bluuebunny/crossref_metadata_2025_split huggingface dataset:
Efficient Circularly Polarized Electroluminescence from Chiral Thermally Activated Delayed Fluorescence Emitters Featuring Symmetrical and Rigid Coplanar Acceptors
Authors: Xie Feng‐Ming , Zhou Jing‐Xiong , Zeng Xin‐Yi , An Zhi‐Dong , Li Yan‐Qing , Han Dong‐Xue , Duan Peng‐Fei , Wu Zheng‐Guang , Zheng You‐Xuan , Tang Jian‐Xin 
Published: March 2021

AbstractCircularly polarized organic light‐emitting diodes (CP‐OLEDs) that enable circularly polarized luminescence (CPL) are promising for 3D display and photonic applications. However, the device efficiency and CPL character of CP‐OLEDs still lag behind the practical requirements. Here, two pairs of axially chiral emitting enantiomers, flexible (R/S)‐ODQPXZ and rigid (R/S)‐ODPPXZ, are reported by fusing (R/S)‐octahydro‐binaphthol chiral source, diphenyl quinoxaline (DQ)/dibenzo[a,c]phenazine (DP) acceptors and phenoxazine (PXZ) donors. The symmetrical chiral‐acceptor‐donor configuration endows them thermally activated delayed fluorescence (TADF) properties with small singlet–triplet energy gaps of 0.16 and 0.07 eV, high photoluminescence quantum yields of 92% and 89% in doped films, and obvious mirror‐image CPL characteristics, respectively. The CP‐OLEDs based on these TADF enantiomers not only show a maximum external quantum efficiency of 28.3% with yellow emission for (R/S)‐ODQPXZ and 20.3% with orange‐red emission for (R/S)‐ODPPXZ, but also display the CPL with dissymmetry factors (gEL) of 6.0 × 10−4 and 2.4 × 10−3, respectively. The high efficiency and obvious CPL of (R)‐ODPPXZ arise from a synergetic interplay of the TADF skeleton and the rigid coplanar acceptor for efficient chiral induction and suppressed intramolecular rotational quenching.
Dual Size/Charge‐Switchable Nanocatalytic Medicine for Deep Tumor Therapy
Authors: Wu Wencheng , Pu Yinying , Shi Jianlin 
Published: March 2021

AbstractElevating intratumoral levels of highly toxic reactive oxygen species (ROS) by nanocatalytic medicine for tumor‐specific therapy without using conventional toxic chemodrugs is recently of considerable interest, which, however, still suffers from less satisfactory therapeutic efficacy due to the relatively poor accumulation at the tumor site and largely blocked intratumoral infiltration of nanomedicines. Herein, an ultrasound (US)‐triggered dual size/charge‐switchable nanocatalytic medicine, designated as Cu‐LDH/HMME@Lips, is constructed for deep solid tumor therapy via catalytic ROS generations. The negatively charged liposome outer‐layer of the nanomedicine enables much‐prolonged blood circulation for significantly enhanced tumoral accumulation, while the positively charged Fenton‐like catalyst Cu‐LDH released from the liposome under the US stimulation demonstrates much enhanced intratumoral penetration via transcytosis. In the meantime, the co‐released sonosensitizer hematoporphyrin monomethyl ether (HMME) catalyze the singlet oxygen (1O2) generation upon the US irradiation, and deep‐tumoral infiltrated Cu‐LDH catalyzes the H2O2 decomposition to produce highly toxic hydroxyl radical (·OH) specifically within the mildly acidic tumor microenvironment (TME). The efficient intratumoral accumulation and penetration via the dual size/charge switching mechanism, and the ROS generations by both sonosensitization and Fenton‐like reactions, ensures the high therapeutic efficacy for the deep tumor therapy by the nanocatalytic medicine.
Cell‐Laden Multiple‐Step and Reversible 4D Hydrogel Actuators to Mimic Dynamic Tissue Morphogenesis
Authors: Ding Aixiang , Jeon Oju , Tang Rui , Lee Yu Bin , Lee Sang Jin , Alsberg Eben 
Published: March 2021

