bluuebunny/crossref_metadata_2025_split huggingface dataset:
Dissolving Vanadium into Titanium Nitride Lattice Framework for Rational Polysulfide Regulation in Li–S Batteries
Authors: Shang Chaoqun , Li Gaoran , Wei Benben , Wang Jiayi , Gao Rui , Tian Yuan , Chen Qing , Zhang Yongguang , Shui Lingling , Zhou Guofu , Hu Yongfeng , Chen Zhongwei , Wang Xin 
Published: December 2020

AbstractRational regulation of host–guest interactive chemistry is of great significance but has not yet effectively been applied in lithium–sulfur (Li–S) batteries. Herein, a unique titanium vanadium nitride (TVN) solid solution fabric is developed as an ideal platform for fine structure modulation towards efficient and durable sulfur electrochemistry. The dissolution of V into the TiN lattice framework is shown to subtly tailor the coordinative and electronic structures of Ti and V, tuning their respective chemical affinity to sulfur species. Consequently, the optimized Ti–V interplay renders the highest overall polysulfide adsorpabiltiy, and contributes to strong sulfur immobilization and fast reaction kinetics. The resultant Li–S cells realize an outstanding cyclability with high capacity retention of 97.7% after 400 cycles. Moreover, reversible areal capacity over 6.11 mAh cm−2 can be sustained under a high sulfur loading of 6.0 mg cm−2 and a limited electrolyte concentration of 6.5 mL g−1. This work provides a novel strategic perspective for the rational regulation of fine structure towards superior Li–S batteries and beyond.
Autonomous Strategies for Improved Performance and Reliability of Li‐Ion Batteries
Authors: Zhao Lihong , Sottos Nancy R. 
Published: December 2020

AbstractThe battery community has devoted significant effort to improve the performance and reliability of Li‐ion batteries through the development of new materials. The integration of autonomous function provides an alternative strategy to further extend performance. Autonomous material systems mimic the ability of biological systems to self‐protect, sense, regulate, and heal in response to damage and other environmental changes. When incorporated in batteries, these materials enable autonomic restoration of battery performance upon degradation, as well as autonomic shutdown or extinguishment in response to thermal runaway. Successful strategies for improving Li‐ion battery performance include controlled release of microencapsulated functional additives and the integration of self‐healing or adaptive interlayers and binders. These methods have been effective for stabilizing the solid electrolyte interface, preventing battery fires, restoring electrode conductivity, and suppressing Li dendrite growth. Challenges and opportunities exist in the further application of autonomous strategies in the battery environment. A greater variety of encapsulated additives with precise triggered‐release are needed to address specific battery degradation mechanisms. Incorporation of self‐healing polymers in solid‐state batteries facilitates improvement in interfacial and mechanical stability. The integration of autonomous strategies with battery management systems potentially enables enhanced control over multiple battery cycling parameters.
Traffic form and season of wear affect responses of fine fescues
Authors: Chen Hui , Park Bradley S. , Murphy James A. 
Published: December 2020

AbstractThe performance of fine fescue (Festuca spp.) species and cultivars may differ by traffic form or the season of wear simulation. Two trials were initiated in 2012 to evaluate the effect of traffic form (abrasive wear vs. cleated traffic) and season of wear (spring, summer, or autumn) on 10 fine fescues seeded in North Brunswick, NJ. Plots were visually assessed for the fullness of turfgrass canopy (FTC) and leaf bruising. Verdure and soil physical properties were assessed after the last assessment period in the traffic form trial. Abrasive wear constantly reduced the FTC (14–30%) of fine fescues compare to the non‐trafficked control, while the FTC of plots with cleated traffic was similar to the non‐trafficked control towards the end of the study. Although both traffic forms caused soil compaction, cleated traffic resulted in a more compacted soil. Abrasive wear improved selection efficiency for fine fescues compared to cleated traffic. The FTC response of fine fescues cultivars interacted with the season of wear; thus, screening for fine fescues with improved ability to withstand abrasive wear might be more effective and accurate during spring to avoid high disease pressure and other confounding stresses during summer. ‘Blueray’ and ‘Beacon’ hard fescue, ‘Quatro’ sheep fescue, and ‘Radar’ Chewings were more traffic tolerant than other fine fescue cultivars under low disease pressure. The propensity of fine fescues to bruising under wear needs to be assessed in both summer and autumn.
Prognostic impact of LY6K and CDCA1 expression for patients with esophageal squamous cell carcinoma
Authors: Oguma Junya , Ozawa Soji , Sakakibara Terue , Kajiwara Hiroshi , Nakamura Naoya , Makuuchi Hiroyasu 
Published: December 2020

