bluuebunny/crossref_metadata_2025_split huggingface dataset:
Hydrocortisone with fludrocortisone for septic shock: a systematic review and meta‐analysis
Authors: Yamamoto Ryo , Nahara Isao , Toyosaki Mitsunobu , Fukuda Tatsuma , Masuda Yoshiki , Fujishima Seitaro 
Published: September 2020

AimCombined hydrocortisone and fludrocortisone therapy for septic shock has not been evaluated with an independent systematic review. We aimed to elucidate the beneficial effects of a dual corticosteroid treatment regime involving both hydrocortisone and fludrocortisone for adult patients with septic shock on mortality.MethodsWe searched the Medline, Cochrane CENTRAL, and ICHUSHI databases for reports published before April 2019. We included randomized controlled trials that compared the use of both hydrocortisone and fludrocortisone with either corticosteroid‐free or hydrocortisone‐only treatments on adult patients with septic shock. Three researchers independently reviewed the studies. The meta‐analyses were undertaken to assess primary outcome (28‐day mortality) and secondary outcomes (in‐hospital mortality, long‐term mortality, shock reversal, and adverse events).ResultsAmong the four studies eligible for data synthesis, we included 2,050 patients from three studies for quantitative synthesis. All studies used similar regimens (hydrocortisone and fludrocortisone for 7 days without tapering). The 28‐day mortality rate was reduced after dual corticosteroid treatment (risk ratio, 0.88; 95% confidence intervals [CI], 0.78–0.99). The heterogeneity between the studies was low (I2 = 0%). Patients who underwent dual corticosteroid treatment had lower long‐term mortality rates (risk ratio, 0.90; 95% CI, 0.83–0.98) and higher rate of shock reversal after 28 days (odds ratio, 1.06; 95% CI, 1.01–1.12) than control patients. Adverse events (except for hyperglycemia) were similar among the treatment groups.ConclusionsThe available evidence suggests that a combination of fludrocortisone and hydrocortisone is more effective than adjunctive therapy and could be recommended for septic shock.
Unravelling Structural Dynamics within a Photoswitchable Single Peptide: A Step Towards Multimodal Bioinspired Nanodevices
Authors: Chen Xinjiani , Yeoh Yuan Qi , He Yanbin , Zhou Chenguang , Horsley John R. , Abell Andrew D. , Yu Jingxian , Guo Xuefeng 
Published: September 2020

AbstractThe majority of the protein structures have been elucidated under equilibrium conditions. The aim herein is to provide a better understanding of the dynamic behavior inherent to proteins by fabricating a label‐free nanodevice comprising a single‐peptide junction to measure real‐time conductance, from which their structural dynamic behavior can be inferred. This device contains an azobenzene photoswitch for interconversion between a well‐defined cis, and disordered trans isomer. Real‐time conductance measurements revealed three distinct states for each isomer, with molecular dynamics simulations showing each state corresponds to a specific range of hydrogen bond lengths within the cis isomer, and specific dihedral angles in the trans isomer. These insights into the structural dynamic behavior of peptides may rationally extend to proteins. Also demonstrated is the capacity to modulate conductance which advances the design and development of bioinspired electronic nanodevices.
Photo‐Effect on Ion Transport in Mixed Cation and Halide Perovskites and Implications for Photo‐Demixing**
Authors: Kim Gee Yeong , Senocrate Alessandro , Wang Ya‐Ru , Moia Davide , Maier Joachim 
Published: September 2020

AbstractLead halide perovskites are considered to be most promising photovoltaic materials. Highest efficiency and improved stability of perovskite solar cells have been achieved by using cation and anion mixtures. Experimental information on electronic and ionic charge carriers is key to evaluate device performance, as well as processes of photo‐decomposition and photo‐demixing which are observed in these materials. Here, we measure ionic and electronic transport properties and investigate various cation and anion substitutions with a special eye on their photo‐ionic effect, following our previous study on CH3NH3PbI3, where we found that light enhances not only electronic but also ionic conductivities. We find that this phenomenon is very sensitive to the nature of the halide, while the cationic substitutions are less relevant. Based on the observation that the ionic conductivity enhancement found for iodide perovskites is significantly weakened by bromide substitution, we provide a chemical rationale for the photo‐demixing in mixed halide compositions.
Dendritic Mesoporous Silica Nanoparticle Adjuvants Modified with Binuclear Aluminum Complex: Coordination Chemistry Dictates Adjuvanticity
Authors: Yang Yang , Tang Jie , Song Hao , Yang Yannan , Gu Zhengying , Fu Jianye , Liu Yang , Zhang Min , Qiao Zhen‐An , Yu Chengzhong 
Published: September 2020

