bluuebunny/crossref_metadata_2025_split huggingface dataset:
Relationship between the prehospital quick Sequential Organ Failure Assessment and prognosis in patients with sepsis or suspected sepsis: a population‐based ORION registry
Authors: Hirose Tomoya , Katayama Yusuke , Ogura Hiroshi , Umemura Yutaka , Kitamura Tetsuhisa , Mizushima Yasuaki , Shimazu Takeshi 
Published: August 2021

AimThe quick Sequential Organ Failure Assessment (qSOFA) was proposed for use as a simple screening tool for sepsis. In this study, we evaluated the relationship between the prehospital use of qSOFA and prognosis in patients with sepsis or suspected sepsis using the population‐based Osaka Emergency Information Research Intelligent Operation Network (ORION) registry, which compiles prehospital ambulance data and in‐hospital information.MethodsThe study enrolled 437,974 patients in the ORION registry from January 1 to December 31, 2016. We selected hospitalized patients with sepsis or suspected sepsis using the appropriate codes from the International Classification of Diseases revision 10. We excluded patients with: (i) missing data (outcome, Japan Coma Scale, respiratory rate, and blood pressure); (ii) respiratory rate ≥60/min; and (iii) blood pressure ≥250 mmHg. These measures were evaluated by ambulance personnel when they first contacted the patient in the prehospital setting. The primary end‐point was discharge to death.ResultsIn total, 12,646 patients (median age, 78 [interquartile range, 65–85] years; male, n = 6,760 [53.5%]) were eligible for our analysis. In a multivariable logistic regression analysis adjusted for confounding factors, the proportion of patients discharged to death was significantly higher for those evaluated as qSOFA positive (≥2 points) than qSOFA negative (≤1 point) (265/2,250 [11.78%] vs. 415/10,396 [3.99%]; adjusted odds ratio 2.91; 95% confidence interval, 2.47–3.43; P < 0.0001). The specificity and sensitivity were 83.4% and 39.0%, respectively, and the area under the receiver operating characteristic curve for qSOFA positive was 0.61.ConclusionsThe qSOFA evaluated by ambulance personnel in the prehospital setting was significantly associated with prognosis in patients with sepsis or suspected sepsis.
Discrete Heteropolynuclear Yb/Er Assemblies: Switching on Molecular Upconversion Under Mild Conditions
Authors: Wang Jie , Jiang Yue , Liu Jiao‐Yang , Xu Hai‐Bing , Zhang Yue‐Xing , Peng Xu , Kurmoo Mohamedally , Ng Seik Weng , Zeng Ming‐Hua 
Published: August 2021

AbstractThe salts {[Ln2Ln*(Hhmq)3(OAc)3(hfac)2]+ [Ln*(hfac)3(OAc)(MeOH)]−} (Hhmq=2‐methanolquinolin‐8‐oxide, hfac=hexafluoroacetylacetonate; Ln, Ln*=Er, Gd, Yb) feature a discrete heteronuclear cation consisting of two types of lanthanide atoms. The quinolinoxy O‐atom serves as a μ2‐bridge to two Ln atoms and as a μ3‐bridge to all three atoms, with metal⋅⋅⋅metal distances being around 3.7 Å. For 1 ([Yb2Er]+), near‐infrared downshifted luminescence is switched to competitive upconversion luminescence upon irradiation by a 980 nm laser under an extremely low excitation power (0.288 W cm−2) through introduction of fluoride ions. The stability of 1 after addition of fluoride was confirmed by powder X‐ray diffraction and multistage mass spectrometry, associated with the 1H NMR of 6 ([La2Eu]+). More importantly, the at least 20‐fold enhancement of the quantum yield in non‐deuterated solvents at room temperature under low power densities (2 W cm−2) is the highest among the few molecular examples reported.
Palladium‐Catalyzed Cascade Carbonylation to α,β‐Unsaturated Piperidones via Selective Cleavage of Carbon–Carbon Triple Bonds
Authors: Ge Yao , Ye Fei , Yang Ji , Spannenberg Anke , Jiao Haijun , Jackstell Ralf , Beller Matthias 
Published: August 2021

AbstractA direct and selective synthesis of α,β‐unsaturated piperidones by a new palladium‐catalyzed cascade carbonylation is described. In the presented protocol, easily available propargylic alcohols react with aliphatic amines to provide a broad variety of interesting heterocycles. Key to the success of this transformation is a remarkable catalytic cleavage of the present carbon–carbon triple bond by using a specific catalyst with 2‐diphenylphosphinopyridine as ligand and appropriate reaction conditions. Mechanistic studies and control experiments revealed branched unsaturated acid 11 as crucial intermediate.
Introducing A New Class of Sulfonyl Fluoride Hubs via Radical Chloro‐Fluorosulfonylation of Alkynes
Authors: Nie Xingliang , Xu Tianxiao , Hong Yuhao , Zhang Honghai , Mao Chenxi , Liao Saihu 
Published: August 2021

