bluuebunny/crossref_metadata_2025_split huggingface dataset:
A Gas‐Steamed MOF Route to P‐Doped Open Carbon Cages with Enhanced Zn‐Ion Energy Storage Capability and Ultrastability
Authors: Hou Chun‐Chao , Wang Yu , Zou Lianli , Wang Miao , Liu Hongwen , Liu Zheng , Wang Hao‐Fan , Li Caixia , Xu Qiang 
Published: June 2021

AbstractCarbon micro/nanocages have received great attention, especially in electrochemical energy‐storage systems. Herein, as a proof‐of‐concept, a solid‐state gas‐steamed metal–organic‐framework approach is designed to fabricate carbon cages with controlled openings on walls, and N, P dopants. Taking advantage of the fabricated carbon cages with large openings on their walls for enhanced kinetics of mass transport and N, P dopants within the carbon matrix for favoring chemical adsorption of Zn ions, when used as carbon cathodes for advanced aqueous Zn‐ion hybrid supercapacitors (ZHSCs), such open carbon cages (OCCs) display a wide operation voltage of 2.0 V and an enhanced capacity of 225 mAh g−1 at 0.1 A g−1. Also, they exhibit an ultralong cycling lifespan of up to 300 000 cycles with 96.5% capacity retention. Particularly, such OCCs as electrode materials lead to a soft‐pack ZHSC device, delivering a high energy density of 97 Wh kg−1 and a superb power density of 6.5 kW kg−1. Further, the device can operate in a wide temperature range from −25 to + 40 °C, covering the temperatures for practical applications in daily life.
Crowning Metal Ions by Supramolecularization as a General Remedy toward a Dendrite‐Free Alkali‐Metal Battery
Authors: Lu Ziyang , Guo Yong , Zhang Siwei , Wu Shichao , Meng Rongwei , Hong Shuang , Li Jiaxi , Xue Haoyu , Zhang Boyi , Fan Dinghui , Zhang Yifang , Zhang Chen , Lv Wei , Yang Quan‐Hong 
Published: June 2021

AbstractAlkali metals have low potentials and high capacities, making them ideal anodes for next‐generation batteries, but they suffer major problems, including dendrite growth and low Coulombic efficiency (CE). Achieving uniform metal deposition and having a reliable solid electrolyte interphase (SEI) are the basic requirements for overcoming these problems. Here, a general remedy is reported for various alkali‐metal anodes by the supramolecularization of alkali‐metal cations with crown ethers that follows a size‐matching rule. The positively charged supramolecular complex provides electrostatic shielding layers to regulate metal deposition and suppress dendrite formation. More promisingly, it reforms electric double layers and drives the production of organic‐dominated SEIs with improved flexibility that can accommodate large volume changes. The high flexibility of SEIs during metal deposition and dissolution reduces the amount of dead metal and improves CE and cycling stability. Specifically, a 200% excess Li‐based full cell has a capacity retention of ≈100% after 100 cycles. This crown‐like supramolecularization strategy is a new chemistry that may be used for the production of dendrite‐free metal‐anode‐based batteries not limited to the cases with alkali metal. It is also expected as a practical technology to improve the uniformity of coatings produced in the electrodeposition industry.
Multimodal Tuning of Synaptic Plasticity Using Persistent Luminescent Memitters
Authors: Bian Hongyu , Qin Xian , Wu Yiming , Yi Zhigao , Liu Sirui , Wang Yu , Brites Carlos D. S. , Carlos Luís D. , Liu Xiaogang 
Published: June 2021

AbstractMimicking memory processes, including encoding, storing, and retrieving information, is critical for neuromorphic computing and artificial intelligence. Synaptic behavior simulations through electronic, magnetic, or photonic devices based on metal oxides, 2D materials, molecular complex and phase change materials, represent important strategies for performing computational tasks with enhanced power efficiency. Here, a special class of memristive materials based on persistent luminescent memitters (termed as a portmanteau of “memory” and “emitter”) with optical characteristics closely resembling those of biological synapses is reported. The memory process and synaptic plasticity can be successfully emulated using such memitters under precisely controlled excitation frequency, wavelength, pulse number, and power density. The experimental and theoretical data suggest that electron‐coupled trap nucleation and propagation through clustering in persistent luminescent memitters can explain experience‐dependent plasticity. The use of persistent luminescent memitters for multichannel image memorization that allows direct visualization of subtle changes in luminescence intensity and realization of short‐term and long‐term memory is also demonstrated. These findings may promote the discovery of new functional materials as artificial synapses and enhance the understanding of memory mechanisms.
Amine‐Acrylate Liquid Single Crystal Elastomers Reinforced by Hydrogen Bonding
Authors: Zou Weike , Lin Xueyan , Terentjev Eugene M. 
Published: June 2021

