bluuebunny/crossref_metadata_2025_split huggingface dataset:
Room‐Temperature Triple‐Ligand Surface Engineering Synergistically Boosts Ink Stability, Recombination Dynamics, and Charge Injection toward EQE‐11.6% Perovskite QLEDs
Authors: Song Jizhong , Li Jinhang , Xu Leimeng , Li Jianhai , Zhang Fengjuan , Han Boning , Shan Qingsong , Zeng Haibo 
Published: June 2018

AbstractDeveloping low‐cost and high‐quality quantum dots (QDs) or nanocrystals (NCs) and their corresponding efficient light‐emitting diodes (LEDs) is crucial for the next‐generation ultra‐high‐definition flexible displays. Here, there is a report on a room‐temperature triple‐ligand surface engineering strategy to play the synergistic role of short ligands of tetraoctylammonium bromide (TOAB), didodecyldimethylammonium bromide (DDAB), and octanoic acid (OTAc) toward “ideal” perovskite QDs with a high photoluminescence quantum yield (PLQY) of >90%, unity radiative decay in its intrinsic channel, stable ink characteristics, and effective charge injection and transportation in QD films, resulting in the highly efficient QD‐based LEDs (QLEDs). Furthermore, the QD films with less nonradiative recombination centers exhibit improved PL properties with a PLQY of 61% through dopant engineering in A‐site. The robustness of such properties is demonstrated by the fabrication of green electroluminescent LEDs based on CsPbBr3 QDs with the peak external quantum efficiency (EQE) of 11.6%, and the corresponding peak internal quantum efficiency (IQE) and power efficiency are 52.2% and 44.65 lm W−1, respectively, which are the most‐efficient perovskite QLEDs with colloidal CsPbBr3 QDs as emitters up to now. These results demonstrate that the as‐obtained QD inks have a wide range application in future high‐definition QD displays and high‐quality lightings.
Quantitative Prediction of Yield in Transglycosylation Reaction Catalyzed by Nucleoside Phosphorylases
Authors: Alexeev Cyril S. , Kulikova Irina V. , Gavryushov Sergei , Tararov Vitali I. , Mikhailov Sergey N. 
Published: June 2018

AbstractPhosphorolytic transglycosylation catalyzed by nucleoside phosphorylases is an important biotechnological process. The reaction is reversible, and the yield of the target nucleoside depends on its concentration at the equilibrium state. We have shown that initial concentrations of the starting compounds and the phosphorolysis equilibrium constants of starting and final glycosides determine concentrations of all the components at the equilibrium state. Based on that, we developed a novel quantitative approach for the prediction of yields in transglycosylation reactions. This method simplifies the choice of reagent concentrations and their ratios for the maximization of the target nucleoside yield. It is advantageous over widely applied blind and cumbersome trial‐and‐error approach and can reduce the required chemical and energy resources. The described algorithm could also be applied for other equilibrium transfer reactions.magnified image
Regioselective [3+3] Cyclization of 2‐Indolymethanols with Vinylcyclopropanes via Metal Catalysis
Authors: Zhu Zi‐Qi , Yu Lei , Sun Meng , Mei Guang‐Jian , Shi Feng 
Published: June 2018

AbstractThe first [3+3] cyclization of 2‐indolylmethanols with vinylcyclopropanes has been established under iridium catalysis. The reaction regioselectively constructs tetrahydrocarbazole frameworks bearing two vicinal all‐carbon quaternary stereocenters in high yields (up to 99%, up to 20:1 rr). This reaction not only is the first example of a metal‐catalyzed [3+3] cyclization of 2‐indolylmethanols but also is the first one‐step [3+3] cyclization of vinylcyclopropanes. More importantly, this reaction shows reversed regioselectivity compared to other 2‐indolylmethanol‐involved transformations, which will advance the chemistry of 2‐indolylmethanols.magnified image
Drug‐Bearing Supramolecular MMP Inhibitor Nanofibers for Inhibition of Metastasis and Growth of Liver Cancer
Authors: Ji Yujie , Xiao Yanyu , Xu Liu , He Jiayu , Qian Chen , Li Weidong , Wu Li , Chen Rui , Wang Jingjing , Hu Rongfeng , Zhang Xudong , Gu Zhen , Chen Zhipeng 
Published: June 2018