AbstractSulfonyl fluorides have widespread applications in many important fields, including ligation chemistry, chemical biology, and drug discovery. Therefore, new methods to increase the synthetic efficiency and expand the available structures of sulfonyl fluorides are highly in demand. Here, we introduce a new and powerful class of sulfonyl fluoride hubs, β‐chloro alkenylsulfonyl fluorides (BCASF), which can be constructed via radical chloro‐fluorosulfonyl difunctionalization of alkynes under photoredox conditions. BCASF molecules exhibit versatile reactivities and well undergo a series of transformations at the chloride site while keeping the sulfonyl fluoride group intact, including reduction, Suzuki coupling, Sonogashira coupling, as well as nucleophilic substitution with various nitrogen, oxygen, and sulfur nucleophiles. By using BCASF as a synthetic hub, a wide range of sulfonyl fluorides becomes readily accessible, such as cis alkenylsulfonyl fluorides, dienylsulfonyl fluorides, and ynenylsulfonyl fluorides, which are challenging or even not possible to synthesize before with the known methods. Moreover, further application of BCASF to the late‐stage modification of peptides and drugs is also demonstrated.
An Open‐Shell Coronoid with Hybrid Chichibabin–Schlenk Conjugation
Authors: Prajapati Bibek , Dang Duy‐Khoi , Chmielewski Piotr J. , Majewski Marcin A. , Lis Tadeusz , Gómez‐García Carlos J. , Zimmerman Paul M. , Stępień Marcin 
Published: August 2021

AbstractA hexaradicaloid molecule with alternating Kekulé and non‐Kekulé connectivities between adjacent spin centers was obtained by fusing two conjugation motifs in Chichibabin and Schlenk hydrocarbons into a coronoid structure. 1H NMR, ESR, and SQUID experiments and computational analyses show that the system has a singlet ground state with a significant hexaradicaloid character (γ0=0.826, γ1=γ2=0.773). It has multiple thermally accessible high‐spin states (up to the septet), with uniform energy gaps of ca 1.0 kcal mol−1 between consecutive multiplicities. In line with its open‐shell character, the coronoid has a small electronic band gap (ca. 0.8 eV) and undergoes two consecutive one‐electron oxidations at low potentials, yielding cationic forms with extended near‐infrared absorption. The hexaradicaloid, which combines open‐shell and macrocyclic contributions to its π conjugation, is an example of a design strategy for multistate spin switches and redox‐amphoteric NIR dyes.
Designing Anion‐Type Water‐Free Zn2+ Solvation Structure for Robust Zn Metal Anode
Authors: Zhang Qiu , Ma Yilin , Lu Yong , Zhou Xunzhu , Lin Liu , Li Lin , Yan Zhenhua , Zhao Qing , Zhang Kai , Chen Jun 
Published: August 2021

AbstractRechargeable aqueous Zn batteries are potential for large‐scale electrochemical energy storage due to their low cost and high security. However, Zn metal anode suffers from the dendritic growth and interfacial hydrogen evolution reaction (HER), resulting in the deterioration of electrode/battery performance. Here we propose that both dendrites and HER are related to the water participated Zn2+ solvation structure‐Zn(H2O)62+ and thus can be resolved by transforming Zn(H2O)62+ to an anion‐type water‐free solvation structure‐ZnCl42−, which is achieved in traditional ZnSO4 aqueous electrolyte after adding chloride salt with a bulky cation (1‐ethyl‐3‐methylimidazolium chloride). The elimination of cation‐water interaction suppresses HER, while the electrostatic repulsion between Zn tips and the anion solvation structure inhibits dendrite formation. As a result, the electrolyte shows uniform Zn deposition with an average Zn plating/stripping Coulombic efficiency of ≈99.9 %, enabling a capacity retention of 78.8 % after 300 cycles in anode‐free Zn batteries with pre‐zincificated polyaniline as the cathode. This work provides a novel electrolyte design strategy to prevent HER and realize long‐lifespan metal anode.
A Selection of Macrocyclic Peptides That Bind STING From an mRNA‐Display Library With Split Degenerate Codons
Authors: Lin Chi‐Wang , Harner Mary J. , Douglas Andrew E. , Lafont Virginie , Yu Fei , Lee Ving G. , Poss Michael A. , Swain Joanna F. , Wright Martin , Lipovšek Daša 
Published: August 2021