AbstractAluminum‐containing adjuvants used in vaccine formulations suffer from low cellular immunity, severe aggregation, and accumulation in the brain. Conventional aluminosilicates widely used in the chemical industry focus mainly on acidic sites for catalytic applications, but they are rarely used as adjuvants. Reported here is an innovative “ligand‐assisted steric hindrance” strategy to create a high density of six‐coordinate VIAl−OH groups with basicity on dendritic mesoporous silica nanoparticles as new nanoadjuvants. Compared to four‐coordinate IVAl‐modified counterparts, VIAl−OH‐rich aluminosilicate nanoadjuvants enhance cellular delivery of antigens and provoke stronger cellular immunity. Moreover, the aluminum accumulation in the brain is more reduced than that with a commercial adjuvant. These results show that coordination chemistry can be used to control the adjuvanticity, providing new understanding in the development of next‐generation vaccine adjuvants.
A Paclitaxel Prodrug Activatable by Irradiation in a Hypoxic Microenvironment
Authors: Zhou Shiyu , Hu Xiuli , Xia Rui , Liu Shi , Pei Qing , Chen Guang , Xie Zhigang , Jing Xiabin 
Published: September 2020

AbstractThe innate hypoxic microenvironment of most solid tumors has a major influence on tumor growth, invasiveness, and distant metastasis. Here, a hypoxia‐activated self‐immolative prodrug of paclitaxel (PTX2‐Azo) was synthesized and encapsulated by a peptide copolymer decorated with the photosensitizer chlorin e6 (Ce6) to prepare light‐boosted PTX nanoparticle (Ce6/PTX2‐Azo NP). In this nanoparticle, PTX2‐Azo prevents premature drug leakage and realizes specific release in hypoxic tumor microenvironment and the photosensitizer Ce6 not only efficiently generates singlet oxygen under light irradiation but also acts as a positive amplifier to promote the release of PTX. The combination of photodynamic therapy (PDT) and chemotherapy results in excellent antitumor efficacy, demonstrating the great potential for synergistic cancer therapy.
Intramolecular Coupling of Terminal Alkynes by Atom Manipulation
Authors: Albrecht Florian , Rey Dulce , Fatayer Shadi , Schulz Fabian , Pérez Dolores , Peña Diego , Gross Leo 
Published: September 2020

AbstractGlaser‐like coupling of terminal alkynes by thermal activation is extensively used in on‐surface chemistry. Here we demonstrate an intramolecular version of this reaction performed by atom manipulation. We used voltage pulses from the tip to trigger a Glaser‐like coupling between terminal alkyne carbons within a custom‐synthesized precursor molecule adsorbed on bilayer NaCl on Cu(111). Different conformations of the precursor molecule and the product were characterized by molecular structure elucidation with atomic force microscopy and orbital density mapping with scanning tunneling microscopy, accompanied by density functional theory calculations. We revealed partially dehydrogenated intermediates, providing insight into the reaction pathway.
Collective Total Synthesis of Aspidofractinine Alkaloids through the Development of a Bischler–Napieralski/Semipinacol Rearrangement Reaction
Authors: Wang Shuang‐Hu , Si Rui‐Qi , Zhuang Qing‐Bo , Guo Xiang , Ke Tian , Zhang Xiao‐Ming , Zhang Fu‐Min , Tu Yong‐Qiang 
Published: September 2020