AbstractTreatment of hepatocellular carcinoma (HCC) requires sustained suppression of tumor cell growth and metastasis for long‐term efficacy. However, traditional intratumoral drug delivery system always exhibits burst release with less therapeutic outcomes. Here, a new self‐assembling amphiphilic peptide drug conjugate (SAAPDC) is fabricated as a “two‐in‐one” nanofiber system comprising a hexapeptide as a matrix metalloproteinases (MMP) inhibitor and doxorubicin (DOX) for the treatment of HCC. The results indicate that doxorubicin‐conjugated peptide (DOX‐KGFRWR) self‐assembles to form long nanofibers showing sustained release property for inhibiting the enzymatic activities of MMP‐2 and MMP‐9. This nanofiber not only inhibits tumor growth in situ but also effectively prevents pulmonary metastasis in an SMMC7721 cell line–based mouse model. In summary, this hexapeptide‐based supermolecule system represents a promising nanoscale platform to sustain drug release with high loading capacity for intratumoral administration. Moreover, the delivery of chemotherapeutic drugs via drug‐bearing supramolecular MMP inhibitor nanofibers simultaneously inhibits metastasis and tumor growth to achieve synergistic effects for metastatic HCC therapy.
Chinese expert consensus on the diagnosis and treatment of hypertension in the elderly (2017)
Authors: Liu Meilin ,   Committee of cardio‐cerebro‐vascular Disease of China Association of Gerontology and Geriatrics, Chinese College of Cardiovascular Physician of Chinese Medical Doctor Association
Published: June 2018

AbstractChina has stepped into an aging society. The social service development statistical bulletin 2015 published in July 2016 by Ministry of Civil Affairs showed that till the end of 2015, the amount of people ≥60 years of age had already approached to 222 million, which comprised 16.1% of the Chinese population, while the amount of people ≥65 years of age comprised 10.5% of the Chinese population was 143 million.1 Hypertension is an independent risk factor for cardio‐cerebral‐vascular diseases and is a primary and contributory cause for death and disability in the elderly. A large number of epidemiological and clinical studies have shown that the risk of target organ damage of hypertension such as ischemic heart disease, cardiac insufficiency, stroke, chronic kidney disease, and aortic and peripheral artery diseases significantly increases with aging. Blood pressure control plays a significant role in reducing cardio‐cerebral‐vascular events and all‐cause mortality.2 Compared to younger patients with similar blood pressure elevation, the risks of cardiovascular and cerebrovascular events significantly increase in the elderly. Because of specialties in the pathogenesis and clinical manifestation in older patients with hypertension, physicians should pay more attention to the population characteristics and individual treatments.
Identification of the pyranonigrin A biosynthetic gene cluster by genome mining in Penicillium thymicola IBT 5891
Authors: Tang Man‐Cheng , Zou Yi , Yee Danielle , Tang Yi 
Published: June 2018

SignificanceA polyketide synthase and nonribosomal peptide synthetase hybrid gene cluster from the genome of Penicillium thymicola was identified through genome mining. Heterologous expression of this cluster leads to the production of pyranonigrin A. A series of experiments established that only four genes are sufficient to biosynthesize pyranonigrin A. Based on the results from the current study, a biosynthetic pathway of pyranonigrin A is proposed. © 2018 American Institute of Chemical Engineers AIChE J, 64: 4182–4186, 2018
Role of sublingual immunotherapy in the treatment of asthma: An updated systematic review
Authors: Lin Sandra Y. , Azar Antoine , Suarez‐Cuervo Catalina , Diette Gregory B. , Brigham Emily , Rice Jessica , Ramanathan Murugappan , Robinson Karen A. 
Published: June 2018