AbstractRecent improvements in mRNA display have enabled the selection of peptides that incorporate non‐natural amino acids, thus expanding the chemical diversity of macrocycles beyond what is accessible in nature. Such libraries have incorporated non‐natural amino acids at the expense of natural amino acids by reassigning their codons. Here we report an alternative approach to expanded amino‐acid diversity that preserves all 19 natural amino acids (no methionine) and adds 6 non‐natural amino acids, resulting in the highest sequence complexity reported to date. We have applied mRNA display to this 25‐letter library to select functional macrocycles that bind human STING, a protein involved in immunoregulation. The resulting STING‐binding peptides include a 9‐mer macrocycle with a dissociation constant (KD) of 3.4 nM, which blocks binding of cGAMP to STING and induces STING dimerization. This approach is generalizable to expanding the amino‐acid alphabet in a library beyond 25 building blocks.
A Family of Heterobimetallic Cubes Shows Spin‐Crossover Behaviour Near Room Temperature
Authors: Hardy Matthias , Tessarolo Jacopo , Holstein Julian J. , Struch Niklas , Wagner Norbert , Weisbarth Ralf , Engeser Marianne , Beck Johannes , Horiuchi Shinnosuke , Clever Guido H. , Lützen Arne 
Published: August 2021

AbstractUsing 4‐(4′‐pyridyl)aniline as a simple organic building block in combination with three different aldehyde components together with metal(II) salts gave three different Fe8Pt6‐cubes and their corresponding Zn8Pt6 analogues by employing the subcomponent self‐assembly approach. Whereas the use of zinc(II) salts gave rise to diamagnetic cages, iron(II) salts yielded metallosupramolecular cages that show spin‐crossover behaviour in solution. The spin‐transition temperature T1/2 depends on the incorporated aldehyde component, giving a construction kit for the deliberate synthesis of spin‐crossover compounds with tailored transition properties. Incorporation of 4‐thiazolecarbaldehyde or N‐methyl‐2‐imidazole‐carbaldehyde yielded cages that undergo spin‐crossover around room temperature whereas the cage obtained using 1H‐4‐imidazolecarbaldehyde shows a spin‐transition at low temperatures. Three new structures were characterized by synchrotron X‐ray diffraction and all structures were characterized by mass spectrometry, NMR and UV/Vis spectroscopy.
Phase‐Dependent Electrocatalytic CO2 Reduction on Pd3Bi Nanocrystals
Authors: Jia Lin , Sun Mingzi , Xu Jie , Zhao Xuan , Zhou Rui , Pan Binbin , Wang Lu , Han Na , Huang Bolong , Li Yanguang 
Published: August 2021

AbstractAlloying is a general strategy for modulating the electronic structures of catalyst materials. Compared to more common solid–solution alloys, intermetallic alloys feature well‐defined atomic arrangements and provide the unique platform for studying the structure‐performance correlations. It is, unfortunately, synthetically challenging to prepare the nanostructures of intermetallic alloys for catalysis research. In this contribution, we prepare intermetallic Pd3Bi nanocrystals of a uniform size via a facile solvothermal method. These nanocrystals can phase‐transform into solid solution alloy via thermal annealing while retaining a similar composition and size. In 0.1 M KHCO3 aqueous solution, the intermetallic Pd3Bi can selectively reduce CO2 to formate with high selectivity (≈100 %) and stability even at <‐0.35 V versus reversible hydrogen electrode, whereas the solid solution alloy has limited formate selectivity of <60 %. Such unique phase‐dependence is understood via theoretical simulations showing that the crystallographic ordering of Pd and Bi atoms within intermetallic alloys can suppress CO poisoning and enhance the *OCHO adsorption during electrochemical CO2 reduction to formate.
Ball‐Milling Induced Debonding of Surface Atoms from Metal Bulk for Construing High‐Performance Dual‐Site Single‐Atom Catalysts
Authors: Wang Huilin , Wang Xiao , Pan Jing , Zhang Lingling , Zhao Meng , Xu Jing , Liu Bo , Shi Weidong , Song Shuyan , Zhang Hongjie 
Published: August 2021