AbstractAimIn the present study, we investigated the relationship between the expressions of two cancer testis antigens (CTA), LY6K (lymphocyte antigen 6 complex locus K) and CDCA1 (cell division cycle associated 1), in esophageal squamous cell carcinoma (ESCC) tumors and the long‐term outcomes of patients with ESCC to clarify the clinical significance of LY6K and CDCA1 expression in ESCC tumors.MethodsA total of 175 patients with thoracic ESCC who had undergone a thoracic esophagectomy with three‐field lymphadenectomy without neoadjuvant therapy were retrospectively reviewed in this study. LY6K and CDCA1 expressions were evaluated in tumor tissues using immunohistochemical (IH) staining.ResultsMedian patient age was 63 years; 159 patients (90.9%) were men. Ninety‐four patients (55.3%) were LY6K‐positive, and 85 patients (48.6%) were CDCA1‐positive. The LY6K‐positive group had a significantly worse overall survival (OS) than the LY6K‐negative group (P = 0.012), and the CDCA1‐positive group had a significantly worse OS than the CDCA1‐negative group (P = 0.010). A multivariate analysis suggested that pathological N stage, venous invasion, LK6Y‐positive and CDCA1‐positive were independent prognostic factors. The patients were classified into four groups according to the staining pattern combinations of the two CTA. The LY6K‐positive and CDCA1‐positive group was found to have a significantly poorer outcome than the other groups.ConclusionESCC patients with a combination of LY6K and CDCA1 expression in their tumor tissues had a worse prognosis than all the other ESCC patients and it was an independent factor associated with prognosis for patients with ESCC.
Partially Coherent Dual Nonparaxial Accelerating Beams
Authors: Zeng Zishuai , Zhao Daomu 
Published: December 2020

AbstractPartially coherent dual nonparaxial accelerating beams are constructed from the perspective of a superposition of fully coherent modes and incoherent interference effects among these modes. It is found that divergence angle and partial coherence of such beams can be altered by a curvature parameter. At the beginning of the propagation, such beams focus in the case of constructive interference, but they leave a central dip in the destructive case. Additionally, the extension of a crossed‐shaped intensity distribution caused by interference is slower than that of the transverse beam frame evidently. In particular, moving along the nonparaxial accelerating trajectory on the micrometer scale, the main lobes of these beams can diverge to a nearly flat angle. As such, these beams are likely to have applications in microscopic particle manipulation and coherence image processing.
Glycoengineering of NK Cells with Glycan Ligands of CD22 and Selectins for B‐Cell Lymphoma Therapy
Authors: Hong Senlian , Yu Chenhua , Wang Peng , Shi Yujie , Cao Weiqian , Cheng Bo , Chapla Digantkumar G. , Ma Yuanhui , Li Jie , Rodrigues Emily , Narimatsu Yoshiki , Yates John R. , Chen Xing , Clausen Henrik , Moremen Kelly W. , Macauley Matthew Scott , Paulson James C. , Wu Peng 
Published: December 2020