BackgroundThe purpose of the systematic review is to evaluate the efficacy and safety of sublingual immunotherapy (SLIT) for the treatment of allergic asthma.MethodsPubMed, Embase, and CENTRAL databases were searched, updating an earlier review (January 1, 2005 through May 8, 2017). Randomized, controlled studies (RCTs) were included, which reported one of the prespecified outcomes: asthma symptoms measured by control composite scores; quality of life; medication use; pulmonary physiology; and health‐care utilization. For safety outcomes, RCTs and observational studies were included. Two independent reviewers extracted data, assessed risk of bias, and graded strength of evidence (SOE) for each outcome.ResultsFourteen RCTs (n = 2585) assessed the efficacy of SLIT for asthma. The RCTs utilized house dust mite (HDM), birch, or grass allergen. SLIT improved asthma symptoms (high SOE), decreased use of long‐term control medication, and improved forced expiratory volume in 1 second (FEV1) (moderate SOE). SLIT may decrease quick‐relief medication use, and improve disease‐specific quality of life (low SOE). For safety, 20 RCTs and 10 observational studies (n = 3621) were identified. Local (risk differences ranged from −0.03 to +0.765) and systemic allergic reactions (risk differences ranged from −0.03 to +0.06) were a common occurrence in SLIT and control groups. Life‐threatening reactions were uncommon, with 3 cases of anaphylaxis and no deaths reported.ConclusionThere is moderate‐to‐high strength evidence that SLIT improves allergic asthma symptoms, reduces long‐term control medication use, and improves FEV1 based on studies of HDM, birch, and grass. SLIT rarely is associated with life‐threatening adverse events.
Stabilization of Aliphatic Phosphines by Auxiliary Phosphine Sulfides Offers Zeptomolar Affinity and Unprecedented Selectivity for Probing Biological CuI
Authors: Morgan M. Thomas , Yang Bo , Harankhedkar Shefali , Nabatilan Arielle , Bourassa Daisy , McCallum Adam M. , Sun Fangxu , Wu Ronghu , Forest Craig R. , Fahrni Christoph J. 
Published: June 2018

AbstractFull elucidation of the functions and homeostatic pathways of biological copper requires tools that can selectively recognize and manipulate this trace nutrient within living cells and tissues, where it exists primarily as CuI. Buffered at attomolar concentrations, intracellular CuI is, however, not readily accessible to commonly employed amine and thioether‐based chelators. Herein, we reveal a chelator design strategy in which phosphine sulfides aid in CuI coordination while simultaneously stabilizing aliphatic phosphine donors, producing a charge‐neutral ligand with low‐zeptomolar dissociation constant and 1017‐fold selectivity for CuI over ZnII, FeII, and MnII. As illustrated by reversing ATP7A trafficking in cells and blocking long‐term potentiation of neurons in mouse hippocampal brain tissue, the ligand is capable of intercepting copper‐dependent processes. The phosphine sulfide‐stabilized phosphine (PSP) design approach, which confers resistance towards protonation, dioxygen, and disulfides, could be readily expanded towards ligands and probes with tailored properties for exploring CuI in a broad range of biological systems.
Engineering the Coordination Environment of Single‐Atom Platinum Anchored on Graphdiyne for Optimizing Electrocatalytic Hydrogen Evolution
Authors: Yin Xue‐Peng , Wang Hong‐Juan , Tang Shang‐Feng , Lu Xiu‐Li , Shu Miao , Si Rui , Lu Tong‐Bu 
Published: June 2018

AbstractTwo Pt single‐atom catalysts (SACs) of Pt‐GDY1 and Pt‐GDY2 were prepared on graphdiyne (GDY)supports. The isolated Pt atoms are dispersed on GDY through the coordination interactions between Pt atoms and alkynyl C atoms in GDY, with the formation of five‐coordinated C1‐Pt‐Cl4 species in Pt‐GDY1 and four‐coordinated C2‐Pt‐Cl2 species in Pt‐GDY2. Pt‐GDY2 shows exceptionally high catalytic activity for the hydrogen evolution reaction (HER), with a mass activity up to 3.3 and 26.9 times more active than Pt‐GDY1 and the state‐of‐the‐art commercial Pt/C catalysts, respectively. Pt‐GDY2 possesses higher total unoccupied density of states of Pt 5d orbital and close to zero value of Gibbs free energy of the hydrogen adsorption (|Δ
|) at the Pt active sites, which are responsible for its excellent catalytic performance. This work can help better understand the structure–catalytic activity relationship in Pt SACs.
Docking Strategy To Construct Thermostable, Single‐Crystalline, Hydrogen‐Bonded Organic Framework with High Surface Area
Authors: Hisaki Ichiro , Suzuki Yuto , Gomez Eduardo , Cohen Boiko , Tohnai Norimitsu , Douhal Abderrazzak 
Published: June 2018