AbstractLiquid crystalline elastomers (LCEs) have been considered one of the most promising material concepts for artificial muscles. However, accomplishing actuation of LCEs requires macroscopic alignment of the liquid‐crystalline orientation in the rubbery network, which imposes challenges in the materials chemistry and processing. A two‐stage curing strategy has been the dominating approach during last three decades. Despite its many successes, the method is difficult in practice and requires delicate experiential skills, dealing with intrinsic fragility of intermediate gels after the first crosslinking stage. Here, a robust fabrication method for monodomain LCE based on the amine‐acrylate aza‐Michael addition is developed, involving two readily commercially available components with no catalyst. The method is based on the large kinetic difference of hydrogen addition in primary amines to acrylates, which offers a sufficient gap separating two stages of curing and enabling versatile mechanical alignment techniques for manufacturing monodomain LCE in both liquid and gel states. Importantly, the mechanically robust network, helping processability at a partial‐crosslinking stage, is facilitated by the chemically generated hydrogen bonding all through the process, as a by‐product of hydrogen addition. Such a facile two‐component kit‐like fabrication should aid researchers from various fields in the search for a practical and reliable process of making soft actuators.
Magnetic Dynamic Polymers for Modular Assembling and Reconfigurable Morphing Architectures
Authors: Kuang Xiao , Wu Shuai , Ze Qiji , Yue Liang , Jin Yi , Montgomery S. Macrae , Yang Fengyuan , Qi H. Jerry , Zhao Ruike 
Published: June 2021

AbstractShape‐morphing magnetic soft materials, composed of magnetic particles in a soft polymer matrix, can transform shape reversibly, remotely, and rapidly, finding diverse applications in actuators, soft robotics, and biomedical devices. To achieve on‐demand and sophisticated shape morphing, the manufacture of structures with complex geometry and magnetization distribution is highly desired. Here, a magnetic dynamic polymer (MDP) composite composed of hard‐magnetic microparticles in a dynamic polymer network with thermally responsive reversible linkages, which permits functionalities including targeted welding for magnetic‐assisted assembly, magnetization reprogramming, and permanent structural reconfiguration, is reported. These functions not only provide highly desirable structural and material programmability and reprogrammability but also enable the manufacturing of functional soft architected materials such as 3D kirigami with complex magnetization distribution. The welding of magnetic‐assisted modular assembly can be further combined with magnetization reprogramming and permanent reshaping capabilities for programmable and reconfigurable architectures and morphing structures. The reported MDP are anticipated to provide a new paradigm for the design and manufacture of future multifunctional assemblies and reconfigurable morphing architectures and devices.
Bipolar Light‐Addressable Potentiometric Sensor Based on Fullerene Photosensitive Layer
Authors: Li Yun‐Chong , Jiao Bo , Zhang Yi‐Jun , Wang Jian , Ren Wei , Zhang De‐Wen , Hou Xun , Wu Zhao‐Xin 
Published: June 2021

AbstractLight‐addressable potentiometric sensor (LAPS) is highly attractive in many sectors, including human disease detection, drug screening, and environmental monitoring. Currently, classical LAPS chips adopt inorganic semiconductors, such as silicon, as the photosensitive layer. Organic semiconductors can provide the next generation of the photosensitive layer because of their high absorption efficiency, large structural variability, eco‐friendliness, and bendability. However, no promising organic materials have been reported so far for the construction of LAPS chips. Here, the authors demonstrate the potential of fullerene (C60), a π‐conjugated carbon molecule with high n‐type conduction, as a candidate material for the photosensitive layer of LAPS. They report on a peculiar bipolar photo‐response under both reverse and forward biased conditions for C60‐based LAPS. An oxygen‐trap‐induced space‐charge mechanism is proposed to explain the unique bipolar photo‐response phenomenon. The proposed C60‐based LAPS exhibits an excellent pH sensitivity of 150 mV/pH as well as a high spatial resolution of 3.8 µm. The authors anticipate that these results will spark interest in this field and enable the replacement of the inorganic‐semiconductor photosensitive layer by organic semiconductor materials for the construction of high‐performance LAPS.
In Situ Direct Laser Writing of 3D Graphene‐Laden Microstructures
Authors: Restaino Michael , Eckman Noah , Alsharhan Abdullah T. , Lamont Andrew C. , Anderson Jackson , Weinstein Dana , Hall Asha , Sochol Ryan D. 
Published: June 2021