AbstractShape‐morphing hydrogels bear promising prospects as soft actuators and for robotics. However, they are mostly restricted to applications in the abiotic domain due to the harsh physicochemical conditions typically necessary to induce shape morphing. Here, multilayer hydrogel actuator systems are developed using biocompatible and photocrosslinkable oxidized, methacrylated alginate and methacrylated gelatin that permit encapsulation and maintenance of living cells within the hydrogel actuators and implement programmed and controlled actuations with multiple shape changes. The hydrogel actuators encapsulating cells enable defined self‐folding and/or user‐regulated, on‐demand‐folding into specific 3D architectures under physiological conditions, with the capability to partially bioemulate complex developmental processes such as branching morphogenesis. The hydrogel actuator systems can be utilized as novel platforms for investigating the effect of programmed multiple‐step and reversible shape morphing on cellular behaviors in 3D extracellular matrix and the role of recapitulating developmental and healing morphogenic processes on promoting new complex tissue formation.
Significantly Enhanced Electrochemical Redox for High‐Performance Electrochemical Capacitor via Active Ion‐Tunnel Oriented BaCoF4 Electrodes
Authors: Guo Changjin , Xie Jiyang , Wang Jing , Li Lun , Zhu Zhu , Xie Lin , Mao Yongyun , Hu Wanbiao 
Published: March 2021

AbstractActive plane and specific morphology with reduced particle sizes have long been considered a promising strategy to achieve superior electrochemical properties, but the active sites involved may not be sufficiently utilized or the surface atomic configurations may obscure the activity. Herein, a novel structural “active orientation” strategy is developed to overcome the aforementioned shortcomings and improve the efficiency at active sites. A transition‐metal fluoride BaCoF4 is well controlled to thin the dimensions along an active orientation through a sodium dodecyl benzene sulfonate assisted solution chemistry route. The active orientation facilitates the opening of the ionic pathways, for example, OH– in the electrolyte, to take full advantage of the redox activity of the electrochemically active Co2+/Co3+ cations in ‐BaCoF4, resulting in significantly enhanced electrochemical redox performance. A high specific capacitance (692 F g−1 at 1 A g−1 in 6 m KOH electrolyte) is achieved owing to active‐tunnels orientation, ≈five‐fold higher compared to its bulk counterpart. Strikingly, the asymmetric electrochemical capacitor (AEC) fabricated with ‐BaCoF4 and activated carbon exhibits an ultrahigh energy density of 147.7 Wh kg−1 at a power density of 1.025 kW kg−1 (also >100 Wh kg−1 at 5 kW kg−1), much higher than the majority of existing AEC systems.
Exceeding Single‐Pass Equilibrium with Integrated Absorption Separation for Ammonia Synthesis Using Renewable Energy—Redefining the Haber‐Bosch Loop
Authors: Smith Collin , Torrente‐Murciano Laura 
Published: March 2021

AbstractThe synthesis of ammonia through the Haber‐Bosch process has been at the foundation of the chemical industry for over 100 years, but when the energy and feedstock sources switch from fossil fuels to renewable electricity, the process needs to be reimagined. Herein, the successful integration of ammonia synthesis and separation is demonstrated in a recycle‐less process setting the foundations of green ammonia technology. The ruthenium‐based catalyst uses a nanostructured CeO2 support and Cs electronic promotion to remove hydrogen and ammonia inhibition, respectively, creating a catalyst with low‐temperature (<300 °C) activity that quickly approaches equilibrium. The absorbent uses MnCl2 to avoid the acid releasing decomposition of conventional absorbents like MgCl2, and a support of SiO2 to simultaneously enhance MnCl2 dispersion and improve stabilization. This integrated catalyst‐absorbent system reproducibly exceeds single‐pass ammonia synthesis equilibrium. Kinetic models of the catalyst and absorbent successfully predict the experimental long‐term behavior and facilitate the design of an integrated system. These results present a framework for aligning intermittent and isolated renewable energy with ammonia synthesis by decreasing capital complexity and increasing process agility—adapting to a shifting energy landscape to continue providing fertilizers with minimum CO2 penalty and pioneer energy storage.
Vanadium Dioxide Cathodes for High‐Rate Photo‐Rechargeable Zinc‐Ion Batteries
Authors: Deka Boruah Buddha , Mathieson Angus , Park Sul Ki , Zhang Xiao , Wen Bo , Tan Lifu , Boies Adam , De Volder Michael 
Published: March 2021

