bluuebunny/crossref_metadata_2025_split huggingface dataset:
Fabrication of 3D Printed, Core‐and‐Shell Implants as Controlled Release Systems for Local siRNA Delivery
Authors: Mahmoud Dina B. , Wölk Christian , Schulz‐Siegmund Michaela 
Published: September 2023

AbstractThe development and clinical translation of small interfering RNA (siRNA) therapies remains challenging owing to their poor pharmacokinetics. 3D printing technology presents a great opportunity to fabricate personalized implants for local and sustained delivery of siRNA. Hydrogels can mimic the mechanical properties of tissues, avoiding the problems associated with rigid implants. Herein, a thermoresponsive composite hydrogel suitable for extrusion 3D‐printing is formulated to fabricate controlled‐release implants loaded with siRNA‐Lipofectamine RNAiMAX complexes. A hydrogel matrix mainly composed of uncharged agarose to protect siRNA from decomplexation is selected. Additionally, pluronic F127 and gelatin are added to improve the printability, degradation, and cell adhesion to the implants. To avoid exposing siRNA to thermal stress during the printing process, a core‐and‐shell design is set up for the implants in which a core of siRNA‐complexes loaded‐pluronic F127 is printed without heat and enclosed with a shell comprising the thermoresponsive composite hydrogel. The release profile of siRNA‐complexes is envisioned to be controlled by varying the printing patterns. The results reveal that the implants sustain siRNA release for one month. The intactness of the released siRNA‐complexes is proven until the eighth day. Furthermore, by changing the printing patterns, the release profiles can be tailored.
Glycoprotein Injectable Hydrogels Promote Accelerated Bone Regeneration through Angiogenesis and Innervation
Authors: Barik Debyashreeta , Shyamal Sharmistha , Das Kapilash , Jena Sarita , Dash Mamoni 
Published: September 2023

AbstractGlycoproteins are gaining prominence as multifunctional biomaterials. The study reports development of glycoprotein mucin as biomaterial promoting bone regeneration. Mucin 1 deletion has resulted in stiffer femoral bones with scarce presence of osteoblasts in trabecular linings and its role has been established in determining bone mass and mineralization. Limited information about its structure limits its processability, exploration as biomaterial, which is discussed in this study. The role of mucin in ECM (extracellular cellular matrix) formation validated by RNA sequencing analysis of human bone marrow derived mesenchymal stem cells is reported. The structure and stability of mucins is dependent on the presence of glycans in its structure. A thermosensitive hydrogel acquired from thermosensitive Poly (N‐isopropyl acrylamide)‐(PNIPAM) modified mucin and collagen is developed. The hydrogel demonstrates porous structure and mechanical strength. Newly formed bone tissue is observed at 8 weeks post‐implantation in the hydrogel treated groups. The formation of blood vessels, nerves, and bone is observed with upregulation of angiopoietin (ANG), neurofilament heavy chain (NF‐H), and osteoadherin (OSAD) or osteocalcin (OCN) respectively in rat calvarial defects. The outcome demonstrates that the thermosensitive injectable hydrogel accelerates repair and healing in calvarial bone defects making it a promising biodegradable biomaterial capable of regenerating bone by promoting angiogenesis and innervation.
Magnetic Putty as a Reconfigurable, Recyclable, and Accessible Soft Robotic Material
Authors: Li Meng , Pal Aniket , Byun Junghwan , Gardi Gaurav , Sitti Metin 
Published: September 2023

AbstractMagnetically hard materials are widely used to build soft magnetic robots, providing large magnetic force/torque and macrodomain programmability. However, their high magnetic coercivity often presents practical challenges when attempting to reconfigure magnetization patterns, requiring a large magnetic field or heating. In this study, magnetic putty is introduced as a magnetically hard and soft material with large remanence and low coercivity. It is shown that the magnetization of magnetic putty can be easily reoriented with maximum magnitude using an external field that is only one‐tenth of its coercivity. Additionally, magnetic putty is a malleable, autonomous self‐healing material that can be recycled and repurposed. The authors anticipate magnetic putty could provide a versatile and accessible tool for various magnetic robotics applications for fast prototyping and explorations for research and educational purposes.
Ultra‐Bright Heptamethine Dye Clusters Based on a Self‐Adaptive Co‐Assembly Strategy for NIR‐IIb Biomedical Imaging
Authors: Dang Zetao , Liu Xiangping , Du Yijing , Wang Yajun , Zhou Ding , Zhang Yuewei , Zhu Shoujun 
Published: September 2023