AbstractEnhancing thermal and chemical durability and increasing surface area are two main directions for the construction and improvement of the performance of porous hydrogen‐bonded organic frameworks (HOFs). Herein, a hexaazatriphenylene (HAT) derivative that possesses six carboxyaryl groups serves as a suitable building block for the systematic construction of thermally and chemically durable HOFs with high surface area through shape‐fitted docking between the HAT cores and interpenetrated three‐dimensional network. A HAT derivative with carboxybiphenyl groups forms a stable single‐crystalline porous HOF that displays protic solvent durability, even in concentrated HCl, heat resistance up to 305 °C, and a high Brunauer–Emmett–Teller surface area [SA(BET)] of 1288 m2 g−1. A single crystal of this HOF displays anisotropic fluorescence, which suggests that it would be applicable to polarized emitters based on robust functional porous materials.
Reactions of Group 4 Metallocene Bis(trimethylsilyl)acetylene Complexes with Nitriles and Isonitriles
Authors: Rosenthal Uwe 
Published: June 2018

AbstractThis Review summarizes reactions of Group 4 metallocene bis(trimethylsilyl)acetylene complexes with nitriles and isonitriles. Selected examples of reactions of Group 4 metallocene alkyne complexes of the type Cp′2M(η2‐Me3SiC2SiMe3) with different nitriles and isonitriles are described following the general L‐M‐S principle, in which stoichiometric and catalytic reactions are influenced by ligands L, metals M, and substrate substituents S. The influence of all these parameters is highlighted. The basic reactions with nitriles and in some cases with isonitriles were investigated in detail and are summarized. Selected further reactions of the products again depend on L, M, and S. Most interesting feature for this is the formation of mono‐ and polynuclear 1‐metalla‐2,5‐diazacyclopenta‐2,4‐dienes, which show great potential for the synthesis of complex heterocycles.
The Electric Field as a “Smart” Ligand in Controlling the Thermal Activation of Methane and Molecular Hydrogen
Authors: Yue Lei , Wang Na , Zhou Shaodong , Sun Xiaoyan , Schlangen Maria , Schwarz Helmut 
Published: June 2018

AbstractWhile pristine [TaO2]+ is rather inert in its thermal reactions with both methane and molecular hydrogen, the cluster oxide becomes reactive upon ligation with the closed‐shell ligand CO2. While the presence of CO2 increases the intrinsic barriers of the C−H and H−H bond activation steps, the efficiency of the overall reaction to generate the insertion product [Ta(R)(OH)O]+ (R=CH3, H) is greatly enhanced by the superb leaving‐group properties of CO2. The ligand effect of CO2 has been well mimicked by the electric field of a negative point charge, and mechanistic aspects are addressed by high‐level quantum chemical calculations
NHC‐Pd complex based on 1,3‐bis (4‐ethoxycarbonylphenyl) imidazolium chloride: synthesis, structure and catalytic activity in the synthesis of axially chiral benzophenone hydrazone
Authors: Duan Wenzeng , Sun Zhaofeng , Huo Yanmin , Liu Yanke , Wu Guangqing , Wang Ruifeng , Wu Shuang , Yao Qingxia , Gong Shuwen 
Published: June 2018