AbstractA wide range of applications rely on the ability to integrate electrically conductive microstructures with microfluidic channels. To bypass the planar geometric restrictions of conventional microfabrication processes, researchers have recently explored the use of “Direct Laser Writing (DLW)”—a submicron‐scale additive manufacturing (or “3D printing”) technology—for creating conductive microfeatures with fully 3D configurations. Despite considerable progress in the development of DLW‐compatible photomaterials, thermal post‐processing requirements to support electrical conductivity remain a critical barrier to microfluidics integration. In this work, novel graphene‐laden photocomposites are investigated to enable DLW‐based printing of true 3D conductive microstructures directly inside of enclosed microchannels (i.e., in situ). Photoreactive composite materials comprising reduced graphene oxide (rGO) particle concentrations of up to 10 wt% exhibited high compatibility with DLW, with minimal optical interference at critical wavelengths. Developed rGO‐photocomposites revealed an ultimate DC conductivity of 9.85 ± 0.48 × 10−5 S m−1. Experimental results for DLW of 3D microcoils (1 wt% rGO; wire diameter = 10 µm; coil diameter = 40 µm) revealed an impedance of 2.71 ± 0.12 MΩ at 2 MHz. In addition, results for in situ DLW of geometrically sophisticated rGO‐laden microstructures suggest utility of the presented approach for potential 3D microelectronics‐based microfluidic applications.
Strongly Circularly Polarized Crystalline and β‐Phase Emission from Poly(9,9‐dioctylfluorene)‐Based Deep‐Blue Light‐Emitting Diodes
Authors: Wan Li , Shi Xingyuan , Wade Jessica , Campbell Alasdair J. , Fuchter Matthew J. 
Published: June 2021

AbstractA key challenge in the realization of circularly polarized polymer light‐emitting diodes (CP‐PLEDs) is the generation of highly circularly polarized deep‐blue electroluminescence (EL). Here, by blending the achiral luminescent polymer poly(9,9‐dioctylfluorene) (PFO) with a helically chiral molecule 1‐aza[6]helicene the authors present CP‐PLEDs with state‐of‐the‐art device performance for deep‐blue CP emission: for an inverted device with a semicrystalline microstructure a current efficiency (CE) of 1.13 cd A−1, a power efficiency (PE) of 0.81 lm W−1, and an EL dissymmetry (gEL) of −0.42 are achieved; for the planarized and extended “β‐phase” chain conformation a CE of 1.23 cd A−1, a PE of 0.63 lm W−1, and a gEL of −0.44 are achieved. While these two phases achieve both high CE, as well as gEL, the latter affords the first demonstration of chiral β‐phase emission from solid‐state PFO devices. Such strongly circularly polarized light is generated from a supramolecular assembly of interacting planar polymer backbones. The authors rationalize that the strong chiroptical effects observed within such chiral β‐phase PFO domains originate from coupled interchain aggregates. The findings not only demonstrate efficient deep‐blue CP‐PLEDs, but also provide insight into the mechanisms that underpin the strong CP emission from excitonically coupled polymer chains.
Origin of the Efficiency Roll‐Off in Single‐Layer Organic Light‐Emitting Diodes Based on Thermally Activated Delayed Fluorescence
Authors: van der Zee Bas , Li Yungui , Wetzelaer Gert‐Jan A. H. , Blom Paul W. M. 
Published: June 2021

AbstractThe efficiency roll‐off in organic light‐emitting diodes (OLEDs) based on thermally activated delayed fluorescence (TADF) is attributed to either singlet–triplet or triplet–triplet annihilation (TTA) as well as triplet–charge annihilation. The origin of the efficiency roll‐off on a TADF OLED consisting of a host‐less single‐layer emitter is studied. Varying the charge‐carrier concentration at constant exciton density or the exciton density at constant charge‐carrier density with temperature unambiguously shows that the dominant contribution to the roll‐off originates from TTA. Using an analytical model, also the TTA rate constant can be obtained. These results show that single‐layer TADF OLEDs are suited not only to determine the roll‐off mechanism, but also to provide its rate constant directly from OLED efficiency measurements.
A Flip‐Over Plasmonic Structure for Photoluminescence Enhancement of Encapsulated WS2 Monolayers
Authors: Liang Minpeng , Han Chunrui , Zheliuk Oleksandr , Chen Qihong , Wan Puhua , Peng Xiaoli , Zhang Le , Ye Jianting 
Published: June 2021