AbstractDespite the wide range of applications of bright NIR‐II polymethine scaffolds in biomedical imaging, their solvatochromism and aggregation‐caused quenching (ACQ) effects in aqueous solutions limit their inherent brightness using traditional encapsulation methods, and effective hydrophilization strategies are still scarce. Here, a new set of Flav dyes is synthesized and PEGylated, followed by manufacturing DSPE@FlavP2000 nanoparticles using a self‐adaptive co‐assembly strategy to overcome these limitations. FlavP2000 can autonomously adjust its conformation when co‐assembled with DSPE‐PEG2000, resulting in high‐efficiency luminescence (≈44.9% fluorescence of Flav in DMSO). DSPE@FlavP2000 enables NIR‐IIb (>1500 nm) angiography with high signal‐to‐noise ratios. Notably, this co‐assembly can occur in situ between FlavP2000 with proteins in the living body based on a novel mechanism of brightness activation induced by disassembly (BAD), achieving consistent brightness as DSPE@FlavP2000 in blood or serum. The self‐adaptive co‐assembly strategy can be enhanced by incorporating an IPA moiety, which dynamically binds to albumin to prolong the dye's blood circulation time. Thus, the “enhanced” BAD is successfully applied to long‐term vascular imaging and sciatic nerve imaging. Both the self‐adaptive co‐assembly strategy and BAD phenomenon improve the selectivity and availability of the hydrophilization methods, paving the way for efficient biological applications of polymethine dyes.
Low‐Temperature Water‐Assisted Oxidation of Sponge‐Like Zn Nanostructures for Environmental and Energy Harvesting Applications
Authors: Laurenti Marco , Fontana Marco , Stassi Stefano , Sacco Adriano , Scalia Alberto , Bianco Stefano , Pirri Candido F. , Lamberti Andrea 
Published: September 2023

AbstractIn this work, the oxidation of sponge‐like nanostructured Zn films exploiting their interaction with water in liquid and vapor phases is investigated. By simply exposing the sputtered porous metal layers to a water vapor atmosphere or incubating them in water at different temperatures, the full conversion to ZnO is obtained. Depending on the kind of treatment, the oxidized ZnO layers exhibit different morphologies and physico‐chemical properties. When in combination with low heating of the surface, a better crystallinity and the growth of hexagonal nanocrystals (nanoprisms and nanoflowers) from the nanobranched Zn structure is observed, preserving the sponge‐like morphology of the starting material. Good photocatalytic activities for the degradation of an organic dye are measured under simulated sunlight irradiation. The piezoelectric and semiconducting response of the oxidized ZnO layers is also examined, revealing appealing performance in both cases and envisaging their use as nanogenerators and photoanode material in dye‐sensitized solar cells. The multifunctional properties of the oxidized ZnO film are discussed in terms of the selected water oxidation approach that tune the corresponding morphology and crystallinity. The low‐temperature oxidation approaches here proposed allow the fabrication of flexible semiconductive ZnO films highly desirable in different fields of nanoelectronics.
Boosting Phosphorescence Efficiency of Microstructures by Forming a Triplet Exciplex System
Authors: Yao Wei , Zhang Yusheng , Wang Jiamin , Zhang Shasha , Li Qiuying , Liu Kun , Wang Zhaoyu , Yin Chengzhu , Song Zhicheng , Ma Huili , Tao Youtian , Shi Huifang , An Zhongfu 
Published: September 2023

AbstractLow‐dimensional crystal structures with long lifetime phosphorescence hold great potential in biological imaging, sensors, and micro/nanophotonics. However, the high‐efficient phosphorescence is still scarce on the micro/nanoscale due to the strong nonradiative transitions and quenching of long‐lifetime triplet state caused by the large specific surface area. Herein, a one doped microstructure with high quantum yield phosphorescence is reported by doping an electron‐acceptor (guest) into an electron‐donor (host). The formation of a triplet exciplex between the donor and acceptor enables the doped microcrystals to display highly efficient long‐lived emission with 63.1% quantum yield, while the phosphorescence emissions of microstructures from a neat donor and acceptor are negligible. The emission mechanism in relation to the exciplex is elaborated from temperature‐dependent luminescence behavior and theoretical calculation. This work provides an effective strategy for achieving efficient long‐lived emissions at the micro‐scale, which will accelerate the research and development of advanced miniaturized functional devices.
Photocatalytic Redox‐Neutral Synthesis of Heterotriarymethanes
Authors: Guo Guozhe , Ye Youwan , Bao Xiazhen , Yuan Yong , Huo Congde 
Published: September 2023