AbstractPhotovoltaics are an important source of renewable energy, but due to the intermittent nature of insolation, solar cells usually need to be connected to rechargeable batteries, electrochemical capacitors or other energy storage devices, which adds to the complexity and cost of these systems. In this work, a cathode design for photo‐rechargeable zinc‐ion batteries (photo‐ZIBs) is reported, that is inherently capable of harvesting sunlight to recharge without the need for external solar cells. The proposed photocathodes, comprising a composite of vanadium dioxide nanorods and reduced graphene oxide, are engineered to provide the necessary charge separation and storage for photocharging under illumination. The photo‐ZIBs achieve capacities of ≈282 mAh g−1 in the dark and ≈315 mAh g−1 under illumination, at 200 mA g−1, demonstrating the use of light not only to charge the devices, but additionally to enhance their capacity. The photo‐ZIBs also demonstrate enhanced high‐rate capabilities under illumination, as well as a capacity retention of ≈90% over 1000 cycles. The proposed photo‐ZIBs are considered a promising new technology for addressing energy poverty, due to their high performance and inherent cost‐efficiency and safety.
Cerebellofaciodental syndrome in an adult patient: Expanding the phenotypic and natural history characteristics
Authors: Honjo Rachel Sayuri , Castro Matheus Augusto Araújo , Ferraciolli Suely Fazio , Soares Junior Luiz Alberto Valente , Pastorino Antonio Carlos , Bertola Débora Romeo , Miyake Noriko , Matsumoto Naomichi , Kim Chong Ae 
Published: March 2021

AbstractCerebellofaciodental syndrome is characterized by facial dysmorphisms, intellectual disability, cerebellar hypoplasia, and dental anomalies. It is an autosomal‐recessive condition described in 2015 caused by pathogenic variants in BRF1. Here, we report a Brazilian patient who faced a diagnostic challenge beginning at 11 months of age. Fortunately, whole‐exome sequencing (WES) was performed, detecting the BRF1 variants NM_001519.3:c.1649delG:p.(Gly550Alafs*36) and c.421C>T:p.(Arg141Cys) in compound heterozygosity, thus finally achieving a diagnosis of cerebellofaciodental syndrome. The patient is currently 25 years old and is the oldest patient yet reported. The clinical report and a review of published cases are presented. Atlanto‐occipital fusion, a reduced foramen magnum and basilar invagination leading to compression of the medulla‐spinal cord transition are skeletal findings not reported in previous cases. The description of syndromes with dental findings shows that such anomalies can be an important clue to relevant differential diagnoses. The cooperation of groups from different international centers made possible the resolution of this and other cases and is one of the strategies to bring medical advances to developing countries, where many patients with rare diseases are difficult to diagnose definitively.
Unprecedented 2D Homochiral Hybrid Lead‐Iodide Perovskite Thermochromic Ferroelectrics with Ferroelastic Switching
Authors: Zeng Yu‐Ling , Huang Xue‐Qin , Huang Chao‐Ran , Zhang Hua , Wang Fang , Wang Zhong‐Xia 
Published: March 2021

AbstractChiral perovskites have emerged as a significant class of materials showing promising optoelectronic and spintronic applications. Reports of chiral perovskite ferroelectrics, however, have been scarce. In this work, we have successfully synthesized homochiral lead–iodide perovskite ferroelectrics [(R)‐N‐(1‐phenylethyl)ethane‐1,2‐diaminium]PbI4 and [(S)‐N‐(1‐phenylethyl)ethane‐1,2‐diaminium]PbI4 by introducing a methyl group into the organic cation of the parent (N‐benzylethane‐1,2‐diaminium)PbI4. Vibrational circular dichroism spectra identify the chiral mirroring relationship. They both undergo 222F2‐type paraelectric–ferroelectric behavior at around 378 K coupled with clear ferroelastic domain “ON/OFF” switching. Besides, they exhibit an evident thermochromism with color change from orange–yellow to orange–red. To our knowledge, the discovery of integrated ferroelectricity, ferroelasticity, and reversible thermochromism in chiral perovskites is unprecedented.
Recent Strategies for Carbon−Halogen Bond Formation Using Nickel
Authors: Marchese Austin D. , Adrianov Timur , Lautens Mark 
Published: March 2021