AbstractCD22, a member of Siglec family of sialic acid binding proteins, has restricted expression on B cells. Antibody‐based agents targeting CD22 or CD20 on B lymphoma and leukemia cells exhibit clinical efficacy for treating these malignancies, but also attack normal B cells leading to immune deficiency. Here, we report a chemoenzymatic glycocalyx editing strategy to introduce high‐affinity and specific CD22 ligands onto NK‐92MI and cytokine‐induced natural killer cells to achieve tumor‐specific CD22 targeting. These CD22‐ligand modified cells exhibited significantly enhanced tumor cell binding and killing in vitro without harming healthy B cells. For effective lymphoma cell killing in vivo, we further functionalized CD22 ligand‐modified NK‐92MI cells with the E‐selectin ligand sialyl Lewis X to promote trafficking to bone marrow. The dual‐functionalized cells resulted in the efficient suppression of B lymphoma in a xenograft model. Our results suggest that natural killer cells modified with glycan ligands to CD22 and selectins promote both targeted killing of B lymphoma cells and improved trafficking to sites where the cancer cells reside, respectively.
Rechargeable Aqueous Aluminum Organic Batteries
Authors: Chen Jiangchun , Zhu Qiaonan , Jiang Li , Liu Rongyang , Yang Yan , Tang Mengyao , Wang Jiawei , Wang Hua , Guo Lin 
Published: December 2020

AbstractAqueous aluminum‐ion batteries (AABs) are regarded as promising next‐generation energy storage devices, and the current reported cathodes for AABs mainly focused on inorganic materials which usually implement a typical Al3+ ions (de)insertion mechanism. However, the strong electrostatic forces between Al3+ and the host materials usually lead to sluggish kinetics, poor reversibility and inferior cycling stability. Herein, we employ an organic compound with redox‐active moieties, phenazine (PZ), as the cathode material in AABs. Different from conventional inorganic materials confined by limited lattice spacing and rigid structure, the flexible organic molecules allow a large‐size Al‐complex co‐intercalation through reversible redox active centers (‐C=N‐) of PZ. This co‐intercalation behavior can effectively reduce desolvation penalty, and substantially lower the Coulombic repulsion during the ion (de)insertion process. Consequently, this organic cathode exhibits a high capacity and excellent cyclability, which exceeds those of most reported electrode materials for AABs. This work highlights the anion co‐intercalation chemistry of redox‐active organic materials, which is expected to boost the development of high‐performance multivalent‐ion battery systems.
Carboranealkynyl‐Protected Gold Nanoclusters: Size Conversion and UV/Vis–NIR Optical Properties
Authors: Wang Jie , Wang Zhao‐Yang , Li Shi‐Jun , Zang Shuang‐Quan , Mak Thomas C. W. 
Published: December 2020

AbstractStructure evolution has become an effective way to assemble novel monolayer‐protected metal nanomolecules. However, evolution with alkynyl‐stabilized metal clusters still remains rarely explored. Herein, we present a carboranealkynyl‐protected gold nanocluster [Au28(C4B10H11)12(tht)8]3+ (Au28, tht=tetrahydrothiophene) possessing an open‐shell electronic structure with 13 free electrons, which was isolated by a facile self‐reduction method with 9‐HC≡C‐closo‐1,2‐C2B10H11 as the two‐in‐one reducing and protecting agent. Notably, Au28 undergoes a complete transformation in methanol into a stable and smaller‐sized nanocluster [Au23(C4B10H11)9(tht)6]2+ (Au23) bearing 12 valence electrons and crystal‐field‐like split superatomic 1D orbitals. The transformation process was systematically monitored with ESI‐MS and UV/Vis absorption spectra. Au28 and Au23 both display optical absorption covering the UV/Vis–NIR range and NIR emission, which facilitates their potential application in the biomedical and photocatalytic fields.
Non‐Carbohydrate Glycomimetics as Inhibitors of Calcium(II)‐Binding Lectins
Authors: Kuhaudomlarp Sakonwan , Siebs Eike , Shanina Elena , Topin Jérémie , Joachim Ines , da Silva Figueiredo Celestino Gomes Priscila , Varrot Annabelle , Rognan Didier , Rademacher Christoph , Imberty Anne , Titz Alexander 
Published: December 2020