AbstractThe C(sp3)−H bond decyanative arylations of diverse symmetrical and unsymmetrical BIMs have been successfully accomplished. Aromatic nitriles were utilized as components in the presence of thiobenzoic acid (TBA) under visible‐light irradiation. These redox‐neutral protocols provide a highly efficient and practical strategy for the synthesis of a broad range of bis(indolyl)‐substituted and mono(indolyl)‐substituted hetero‐triarylmethanes. Moreover, this synthetic approach has been expanded to the construction of indole‐substituted triarylmethanes bearing all‐carbon quaternary stereocenters. It is noteworthy that the preparation of the natural product Arsindolin A was effectively achieved using this methodology.
Asymmetrically Functionalized Electron‐Deficient π‐Conjugated System for Printed Single‐Crystalline Organic Electronics
Authors: Yu Craig P. , Kumagai Shohei , Tsutsumi Michitsuna , Kurosawa Tadanori , Ishii Hiroyuki , Watanabe Go , Hashizume Daisuke , Sugiura Hiroki , Tani Yukio , Ise Toshihiro , Watanabe Tetsuya , Sato Hiroyasu , Takeya Jun , Okamoto Toshihiro 
Published: September 2023

AbstractLarge‐area single‐crystalline thin films of n‐type organic semiconductors (OSCs) fabricated via solution‐processed techniques are urgently demanded for high‐end electronics. However, the lack of molecular designs that concomitantly offer excellent charge‐carrier transport, solution‐processability, and chemical/thermal robustness for n‐type OSCs limits the understanding of fundamental charge‐transport properties and impedes the realization of large‐area electronics. The benzo[de]isoquinolino[1,8‐gh]quinolinetetracarboxylic diimide (BQQDI) π‐electron system with phenethyl substituents (PhC2–BQQDI) demonstrates high electron mobility and robustness but its strong aggregation results in unsatisfactory solubility and solution‐processability. In this work, an asymmetric molecular design approach is reported that harnesses the favorable charge transport of PhC2–BQQDI, while introducing alkyl chains to improve the solubility and solution‐processability. An effective synthetic strategy is developed to obtain the target asymmetric BQQDI (PhC2–BQQDI–Cn). Interestingly, linear alkyl chains of PhC2–BQQDI–Cn (n = 5–7) exhibit an unusual molecular mimicry geometry with a gauche conformation and resilience to dynamic disorders. Asymmetric PhC2–BQQDI–C5 demonstrates excellent electron mobility and centimeter‐scale continuous single‐crystalline thin films, which are two orders of magnitude larger than that of PhC2–BQQDI, allowing for the investigation of electron transport anisotropy and applicable electronics.
Clickable Dynamic Bioinks Enable Post‐Printing Modifications of Construct Composition and Mechanical Properties Controlled over Time and Space
Authors: Tournier Pierre , Saint‐Pé Garance , Lagneau Nathan , Loll François , Halgand Boris , Tessier Arnaud , Guicheux Jérôme , Visage Catherine Le , Delplace Vianney 
Published: September 2023

AbstractBioprinting is a booming technology, with numerous applications in tissue engineering and regenerative medicine. However, most biomaterials designed for bioprinting depend on the use of sacrificial baths and/or non‐physiological stimuli. Printable biomaterials also often lack tunability in terms of their composition and mechanical properties. To address these challenges, the authors introduce a new biomaterial concept that they have termed “clickable dynamic bioinks”. These bioinks use dynamic hydrogels that can be printed, as well as chemically modified via click reactions to fine‐tune the physical and biochemical properties of printed objects after printing. Specifically, using hyaluronic acid (HA) as a polymer of interest, the authors investigate the use of a boronate ester‐based crosslinking reaction to produce dynamic hydrogels that are printable and cytocompatible, allowing for bioprinting. The resulting dynamic bioinks are chemically modified with bioorthogonal click moieties to allow for a variety of post‐printing modifications with molecules carrying the complementary click function. As proofs of concept, the authors perform various post‐printing modifications, including adjusting polymer composition (e.g., HA, chondroitin sulfate, and gelatin) and stiffness, and promoting cell adhesion via adhesive peptide immobilization (i.e., RGD peptide). The results also demonstrate that these modifications can be controlled over time and space, paving the way for 4D bioprinting applications.
High Hydrovoltaic Power Density Achieved by Universal Evaporating Potential Devices
Authors: Yu Fei , Li Jialun , Jiang Yi , Wang Liying , Yang Xijia , Yang Yue , Li Xuesong , Jiang Ke , Lü Wei , Sun Xiaojuan 
Published: September 2023