AbstractOne of the most pressing challenges in single‐atom catalysis is the manipulation of the coordination environment of central metals to maximize the catalyst performance. Herein, we fabricated a high‐performance catalyst (Co‐SNC) by introducing S into the neighboring position of the Co‐N4 coordination. The developed ball‐milling method enabled large‐scale synthesis, that over 4.7 g of Co‐SNC can be produced in one pot. In benzylamine coupling reaction, Co‐SNC exhibited the highest conversion of 97.5 % with 99 % selectivity toward N‐benzylidenebenzylamine in 10 h among various Co catalysts. Density functional theory calculations revealed the crucial role of S atoms, which serve as the active sites for O2 activation, leaving the Co atoms free to adsorb benzylamine. Consequently, the adsorption energies of O2 and benzylamine were significantly increased. Our strategy suggests a feasible approach to enhance catalytic performance by delicately integrating dual active sites into a single catalyst unit.
The First High‐Pressure Chromium Oxonitridoborate CrB4O6N—an Unexpected Link to Nitridosilicate Chemistry
Authors: Fuchs Birgit , Johrendt Dirk , Bayarjargal Lkhamsuren , Huppertz Hubert 
Published: August 2021

AbstractCrB4O6N crystallizes in the non‐centrosymmetric space group P63mc (no. 186) with the lattice parameters a=5.1036(1), c=8.3519(3) Å, and a volume of 188.40(1) Å3. It was synthesized in a high‐pressure/high‐temperature experiment at 7 GPa and 1673 K and represents the first high‐pressure oxonitridoborate. It is built up of starlike‐shaped entities of four BO3N tetrahedra, connected via one common nitrogen atom that resembles the fourfold‐coordinated nitrogen atoms in the homeotypic nitridosilicates MYbSi4N7 (M=Sr, Ba). Building up a network with channels that contain the Cr3+ ions, CrB4O6N contains for the first time a tetrahedral building unit in contrast to trigonal planar B(O/N)3 entities in all other known oxonitridoborates. The structural relations as well as the results of spectroscopic measurements and calculations on the chromium oxonitridoborate are discussed.
Fabrication of Integrated Copper‐Based Nanoparticles/Amorphous Metal–Organic Framework by a Facile Spray‐Drying Method: Highly Enhanced CO2 Hydrogenation Activity for Methanol Synthesis
Authors: Mitsuka Yuko , Ogiwara Naoki , Mukoyoshi Megumi , Kitagawa Hiroshi , Yamamoto Tomokazu , Toriyama Takaaki , Matsumura Syo , Haneda Masaaki , Kawaguchi Shogo , Kubota Yoshiki , Kobayashi Hirokazu 
Published: August 2021

AbstractWe report on Cu/amUiO‐66, a composite made of Cu nanoparticles (NPs) and amorphous [Zr6O4(OH)4(BDC)6] (amUiO‐66, BDC=1,4‐benzenedicarboxylate), and Cu‐ZnO/amUiO‐66 made of Cu‐ZnO nanocomposites and amUiO‐66. Both structures were obtained via a spray‐drying method and characterized using high‐resolution transmission electron microscopy, energy dispersive spectra, powder X‐ray diffraction and extended X‐ray absorption fine structure. The catalytic activity of Cu/amUiO‐66 for CO2 hydrogenation to methanol was 3‐fold that of Cu/crystalline UiO‐66. Moreover, Cu‐ZnO/amUiO‐66 enhanced the methanol production rate by 1.5‐fold compared with Cu/amUiO‐66 and 2.5‐fold compared with γ‐Al2O3‐supported Cu‐ZnO nanocomposites (Cu‐ZnO/γ‐Al2O3) as the representative hydrogenation catalyst. The high catalytic performance was investigated using in situ Fourier transform IR spectra. This is a first report of a catalyst comprising metal NPs and an amorphous metal–organic framework in a gas‐phase reaction.
Tuning the piezoresistive strain‐sensing behavior of poly(vinylidene fluoride)–CNT composites: The role of polymer–CNT interface and composite processing technique
Authors: Kumar G. Sudheer , Patro T. Umasankar 
Published: August 2021

AbstractIn order to understand the role of polymer–carbon nanotube (CNT) interface and composite processing method on strain‐sensing properties, poly(vinylidene fluoride) (PVDF)‐CNT composites have been prepared by melt‐mixing and solution‐casting methods using pristine and acid‐treated CNTs with CNT content of 0.15–4 wt%. The strain rate applied was in the order of s−1. Besides the improved mechanical properties of the composites over pristine PVDF, the piezoresistivity was also profoundly affected by the gentle acid‐treatment of CNTs and the composite processing method leading to tunable strain‐sensing properties. The stability of the strain‐sensors has been further predicted by employing cyclic piezoresistive tests. Interestingly, the pristine CNT composites showed higher strain‐sensitivity likely due to weak interface with polymer and higher initial resistance than the acid‐treated counterparts; while the acid‐treated CNT composites showed better retention of sensing properties under repeated cycles. On the other hand, composites with larger CNT length showed higher strain‐sensitivity than that having shorter CNTs. The temperature dependence of strain‐sensitivity showed a transition from positive to negative temperature coefficient at ~90°C. Finally, the composites subjected to a large number of bending cycles showed excellent performance and stability of strain‐sensing properties, paving the way for development of robust strain‐sensors for structural health monitoring.
Tablet‐assisted objective structured spotter practical examination (TOSSPE): Advantages of an innovative anatomy spotter examination method for medical student assessment
Authors: Polak Katarzyna , Gielecki Jerzy Stanisław , Żurada Anna 
Published: August 2021