AbstractNickel catalysis has demonstrated the capability of performing a broad range of synthetically challenging transformations over the last decade. Though recent literature has focused on the formation of C−C and C−N bonds, a variety of breakthroughs in the field of C−X bond generation have also been reported. A diverse range of strategies using nickel have been developed, in an effort to expand the scope and synthetic utility of these halogenation methods. This Minireview will cover six emerging strategies in this field including: oxidatively induced C−X reductive elimination, triflate‐to‐halogen exchange reactions, directed C−H halogenation, non‐directed electrophilic C−H halogenation of arenes, enantioselective α‐fluorination of carbonyl containing compounds, and 1,2‐difunctionalization‐halogenation reactions. The final section has been split into two parts: nickel‐catalyzed hydrohalogenation and nickel‐catalyzed carbohalogenation reactions.
Anterior Cervical Discectomy and Fusion: A Surgical Intervention for Treating Cervical Disc Disease
Authors: Karasin Beth , Grzelak Monica 
Published: March 2021

ABSTRACTCervical disc disease includes chronic disc degeneration, stenosis, spondylosis, and disc herniation; providers initially treat these conditions conservatively through symptomatic care. When conservative measures fail, surgery may be indicated. It is important to explore all the surgical options available and the risks and benefits of each procedure. An anterior cervical discectomy and fusion (ACDF) is a procedure involving the removal of disc material to achieve neural tissue decompression and placement of a bone graft or interbody implant and a cervical plate and screws to stabilize the spinal column at one or more vertebral levels. This article briefly reviews the anatomy of the spine and treatment options for cervical disc disease; presents an in‐depth review of the ACDF procedure, including the expected perioperative course and care considerations; and concludes with a case report of a 37‐year‐old woman who underwent an ACDF at the C5‐C6 and C6‐C7 vertebral levels of the spine.
Crystallization, structure, and enhanced mechanical property of ethylene‐octene elastomer crosslinked with dicumyl peroxide
Authors: Wang Yuan‐Xia , Shi Ying , Wang Chen‐Chen , Cheng Jia‐Hui , Wang Ying , Shao Wen‐Jun , Liu Li‐Zhi 
Published: March 2021

AbstractCrosslinking of polyolefin elastomer (POE, ENGAGE™ 8480) with Dicumyl Peroxide (DCP) can have effects on its crystallization dynamics, crystal structure, and properties. The POE crosslinked uniformly has significantly lower crystalline ability than the one with only amorphous phase crosslinked, which, in turn, has weaker crystalline ability than neat POE. The crystallinity and melting point depend on how the POE is crosslinked. The neat POE and POE crosslinked in amorphous phase only, are investigated with DSC and in‐situ tensile/synchrotron radiation (WAXD/SAXS). In situ tensile/synchrotron X‐ray during a uniaxial stretching process indicates that severe crystal fragmentation is observed at a strain around 45%, and with further increase in strain. The stress in the crosslinked POE is significantly larger than neat POE. For both samples, crystal orientation increases sharply within the strain range up to 88% where orientation‐induced new crystals aligned in stretching direction are observed. The long period increases more in stretching direction for the crosslinked POE, consistent with larger stress in this sample, and the stress difference is more pronounced at large strains (27.3 vs. 10.9 MPa at a strain 435%). Permanent set of the crosslinked POE is smaller, consistent with less oriented crystals observed after the test for permanent set.
Upcycling of polypropylene with various concentrations of peroxydicarbonate and dilauroyl peroxide and two processing steps
Authors: Stanic Sascha , Koch Thomas , Schmid Klaus , Knaus Simone , Archodoulaki Vasiliki‐Maria 
Published: March 2021

AbstractThe influence of two peroxides (peroxydicarbonate/dilauroyl peroxide) with various concentrations (10–200 mmol/kg PP) and their effective opportunity to introduce long chain branched (LCB) were investigated. The dependence of a single and double extrusion step and the changes of the properties were studied. Experiments were carried out in a single screw extruder at 180°C for the first extrusion step (modification) and at 240°C for the second extrusion step (processing simulation). Melt flow rate and dynamic rheological properties were studied at a measuring temperature of 230°C. For the definitive determination of long chain branched polypropylene (LCB‐PP) served the extensional rheology measurements. The mechanical properties were examined via tensile test and impact tensile test. Summarized, LCB (melt strength) could be observed via extensional rheology for all modified specimens and the mechanical properties were maintained or even improved for the modified samples. Particularly, samples containing dilauroyl peroxide display excellent mechanical properties in this study.
Synthesis and antitumor potential of new arylidene ursolic acid derivatives via caspase‐8 activation
Authors: He Baoen , Zhu Zuchang , Chen Fenglian , Zhang Rong , Chen Weiqiang , Zhang Te , Wang Tao , Lei Jiamei 
Published: March 2021

