electron oxidation of 5‐methylcytosine followed by deprotonation to generate the methyl group radical. Cross coupling of the methyl radical with 4‐cyanopyridine installs a 4‐pyridine label at 5‐methylcytosine. We demonstrate use of the pyridination reaction to enrich 5‐methylcytosine‐containing ribonucleic acid.
Reactive Polymer as Artificial Solid Electrolyte Interface for Stable Lithium Metal Batteries
Authors: Naren Tuoya , Kuang Gui‐Chao , Jiang Ruheng , Qing Piao , Yang Hao , Lin Jialin , Chen Yuejiao , Wei Weifeng , Ji Xiaobo , Chen Libao 
Published: April 2023

AbstractLithium (Li) metal anodes have the highest theoretical capacity and lowest electrochemical potential making them ideal for Li metal batteries (LMBs). However, Li dendrite formation on the anode impedes the proper discharge capacity and practical cycle life of LMBs, particularly in carbonate electrolytes. Herein, we developed a reactive alternative polymer named P(St‐MaI) containing carboxylic acid and cyclic ether moieties which would in situ form artificial polymeric solid electrolyte interface (SEI) with Li. This SEI can accommodate volume changes and maintain good interfacial contact. The presence of carboxylic acid and cyclic ether pendant groups greatly contribute to the induction of uniform Li ion deposition. In addition, the presence of benzyl rings makes the polymer have a certain mechanical strength and plays a key role in inhibiting the growth of Li dendrites. As a result, the symmetric Li||Li cell with P(St‐MaI)@Li layer can stably cycle for over 900 h under 1 mA cm−2 without polarization voltage increasing, while their Li||LiFePO4 full batteries maintain high capacity retention of 96 % after 930 cycles at 1C in carbonate electrolytes. The innovative strategy of artificial SEI is broadly applicable in designing new materials to inhibit Li dendrite growth on Li metal anodes.
Insertion of Chemical Handles into the Backbone of DNA during Solid‐Phase Synthesis by Oxidative Coupling of Amines to Phosphites
Authors: Hansen Rikke A. , Märcher Anders , Pedersen Kristian Nørgaard , Gothelf Kurt V. 
Published: April 2023

AbstractConjugation of molecules or proteins to oligonucleotides can improve their functional and therapeutic capacity. However, such modifications are often limited to the 5′ and 3′ end of oligonucleotides. Herein, we report the development of an inexpensive and simple method that allows for the insertion of chemical handles into the backbone of oligonucleotides. This method is compatible with standardized automated solid‐phase oligonucleotide synthesis, and relies on formation of phosphoramidates. A unique phosphoramidite is incorporated into a growing oligonucleotide, and oxidized to the desired phosphoramidate using iodine and an amine of choice. Azides, alkynes, amines, and alkanes have been linked to oligonucleotides via internally positioned phosphoramidates with oxidative coupling yields above 80 %. We show the design of phosphoramidates from secondary amines that specifically hydrolyze to the phosphate only at decreased pH. Finally, we show the synthesis of an antibody‐DNA conjugate, where the oligonucleotide can be selectively released in a pH 5.5 buffer.
Superatom‐in‐Superatom Nanoclusters: Synthesis, Structure, and Photoluminescence
Authors: Yi Hanseok , Song Suhwan , Han Sang Myeong , Lee Jieun , Kim Woojae , Sim Eunji , Lee Dongil 
Published: April 2023

AbstractWe report a new strategy in which a thiolate‐protected Ag25 nanocluster can be doped with open d‐shell group 8 (Ru, Os) and 9 (Ir) metals by forming metal hydride (RuH2, OsH2, IrH) superatoms with a closed d‐shell. Structural analyses using various experimental and theoretical methods revealed that the Ag25 nanoclusters were co‐doped with the open d‐shell metal and hydride species to produce superatom‐in‐superatom nanoclusters, establishing a novel superatom doping phenomenon for open d‐shell metals. The synthesized superatom‐in‐superatom nanoclusters exhibited dopant‐dependent photoluminescence (PL) properties. Comparative PL lifetime studies of the Ag25 nanoclusters doped with 8–10 group metals revealed that both radiative and nonradiative processes were significantly dependent on the dopant. The former is strongly correlated with the electron affinity of the metal dopant, whereas the latter is governed predominantly by the kernel structure changed upon the doping of the metal hydride(s).