AbstractBecause of the antimicrobial resistance crisis, lectins are considered novel drug targets. Pseudomonas aeruginosa utilizes LecA and LecB in the infection process. Inhibition of both lectins with carbohydrate‐derived molecules can reduce biofilm formation to restore antimicrobial susceptibility. Here, we focused on non‐carbohydrate inhibitors for LecA to explore new avenues for lectin inhibition. From a screening cascade we obtained one experimentally confirmed hit, a catechol, belonging to the well‐known PAINS compounds. Rigorous analyses validated electron‐deficient catechols as millimolar LecA inhibitors. The first co‐crystal structure of a non‐carbohydrate inhibitor in complex with a bacterial lectin clearly demonstrates the catechol mimicking the binding of natural glycosides with LecA. Importantly, catechol 3 is the first non‐carbohydrate lectin ligand that binds bacterial and mammalian calcium(II)‐binding lectins, giving rise to this fundamentally new class of glycomimetics.
To Every Rule There is an Exception: A Rational Extension of Loewenstein's Rule
Authors: Fant Magnus , Ångqvist Mattias , Hellman Anders , Erhart Paul 
Published: December 2020

AbstractLoewenstein's rule, which states that Al−O−Al motifs are energetically unstable, is fundamental to the understanding and design of zeolites. Here, using a combination of electronic structure calculations and lattice models, we show under which circumstances this rule becomes invalid and how it can be rationally extended using the chabasite framework for demonstration.
One‐Step Sixfold Cyanation of Benzothiadiazole Acceptor Units for Air‐Stable High‐Performance n‐Type Organic Field‐Effect Transistors
Authors: Kafourou Panagiota , Park Byoungwook , Luke Joel , Tan Luxi , Panidi Julianna , Glöcklhofer Florian , Kim Jehan , Anthopoulos Thomas D. , Kim Ji‐Seon , Lee Kwanghee , Kwon Sooncheol , Heeney Martin 
Published: December 2020

AbstractReported here is a new high electron affinity acceptor end group for organic semiconductors, 2,1,3‐benzothiadiazole‐4,5,6‐tricarbonitrile (TCNBT). An n‐type organic semiconductor with an indacenodithiophene (IDT) core and TCNBT end groups was synthesized by a sixfold nucleophilic substitution with cyanide on a fluorinated precursor, itself prepared by a direct arylation approach. This one‐step chemical modification significantly impacted the molecular properties: the fluorinated precursor, TFBT IDT, a poor ambipolar semiconductor, was converted into TCNBT IDT, a good n‐type semiconductor. The electron‐deficient end group TCNBT dramatically decreased the energy of the highest occupied and lowest unoccupied molecular orbitals (HOMO/LUMO) compared to the fluorinated analogue and improved the molecular orientation when utilized in n‐type organic field‐effect transistors (OFETs). Solution‐processed OFETs based on TCNBT IDT exhibited a charge‐carrier mobility of up to μe≈0.15 cm2 V−1 s−1 with excellent ambient stability for 100 hours, highlighting the benefits of the cyanated end group and the synthetic approach.
Dimerization of Linear Butenes and Pentenes in an Acidic Zeolite (H‐MFI)
Authors: Berger Fabian , Sauer Joachim 
Published: December 2020