AbstractThe affordances of technology‐based assessments, like the objectively structured practical examination, have become an integral part of gross anatomy courses. The Department of Anatomy Faculty of Medicine at the University of Warmia and Mazury developed and introduced an application for tablet devices which has been implemented in student examinations and assessments, called the tablet‐assisted objective structured spotter practical examination. It was created to simplify the educational process and to build a rich learning environment, facilitating deep learning for students through examination and feedback data. The method consists of cadaver stations with traditional corresponding pin spotters in an expanded tablet application. It not only provides instant feedback on various observations of teaching–learning skills but has also positively affected the entire process of education. The method provides an unbiased evaluation of knowledge and understanding of the anatomy course, ensuring objectivity and standardization. The current study was performed on a total of 608 first‐year medical students in Polish and English divisions and focused on the observed advantages since the new method was introduced. Outcomes indicate that after the implementation of the method for both the Polish and English divisions' first‐year medical students, the mean score of examinations significantly increased compared to other teaching–learning methods. The study highlights that students were excited about the implementation of the new method and identified its many benefits. It is recognized that technological development and the digital environment offer a range of opportunities and added value versus traditional assessment activities, methods, and processes.
Utilizing SARS‐CoV‐2 to teach PCR and gel electrophoresis in a pair of asynchronous distant learning laboratory exercises
Authors: Cummings Cristina M. 
Published: August 2021

AbstractAmidst the COVID‐19 pandemic, many colleges shifted to online learning, creating a need for teaching materials that could be deployed in the online setting. A pair of virtual laboratory exercises with a COVID‐19 theme were created for first year Biology majors to introduce students to the topics of polymerase chain reaction and gel electrophoresis. The exercises were effective in promoting student learning of both topics in an online asynchronous setting, and could easily be adapted for use in other courses or in a synchronous online setting.
Biopsy of cervical lymph node does not impact the survival of nasopharyngeal carcinoma
Authors: Yang Shi‐Ping , Li Ji‐Fang , Zhou Ping , Lian Chen‐Lu , Chen Dan‐Xia , Li Zhao‐Jun , Wu San‐Gang 
Published: August 2021

AbstractPurposeThe optimal practice regarding cervical lymph node biopsy (CLNB) remains to be defined to provide the best clinical management in nasopharyngeal carcinoma (NPC). This study aimed to investigate the effect of CLNB on the survival of NPC patients.MethodsPatients diagnosed with NPC from 2004 to 2015 were identified using the Surveillance, Epidemiology, and End Results database. Multivariate logistic regression, Kaplan–Meier method, Cox proportional hazards regression analysis, and propensity score matching (PSM) were used to determine the factors associated with CLNB and prognostic effect of CLNB of NPC.ResultsWe included 1903 patients in this study. There were 321 (16.9%) and 1582 (83.1%) patients with and without CLNB, respectively. The percentage of CLNB was 19.4% in 2004 and was decreased to 8.6% in 2015 (p = 0.044). Patients diagnosed in later years (p = 0.008), older age (p < 0.001), Chinese (p = 0.002), advanced tumor stage (p < 0.001), and early nodal stage (p = 0.003) were less likely to receive additional CLNB. In patients who received additional CLNB, the 5‐years NPC‐specific survival (NPCSS) was 83.6%, which was similar to patients without CLNB (80.1%, p = 0.159). In addition, a similar 5‐years NPCSS was found between those receiving biopsy or aspiration of regional lymph node and those receiving lymph node resection (p = 0.584). There were 187 pairs of patients who were completely matched using PSM, the multivariate prognostic analyses indicated that the receipt of CLNB was not associated with an inferior outcome in the PSM cohort (p = 0.349). Similar results were found after stratification by the year of diagnosis, race/ethnicity, and histology.ConclusionAdditional CLNB is not associated with an inferior survival outcome in NPC. Our study provides a reference for the clinical practice of NPC.