AbstractContinuing our studies on NO‐donating ursolic acid–benzylidene derivatives as potential antitumor agents, we designed and synthesized a series of new arylidene derivatives containing NO‐donating ursolic acid and aromatic heterocyclic units. Compounds 5c and 6c showed a significant broad‐spectrum antitumor activity. Compound 5c exhibited nearly three‐ to nine‐fold higher cytotoxicity as compared with the parent drug in A549, MCF‐7, HepG‐2, HT‐29, and HeLa cells, and it was also found to be the most potent apoptosis inducer of MCF‐7 cells. More importantly, compound 5c arrested the MCF‐7 cell cycle in the G1 phase, which was associated with caspase activation and a decrease of the Bcl‐2/Bax ratio. Meanwhile, compound 5c caused changes in morphological features, dissipation of the mitochondrial membrane potential, and accumulation of reactive oxygen species. A docking study revealed that the nitroxyethyl moiety of compound 5c may form hydrogen bonds with caspase‐8 amino acid residues (SER256 and HIS255). Together, these data suggest that NO‐donating ursolic acid–arylidene derivatives are potent apoptosis inducers in tumor cells.
Effectiveness of Allopurinol in Reducing Mortality: Time‐Related Biases in Observational Studies
Authors: Suissa Samy , Suissa Karine , Hudson Marie 
Published: March 2021

ObjectiveThe treatment of gout with allopurinol is effective at reducing urate levels and the frequency of flares. Several observational studies have shown important reductions in mortality with allopurinol use, with wide variations in results. We undertook this review to assess the extent of bias in these studies, particularly time‐related biases such as immortal time bias.MethodsWe searched the literature to identify all observational studies describing the effect of allopurinol use versus nonuse on all‐cause mortality.ResultsWe identified 12 observational studies, of which 3 were affected by immortal time bias and 3 by immeasurable time bias, while the remaining 6 studies avoided these time‐related biases. Reductions in all‐cause mortality with allopurinol use were observed among the studies with immortal time bias, with a pooled hazard ratio (HR) of death associated with allopurinol of 0.71 (95% confidence interval [95% CI] 0.50–1.01), as well as in those with immeasurable time bias (pooled HR 0.62 [95% CI 0.56–0.67]). The 6 studies that avoided these biases demonstrated a null effect of allopurinol on mortality (pooled HR 0.99 [95% CI 0.87–1.11]), though the lack of an analysis based on treatment adherence may have attenuated the effect.ConclusionObservational studies are important to provide real‐world data on medication effects. The observational studies showing significantly decreased mortality with allopurinol treatment cannot be used as evidence, however, mainly due to time‐related biases that tend to greatly exaggerate the potential benefit of treatments. The ALL‐HEART randomized trial, which is currently underway and evaluates the effect of adding allopurinol to usual care (compared to no added treatment), will provide reliable evidence on mortality.
Observer‐based trajectory control for directional drilling process
Authors: Cai Zhen , Lai Xuzhi , Wu Min , Chen Luefeng , Lu Chengda 
Published: March 2021

AbstractThis paper is concerned with observer‐based trajectory control of directional drilling system with rotary steering devices. Since the trajectory orientation cannot be measured directly, most of the existing results implicitly assume that the trajectory orientation is equal to the measurement of orientation of the bottom hole assembly (BHA) or the drill bit, which would bring in certain control errors in practice. To avoid such control errors, in this paper, a trajectory control approach is established, which includes a state observer to estimate the trajectory orientation based on the measurement of the BHA orientation. Firstly, the relationship between the trajectory orientation and the BHA orientation is analyzed, and a trajectory evolution model is introduced according to the analysis. Secondly, based on this trajectory evolution model, a variable transformation technique is applied such that a trajectory tracking control problem is formulated. Thirdly, a feedback control strategy is devised based on the estimation of the trajectory orientation for trajectory tracking. Fourthly, stability analysis of the closed‐loop system is discussed, and the design of the controller and state observer is done. Finally, a typical case is used to illustrate the correctness and effectiveness of our approach.