AbstractWhile hydrovoltaic electrical energy generation developments in very recent years have provided an alternative strategy to generate electricity from the direct interaction of materials with water, the two main issues still need to be addressed: achieving satisfactory output power density and understanding the reliable mechanism. In the present work, the integration of capacitors and water evaporation devices is proposed to provide a stable power supply. The feasible device structure consuming only water and air is green and environmentally sustainable, achieving a recorded power density of 142.72 µW cm−2. The output power of the series of devices is sufficient to drive portable electronic products with different voltage and current requirements, enabling self‐driving systems for portable appliances. It has been shown that the working behavior originates from evaporating potential other than streaming potential. The present work provides both theoretical support and an experimental design for realizing practical application of hydrovoltaic electrical energy generation devices.
Vanillin: An Effective Additive to Improve the Longevity of Zn Metal Anode in a 30 m ZnCl2 Electrolyte
Authors: Hoang David , Li Yaqiong , Jung Min Soo , Sandstrom Sean K. , Scida Alexis M. , Jiang Heng , Gallagher Trenton C. , Pollard Brenden A. , Jensen Rachel , Chiu Nan‐Chieh , Stylianou Kyriakos , Stickle William F. , Greaney P. Alex , Ji Xiulei 
Published: September 2023

AbstractIt remains a challenge to design aqueous electrolytes to secure the complete reversibility of zinc metal anodes. The concentrated water‐in‐salt electrolytes, e.g., 30 m ZnCl2, are promising candidates to address the challenges of the Zn metal anode. However, the pure 30 m ZnCl2 electrolyte fails to deliver a smooth surface morphology and a practically relevant Coulombic efficiency. Herein, it is reported that a small concentration of vanillin, 5 mg mLwater−1, added to 30 m ZnCl2 transforms the reversibility of Zn metal anode by eliminating dendrites, lowering the Hammett acidity, and forming an effective solid electrolyte interphase. The presence of vanillin in the electrolyte enables the Zn metal anode to exhibit a high Coulombic efficiency of 99.34% at a low current density of 0.2 mA cm−2, at which the impacts of the hydrogen evolution reaction are allowed to play out. Using this new electrolyte, a full cell Zn metal battery with an anode/cathode capacity (N/P) ratio of 2:1 demonstrates no capacity fading over 800 cycles.
Post‐Treatment of Metal Halide Perovskites: From Morphology Control, Defect Passivation to Band Alignment and Construction of Heterostructures
Authors: Hu Min , Zhu Yanqing , Zhou Zhongmin , Hao Mingwei , Harnmanasvate Chinnatip , Waiyawat Jutharat , Wang Yulong , Lu Jianfeng , An Qinyou , Li Xiong , Zhang Tian , Zhou Yuanyuan , Cheacharoen Rongrong , Rong Yaoguang 
Published: September 2023

AbstractMetal halide perovskite solar cells (PSCs) have witnessed a swift increase in power conversion efficiency in the past decade, emerging as one of the most promising next‐generation photovoltaic technologies for commercialization and low‐carbon energy generation. Through significant efforts in optimizing the processing techniques, high‐quality perovskite thin films can now be prepared with polycrystalline morphologies consisting of monolayer grains. Nevertheless, defects and microstructural disorders still form at the surface/heterointerface and in the bulk of the films. Post‐treatment of the as‐crystallized films has been intensively investigated for passivating these defects, being proved effective for improving the device performance. In this review, the versatile strategies for post‐treating the surface of perovskite thin films toward morphology control, defect passivation, and band alignment are discussed. The tailored surface properties are correlated to charge dynamics at interfaces and photovoltaic performance of PSCs. Since the perovskite heterostructures prepared by simple post‐treatments may suffer from degradation at high temperatures, the recent advances in preparing phase‐pure and stable perovskite heterostructures are also discussed. Finally, a perspective elaborating future opportunities for further enhancing the efficiency and stability of PSCs is provided.
Stress Relief in Metal Anodes: Mechanisms and Applications
Authors: Gu Jianan , Shi Yu , Du Zhiguo , Li Meicheng , Yang Shubin 
Published: September 2023