AbstractQuantum chemical evidence is produced to show that dimerization of linear butenes and pentenes at zeolitic Brønsted sites in H‐MFI yields alkanes featuring cyclohexane rings rather than branched alkenes. The absence of any C=C double bond in the formed cyclic alkane explains the observations that oligomerization stops at the dimer. The calculated reaction enthalpies for the dimerization of 2‐pentene in the gas phase are −84 kJ mol−1 for branched alkenes, but −153 and −154 kJ mol−1 for alkyl‐cyclopentane and ‐hexane, respectively. Together with calculated adsorption enthalpies of the dimers, −111 and −127 kJ mol−1, respectively, this implies surface dimer formation enthalpies of −264 and −281 kJ mol−1, respectively, in close agreement with the experimental value of −285 kJ mol−1. In contrast, the predicted enthalpy for formation of branched alkoxides, −198 kJ mol−1, deviates by 87 kJ mol−1 from experiment. Calculated IR spectra for the Brønsted OH group show the observed conversion of the band at approximately 3000 cm−1 (hydrogen bond with alkene) to a less intense band at approximately 3450–3500 cm−1 (interaction with alkane).
Topological‐Distortion‐Driven Amorphous Spherical Metal‐Organic Frameworks for High‐Quality Single‐Mode Microlasers
Authors: Gao Zhenhua , Xu Baoyuan , Fan Yuqing , Zhang Tongjin , Chen Shunwei , Yang Shuo , Zhang Weiguang , Sun Xun , Wei Yanhui , Wang Zifei , Wang Xue , Meng Xiangeng , Zhao Yong Sheng 
Published: December 2020

AbstractMetal‐organic frameworks (MOFs) have recently emerged as appealing platforms to construct microlasers owing to their compelling characters combining the excellent stability of inorganic materials and processable characters of organic materials. However, MOF microstructures developed thus far are generally composed of multiple edge boundaries due to their crystalline nature, which consequently raises significant scattering losses that are detrimental to lasing performance. In this work, we propose a strategy to overcome the above drawback by designing spherically shaped MOFs microcavities. Such spherical MOF microstructures are constructed by amorphizing MOFs with a topological distortion network through introducing flexible building blocks into the growth environment. With an ultra‐smooth surface and excellent circular boundaries, the acquired spherical microcavities possess a Q factor as high as ≈104 and can provide sufficient feedback for high‐quality single‐mode lasing oscillations. We hope that these results will pave an avenue for the construction of new types of flexible MOF‐based photonic components.
Atomically Dispersed Reactive Centers for Electrocatalytic CO2 Reduction and Water Splitting
Authors: Zhang Huabin , Cheng Weiren , Luan Deyan , Lou Xiong Wen (David) 
Published: December 2020

AbstractDeveloping electrocatalytic energy conversion technologies for replacing the traditional energy source is highly expected to resolve the fossil fuel exhaustion and related environmental problems. Exploring stable and high‐efficiency electrocatalysts is of vital importance for the promotion of these technologies. Single‐atom catalysts (SACs), with atomically distributed active sites on supports, perform as emerging materials in catalysis and present promising prospects for a wide range of applications. The rationally designed near‐range coordination environment, long‐range electronic interaction and microenvironment of the coordination sphere cast huge influence on the reaction mechanism and related catalytic performance of SACs. In the current Review, some recent developments of atomically dispersed reactive centers for electrocatalytic CO2 reduction and water splitting are well summarized. The catalytic mechanism and the underlying structure–activity relationship are elaborated based on the recent progresses of various operando investigations. Finally, by highlighting the challenges and prospects for the development of single‐atom catalysis, we hope to shed some light on the future research of SACs for the electrocatalytic energy conversion.
Diols Activation by Cu/Borinic Acids Synergistic Catalysis in Atroposelective Ring‐Opening of Cyclic Diaryliodoniums
Authors: Zhao Kun , Yang Shan , Gong Qi , Duan Longhui , Gu Zhenhua 
Published: December 2020

AbstractA Cu‐catalyzed enantioselective ring‐opening alkoxygenation reaction of cyclic diaryliodonium salts and diols in the presence of borinic acids was reported. Tuning structure of borinic acids with six or five‐membered ring skeleton could selectively activate 1,2‐diols or 1,4‐diols. A catalytic cycle through a key ion pair model that accounts for the observed enantioselectivity was proposed.
Electrocatalytic Iodine Reduction Reaction Enabled by Aqueous Zinc‐Iodine Battery with Improved Power and Energy Densities
Authors: Ma Longtao , Ying Yiran , Chen Shengmei , Huang Zhaodong , Li Xinliang , Huang Haitao , Zhi Chunyi 
Published: December 2020