AbstractTransition metal dichalcogenide (TMD) monolayers, with their direct band gaps, have attracted wide attention from the fields of photonics and optoelectronics. However, monolayer semiconducting TMDs generally suffer from low excitation absorption and emission efficiency, limiting their further applications. Here a flip‐over plasmonic structure comprised of silver nano‐disk arrays supporting a WS2 monolayer sandwiched by hexagonal boron nitride (h‐BN) layers is demonstrated. The flip‐over configuration optimizes the optical process with a free excitation/emission path from the top and a strong plasmonic interaction from the bottom. As a result, the photoluminescence from the TMD monolayers can be greatly enhanced more than tenfold by optimizing the metasurface, which can be further improved nearly tenfold by optimizing the thickness of bottom h‐BN. This study shows the advantages of using the flip‐over structure, where the plasmonic interaction between the metasurface and TMDs can be tuned by introducing optimized plasmonic arrays and h‐BN layers with suitable thickness. This hybrid device configuration paves a reliable platform to study the light–matter interaction, achieving highly efficient plasmonic TMD devices.
Mn3O4 Nanozyme for Inflammatory Bowel Disease Therapy
Authors: Cheng Yuan , Cheng Chaoqun , Yao Jia , Yu Yijun , Liu Yufeng , Zhang He , Miao Leiying , Wei Hui 
Published: June 2021

AbstractRecently, reactive oxygen species (ROS) scavenging nanozymes have been developed as natural enzyme alternatives to treat inflammatory bowel disease (IBD) as well as other inflammatory diseases. Among them, manganese oxide nanozymes are advantageous because of remarkable biocompatibility and their good biodegradability. It is herein reported that phospholipid coated Mn3O4 nanozymes mimic both superoxide dismutase (SOD) and catalase (CAT) to effectively eliminate ROS that exacerbate inflammation and cause damages to tissues and organs. With the help of phospholipid decoration, the Mn3O4 nanozymes are well dispersed and show good stability. Moreover, the coating enables the successful fluorescence labelling to study their biodistribution and fate. Excitingly, the Mn3O4 nanozymes exhibit superior therapeutic efficacy for both ulcerative colitis (UC) and Crohn's disease (CD) in mouse models over aminosalicylic acid, a first‐line medication for IBD, under the same dosage. Thus, the Mn3O4 nanozymes in this work offer a promising nano‐medication for inflammation‐related disease therapy and broaden the spectrum of biomedical application of nanozymes.
Nanoengineering Apolipoprotein A1‐Based Immunotherapeutics
Authors: Schrijver David P. , de Dreu Anne , Hofstraat Stijn R. J. , Kluza Ewelina , Zwolsman Robby , Deckers Jeroen , Anbergen Tom , de Bruin Koen , Trines Mirre M. , Nugraha Eveline G. , Ummels Floor , Röring Rutger J. , Beldman Thijs J. , Teunissen Abraham J. P. , Fayad Zahi A. , van der Meel Roy , Mulder Willem J. M. 
Published: June 2021

AbstractIn the slipstream of targeting the adaptive immune system, innate immunotherapy strategies are being developed. In this context, technologies based on natural carrier vehicles that inherently interact with the innate immune system, are increasingly being considered. Immunoregulatory nanotherapeutics based on natural apolipoprotein A1 (apoA1) are discussed here. This protein is a helical, amphipathic macromolecule and the main constituent of high‐density lipoprotein. In that capacity, apoA1 interacts specifically with innate immune cells, such as monocytes and macrophages, to collect and transport lipophilic molecules throughout the body. Exactly these unique features make apoA1 a compelling elementary constituent of biocompatible self‐assembled nanotherapeutics. Such apoA1‐based nanotherapeutics (A1‐nanotherapeutics) can be engineered and functionalized to induce or mitigate an innate immune response or to orchestrate an adaptive immune response through antigen delivery to dendritic cells. The authors first discuss apoA1's properties and how these can be exploited to generate libraries of A1‐nanotherapeutics using advanced manufacturing approaches such as microfluidics or continuous flow methods. Using high‐throughput in vitro screening methods and in vivo imaging to identify promising formulations are then recommend. Finally, three distinct immunotherapy strategies are proposed to effectively treat a variety of diseases—including cancer, infection, and cardiovascular disease—and promote allograft survival in transplantation.
Enhanced Near‐Infrared Photocatalytic Eradication of MRSA Biofilms and Osseointegration Using Oxide Perovskite‐Based P–N Heterojunction
Authors: Mao Congyang , Zhu Weidong , Xiang Yiming , Zhu Yizhou , Shen Jie , Liu Xiangmei , Wu Shuilin , Cheung Kenneth M. C. , Yeung Kelvin Wai Kwok 
Published: June 2021