A novel NHC–Pd complex of 1,3‐bis (4‐ethoxycarbonylphenyl) imidazolium chloride has been synthesized and characterized by 1H NMR, 13C NMR, IR and X‐ray single‐crystal diffraction studies. TG analysis shows that the NHC‐Pd complex is stable under 208 °C. The catalytic activities have been explored for the synthesis of axially chiral N‐(2′‐methoxy‐1,1′‐binaphthalen‐2‐yl) benzophenone hydrazone. The result indicates that the novel NHC‐Pd complex can achieve better catalytic activity than the Pd‐phosphine catalysts in the synthesis of axially chiral N‐(2′‐methoxy‐1,1′‐binaphthalen‐2‐yl) benzophenone hydrazone.
Synthesis, cytotoxic characterization, and SAR study of imidazo[1,2‐b]pyrazole‐7‐carboxamides
Authors: Demjén András , Alföldi Róbert , Angyal Anikó , Gyuris Márió , Hackler László , Szebeni Gábor J. , Wölfling János , Puskás László G. , Kanizsai Iván 
Published: June 2018

AbstractThe synthesis and in vitro cytotoxic characteristics of new imidazo[1,2‐b]pyrazole‐7‐carboxamides were investigated. Following a hit‐to‐lead optimization exploiting 2D and 3D cultures of MCF‐7 human breast, 4T1 mammary gland, and HL‐60 human promyelocytic leukemia cancer cell lines, a 67‐membered library was constructed and the structure–activity relationship (SAR) was determined. Seven synthesized analogues exhibited sub‐micromolar activities, from which compound 63 exerted the most significant potency with a remarkable HL‐60 sensitivity (IC50 = 0.183 μM).
Controllable Synthesis of a Highly Ordered Polymeric Structure Assembled from Cobalt‐Cluster‐based Racemic Supramolecules
Authors: Mai Hien Duy , Lee Inme , Yoo Hyojong 
Published: June 2018

AbstractMetallosupramolecule‐based polymeric platforms with high degrees of hierarchy and tailorable functionalities are of great interests because of their unique morphologies and potential applications. Herein, the controllable synthesis of a highly‐ordered polymeric structure, {[M,P‐Co8(PDA)6(HIP)3(DMF)5(H2O)]3‐[Co(DMF)(H2O)2]} (1) (PDA=2,6‐pyridinedicarboxylate, HIP=5‐hydroxyisophthalate, DMF=dimethylformamide) with unique topology is reported. The solid‐state structure of 1 reveals that it is alternately and periodically assembled from racemic supramolecular monomers to form a zigzag‐shaped polymeric strand. Discrete racemic supramolecules (2) with topologies similar to those of monomeric species of 1 are also controllably synthesized in a separate reaction. Formation of intermolecular hydrogen bonds between supramolecules associated with hydroxyl groups of HIPs are critical for the unique solid‐state packing geometries of 1 and 2.
Rare compound heterozygous mutations in gene MSH6 cause constitutive mismatch repair deficiency syndrome
Authors: Ling Chao , Yang Wei , Sun Hailang , Ge Ming , Ji Yuanqi , Han Shirui , Zhang Di , Zhang Xue 
Published: June 2018

Key Clinical MessageFew studies reported patients who harbored three kinds of primary tumors simultaneously. Here, we present a 9‐year‐old boy with colon carcinoma, brain medulloblastoma, and lymphoma. Genetic mutation detection was explored with next‐generation sequencing, and compound heterozygous mutations in gene MSH6 c.3103C>T p.Arg1035Ter and c.3261dupC p.Phe1088LeufsTer were discovered.
Latent and Air‐Stable Pre‐Catalysts for the Polymerization of Dicyclopentadiene: From Penta‐ to Hexacoordination in Molybdenum Imido Alkylidene N‐Heterocyclic Carbene Complexes
Authors: Elser Iris , Kordes Benjamin R. , Frey Wolfgang , Herz Katharina , Schowner Roman , Stöhr Laura , Altmann Hagen J. , Buchmeiser Michael R. 
Published: June 2018