AbstractProposed are Prussian blue analogue hosts with ordered and continuous channels, and electrocatalytic functionality with open Co and Fe species, which facilitate maximum I2 utilization efficiency and direct I2 to I− conversion kinetics of the I2 reduction reaction, and free up 1/3 I− from I3−. Co[Co1/4Fe3/4(CN)6] exhibits a low energy barrier (0.47 kJ mol−1) and low Tafel slope (76.74 mV dec−1). Accordingly, the Co[Co1/4Fe3/4(CN)6]/I2//Zn battery delivers a capacity of 236.8 mAh g−1 at 0.1 A g−1 and a rate performance with 151.4 mAh g−1 achieved even at 20 A g−1. The battery delivers both high energy density and high‐power density of 305.5 Wh kg−1 and 109.1 kW kg−1, higher than I2//Zn batteries reported to date. Furthermore, solid‐state flexible batteries were constructed. A 100 mAh high capacity solid‐state I2//Zn battery is demonstrated with excellent cycling performance of 81.2 % capacity retained after 400 cycles.
Probing Transient DNA Conformation Changes with an Intercalative Fluorescent Excimer
Authors: Chen Bin , Huang Qiuling , Qu Zhibei , Li Cong , Li Qian , Shi Jiye , Fan Chunhai , Wang Lihua , Zuo Xiaolei , Shen Jianlei , Li Jiang 
Published: December 2020

AbstractVariation of DNA conformation is important in regulating gene expression and mediating drug‐DNA interactions. However, directly probing transient DNA conformation changes is challenging owing to the dynamic nature of this process. We show a label‐free fluorescence method to monitor transient DNA conformation changes in DNA structures with various lengths and shapes using a DNA intercalator, K21. K21 can form transient excimers on the surface of DNA; the ratiometric emission of monomer and excimer correlate to DNA transient conformation stability in numerous DNA structures, including i‐motifs, G‐quadruplex structures, and single nucleotide mutation at random position. We analyzed the conformation dynamics of a single plasmid before and after enzyme digestion with confocal fluorescence microscopy. This method provides a label‐free fluorescence strategy to probe transient conformation changes of DNA structures and has potential in uncovering transient genomic processes in living cells.
Das riechende Prinzip des Vetiveröls, aufgeklärt durch chemische Synthese
Authors: Ouyang Jie , Bae Hanyong , Jordi Samuel , Dao Quang Minh , Dossenbach Sandro , Dehn Stefanie , Lingnau Julia B. , Kanta De Chandra , Kraft Philip , List Benjamin 
Published: December 2020

AbstractVetiveröl wird im Multitonnen‐Maßstab aus den Wurzeln des Vetivergrases gewonnen und ist einer der begehrtesten Duftbausteine der modernen Parfümerie. Das exquisite ätherische Öl, das sich in über einem Drittel aller Parfüms findet, ist eine komplexe Mischung aus Hunderten von unterschiedlichen Verbindungen, wobei das riechende Prinzip, das für den charakteristischen sanften und süßen, transparenten, holzig‐ambrierten Geruchscharakter verantwortlich ist, bis heute Rätsel aufgibt. Durch eine elfstufige chemische Synthese mit einer neuartigen asymmetrischen organokatalytischen Mukaiyama‐Michael‐Addition im Zentrum beweisen wir hier, dass (+)‐2‐epi‐Ziza‐6(13)en‐3‐on das riechende Prinzip des Vetiveröls ist. Seine olfaktorische Charakterisierung ergab einen außergewöhnlich tiefen Schwellenwert von 29 Pikogramm pro Liter Luft, der für die sinnliche Aura und die quasi‐pheromonartige Anziehung, die es auf Parfümeure wie Verbraucher gleichermaßen ausübt, verantwortlich ist.