AbstractMethicillin‐resistant Staphylococcus aureus (MRSA) biofilm infections after orthopedic implant increase the risk of failure and potentially cause amputation of limbs or life‐threatening sepsis in severe cases. Additionally, satisfactory bone‐implant integration is another important indicator of an ideal implant. Here, an antibiotic‐free antibacterial nanofilm based on oxide perovskite‐type calcium titanate (CTO)/fibrous red phosphorus (RP) on titanium implant surface (Ti‐CTO/RP) in which the P–N heterojunction and internal electric field are established at the heterointerface, is designed. Near‐infrared light‐excited electron–hole pairs are effectively separated and transferred through the synergism of the internal electric field and band offset, which strongly boosts the photocatalytic eradication of MRSA biofilms by reactive oxygen species with an efficacy of 99.42% ± 0.22% in vivo. Additionally, the charge transfer endows the heterostructure with hyperthermia to assist biofilm eradication. Furthermore, CTO/RP nanofilm provides a superior biocompatible and osteoconductive platform that enables the proliferation and osteogenic differentiation of mesenchymal stem cells, thus contributing to the subsequent implant‐to‐bone osseointegration after eradicating MRSA biofilms.
Bias‐Polarity‐Dependent Direct and Inverted Marcus Charge Transport Affecting Rectification in a Redox‐Active Molecular Junction
Authors: Han Yingmei , Nickle Cameron , Maglione Maria Serena , Karuppannan Senthil Kumar , Casado‐Montenegro Javier , Qi Dong‐Chen , Chen Xiaoping , Tadich Anton , Cowie Bruce , Mas‐Torrent Marta , Rovira Concepció , Cornil Jérôme , Veciana Jaume , del Barco Enrique , Nijhuis Christian A. 
Published: June 2021

AbstractThis paper describes the transition from the normal to inverted Marcus region in solid‐state tunnel junctions consisting of self‐assembled monolayers of benzotetrathiafulvalene (BTTF), and how this transition determines the performance of a molecular diode. Temperature‐dependent normalized differential conductance analyses indicate the participation of the HOMO (highest occupied molecular orbital) at large negative bias, which follows typical thermally activated hopping behavior associated with the normal Marcus regime. In contrast, hopping involving the HOMO dominates the mechanism of charge transport at positive bias, yet it is nearly activationless indicating the junction operates in the inverted Marcus region. Thus, within the same junction it is possible to switch between Marcus and inverted Marcus regimes by changing the bias polarity. Consequently, the current only decreases with decreasing temperature at negative bias when hopping is “frozen out,” but not at positive bias resulting in a 30‐fold increase in the molecular rectification efficiency. These results indicate that the charge transport in the inverted Marcus region is readily accessible in junctions with redox molecules in the weak coupling regime and control over different hopping regimes can be used to improve junction performance.
A Smart Design Strategy for Super‐Elastic Hydrogel with Long‐Term Moisture, Extreme Temperature Resistance, and Non‐Flammability
Authors: Zhang Haiquan , Liu Zijing , Mai Junping , Wang Ning , Liu Houji , Zhong Jie , Mai Xianmin 
Published: June 2021

AbstractElastic hydrogel is a promising material category for designing biological muscles, repairable building materials, flexible electronic devices, and vulcanized rubber substitutes, which is required to have a long life, good self‐healing performance and extreme temperature tolerance. Herein, a super‐elastic mineral hydrogel is developed with long‐lasting moisture, based on dynamic physical crosslinking between hydrated calcium ion clusters and amide groups of polyacrylamide (PAM). The complex hydrogel exhibits a super stretchability of 13 600% at room temperature, and can maintain the super flexibility in a wide temperature range of −40–50 °C or for a long period of 28 days. Particularly, the soft material cannot be ignited under an open flame at 400–500 °C, because of coupling dual flame retardant mechanisms containing the endothermic effect of liquid water evaporation and the barrier effect of calcium mineral salt on oxygen. In conclusion, the novel complex hydrogel with excellent tensile property, stability in extreme temperature or long operating time, and flame retardancy may become a promising candidate in the fields of agriculture, food, construction, medicine, and machinery.