AbstractMetal anodes (lithium/sodium/zinc) are recognized as the most promising choice for rechargeable batteries due to their high theoretical capacity and low electrochemical redox potential. Unfortunately, metal anodes face serious metal dendrite problems, hindering their practical applications. Recent research has shown that metal dendrites can also be caused by high levels of stress generated during the metal deposition process. To address this issue, an alternative strategy based on stress relief is proposed to inhibit the growth of metal dendrites. Herein, this work aims to investigate the mechanism of stress generation and evolution within metal anodes. In addition, this work explores the utilization of stress to induce metal nucleation. This work further discuss the various experimental techniques used to study stress release in metal dendrites and review recent research findings on stress relief in metal dendrites within metal anodes. Specifically, this work examines how microstructure and processing conditions affect stress release and discuss potential strategies for improving the efficiency of stress relief strategies in metal dendrites. As a result, a deeper understanding of stress release in metal dendrites can lead to the development of rechargeable batteries with superior performance, longer cycle life, as well as enhanced safety for practical applications in various fields.
Bioelectrocatalytic CO2 Reduction by Mo‐Dependent Formylmethanofuran Dehydrogenase
Authors: Sahin Selmihan , Lemaire Olivier N. , Belhamri Mélissa , Kurth Julia M. , Welte Cornelia U. , Wagner Tristan , Milton Ross D. 
Published: September 2023

AbstractMassive efforts are invested in developing innovative CO2‐sequestration strategies to counter climate change and transform CO2 into higher‐value products. CO2‐capture by reduction is a chemical challenge, and attention is turned toward biological systems that selectively and efficiently catalyse this reaction under mild conditions and in aqueous solvents. While a few reports have evaluated the effectiveness of isolated bacterial formate dehydrogenases as catalysts for the reversible electrochemical reduction of CO2, it is imperative to explore other enzymes among the natural reservoir of potential models that might exhibit higher turnover rates or preferential directionality for the reductive reaction. Here, we present electroenzymatic catalysis of formylmethanofuran dehydrogenase, a CO2‐reducing‐and‐fixing biomachinery isolated from a thermophilic methanogen, which was deposited on a graphite rod electrode to enable direct electron transfer for electroenzymatic CO2 reduction. The gas is reduced with a high Faradaic efficiency (109±1 %), where a low affinity for formate prevents its electrochemical reoxidation and favours formate accumulation. These properties make the enzyme an excellent tool for electroenzymatic CO2‐fixation and inspiration for protein engineering that would be beneficial for biotechnological purposes to convert the greenhouse gas into stable formate that can subsequently be safely stored, transported, and used for power generation without energy loss.
Hydrogen Transport and Evolution in Ni‐MH Batteries by Neutron Imaging
Authors: Nikolic Marin , Cesarini Alessia , Billeter Emanuel , Weyand Fabian , Trtik Pavel , Strobl Markus , Borgschulte Andreas 
Published: September 2023

AbstractEfficiency losses due to side reactions are one of the main challenges in battery development. Despite providing valuable insights, the results of standard analysis on the individual components cannot be simply extrapolated to the full operating system. Therefore, non‐destructive, and high resolution approaches that allow the investigation of the full system are desired. Herein, we combined neutron radiography and tomography with electrical monitoring of the state of charge of commercial Ni‐mischmetal hydride batteries, to track the exchange and transport of hydrogen under operating conditions. This non‐destructive approach allowed both the quantification of the hydrogen distribution in the electrodes in 4D, and the distinction between the electrochemically exchanged hydrogen and the hydrogen gas pressure generated by side reactions, as a function of the applied potential and current. One of the most counter‐intuitive observation is that the generation of hydrogen gas during discharge depends on the charging state of the battery. The results presented provide critical new insights in the mechanisms governing the electrochemical processes during Nimischmetal hydride battery operation, and also pave the way for the extrapolation of this approach to the investigation of state‐of‐the‐art Li‐ions batteries.