AbstractThe pentacoordinated, 16‐valence electron (VE) Mo imido alkylidene N‐heterocyclic carbene (NHC) complexes I1–I5 and the hexacoordinated 18‐VE Mo imido alkylidene NHC complexes 1–4, 8, 10 and 12 containing a chelating ligand have been prepared and used as thermally latent catalysts in the ring‐opening metathesis polymerization (ROMP) of dicyclopentadiene (DCPD). Both 10 and 12 are the first Mo imido alkylidene complexes with a chelating alkylidene featuring a carboxylate group. Complexes I1–I3 and I5 as well as 1–4 proved to be fully thermally latent in the presence of DCPD. With the changes in both the electronic and steric situation at the imido ligand provided by these pre‐catalysts, different temperatures of the onset of polymerization (Tonset=65–140 °C) and for the exothermic maximum of the curing curve (Texo,max=98–183 °C) of DCPD were achieved. Also, the degree of crosslinking was successfully varied as indicated by swelling experiments in toluene, which revealed degrees of swelling between 0 and 50 %. While the introduction of a chelating alkylidene increases Tonset, the introduction of more electron‐donating anionic ligands (tert‐butoxide, phenoxide) resulted in a drastic reduction in Tonset, underlining the high flexibility of these systems. The hexacoordinated high‐oxidation state molybdenum imido alkylidene NHC complexes 2, 3 and 4 were stable under air for at least twelve hours in the solid state.
Enantiopure versus Racemic Mixture in Reversible, Two‐Step, Single‐Crystal‐to‐Single‐Crystal Transformations of Copper(II) Complexes
Authors: Ene Cristian D. , Maxim Catalin , Rouzières Mathieu , Clérac Rodolphe , Avarvari Narcis , Andruh Marius 
Published: June 2018

AbstractInvited for the cover of this issue is the group of Catalin Maxim and Marius Andruh at the University of Bucharest. The image depicts la coupe du roi, a popular demonstration of chirality through the cutting of apples. Read the full text of the article at 10.1002/chem.201800404.
Utilization of deep‐sea microbial esterase PHE21 to generate chiral sec‐butyl acetate through kinetic resolutions
Authors: Wang Yilong , Xu Yongkai , Zhang Yun , Sun Aijun , Hu Yunfeng 
Published: June 2018

AbstractWe previously identified and characterized 1 novel deep‐sea microbial esterase PHE21 and used PHE21 as a green biocatalyst to generate chiral ethyl (S)‐3‐hydroxybutyrate, 1 key chiral chemical, with high enantiomeric excess and yield through kinetic resolution. Herein, we further explored the potential of esterase PHE21 in the enantioselective preparation of secondary butanol, which was hard to be resolved by lipases/esterases. Despite the fact that chiral secondary butanols and their ester derivatives were hard to prepare, esterase PHE21 was used as a green biocatalyst in the generation of (S)‐sec‐butyl acetate through hydrolytic reactions and the enantiomeric excess, and the conversion of (S)‐sec‐butyl acetate reached 98% and 52%, respectively, after process optimization. Esterase PHE21 was also used to generate (R)‐sec‐butyl acetate through asymmetric transesterification reactions, and the enantiomeric excess and conversion of (R)‐sec‐butyl acetate reached 64% and 43%, respectively, after process optimization. Deep‐sea microbial esterase PHE21 was characterized to be a useful biocatalyst in the kinetic resolution of secondary butanol and other valuable chiral secondary alcohols.
Direct Synthesis of Structurally Divergent Indole Alkaloids from Simple Chemicals
Authors: Shen Tao , Zhu Bencong , Lin Fengguirong , Pan Jun , Wei Jialiang , Luo Xiao , Liu Jianzhong , Jiao Ning 
Published: June 2018

AbstractA direct and structurally divergent synthesis of indole alkaloids from very simple 2‐vinylanilines, alkynes and TBN via a novel substrate fragmentation/cycloaddition strategy has been developed, which provides an efficient noble‐metal‐free approach to access a library of highly valuable indole derivatives of tryptamines and tryptamine‐related oximes, lactams, and lactones, as well as β‐carbolines, spiroindolines, and hexa‐hydropyrrolo[2,3‐b]indoles.