AbstractA tandem Bischler–Napieralski/semipinacol rearrangement reaction has been developed for the purpose of assembling a bis(spirocyclic) indole framework, a privileged structural unit of aspidofractinine‐type monoterpenoid indole alkaloids, and was used in combination with a subsequent Mannich reaction to expeditiously construct the central bridged bicyclo[2.2.1]heptane ring system of these molecules with contiguous quaternary centers. The development of this novel strategy culminated in the collective total synthesis of four aspidofractinine alkaloids.
Reductive Charge Transfer through an RNA Aptamer
Authors: Frommer Jennifer , Müller Sabine 
Published: September 2020

AbstractThe transfer of charges through double helical DNA is a very well investigated bioelectric phenomenon. RNA, on the contrary, has been less studied in this regard. The few available data report on charge transfer through RNA duplex structures mainly composed of homonucleotide sequences. In the light of the RNA world scenarios, it is an interesting question, if charge transfer can be coupled with RNA function. Functional RNAs however, contain versatile structural motifs. Therefore, electron transport also through non‐Watson–Crick base‐paired regions might be required. We here demonstrate distance‐dependent reductive charge transfer through RNA duplexes and through the non‐Watson–Crick base‐paired region of an RNA aptamer.
Pb18O8Cl15I5: A Polar Lead Mixed Oxyhalide with Unprecedented Architecture and Excellent Infrared Nonlinear Optical Properties
Authors: Chen Xinglong , Jing Qun , Ok Kang Min 
Published: September 2020

AbstractTo develop high‐performance nonlinear optical (NLO) materials for infrared (IR) applications, we have applied a rational element‐composition design strategy and investigated the unexplored PbO–PbCl2–PbI2 system. By doing so, we discovered a new polar lead mixed oxyhalide, Pb18O8Cl15I5, the first synthetic metal oxyhalide combining both Cl− and I−. Pb18O8Cl15I5 reveals an unprecedented structural feature with two different dimensional types of oxocentered Pb–O units, namely, [O4Pb8]8+ clusters and [OPb2]2+ chains. Centimeter‐sized single crystals of Pb18O8Cl15I5 have been successfully grown under ambient conditions. Remarkably, Pb18O8Cl15I5 satisfies all fundamental yet rigorous criteria for high‐performance IR NLO materials, exhibiting the widest IR transparency (up to 16.0 μm) among oxide‐based crystals, strong second‐harmonic generation response (1.05×AgGaS2), superior birefringence (0.086 at 636 nm), and a high laser‐induced damage threshold (8.5×AgGaS2).
Colyliform Crystalline 2D Covalent Organic Frameworks (COFs) with Quasi‐3D Topologies for Rapid I2 Adsorption
Authors: Guo Xinghua , Li Yang , Zhang Meicheng , Cao Kecheng , Tian Yin , Qi Yue , Li Shoujian , Li Kun , Yu Xiaoqi , Ma Lijian 
Published: September 2020

AbstractConstructing three‐dimensional (3D) structural characteristics on two‐dimensional (2D) covalent organic frameworks (COFs) is a good approach to effectively improve the permeability and mass transfer rate of the materials and realize the rapid adsorption for guest molecules, while avoiding the high cost and monomer scarcity in preparing 3D COFs. Herein, we report for the first time a series of colyliform crystalline 2D COFs with quasi‐three‐dimensional (Q‐3D) topologies, consisting of unique “stereoscopic” triangular pores, large interlayer spacings and flexible constitutional units which makes the pores elastic and self‐adaptable for the guest transmission. The as‐prepared QTD‐COFs have a faster adsorption rate (2.51 g h−1) for iodine than traditional 2D COFs, with an unprecedented maximum adsorption capacity of 6.29 g g−1. The excellent adsorption performance, as well as the prominent irradiation stability allow the QTD‐COFs to be applied for the rapid removal of radioactive iodine.
Aminopotassiation by Mixed Potassium/Lithium Amides: A Synthetic Path to Difficult to Access Phenethylamine Derivates
Authors: Hermann Andreas , Opper Ulrike , Voß Andreas , Brieger Lukas , Otte Felix , Unkelbach Christian , O'Shea Donal F. , Strohmann Carsten 
Published: September 2020

AbstractInsights gained from a comparison of aminometalation reactions with lithium amides, potassium amides and mixed lithium/potassium amides are presented. A combination of structural characterization, DFT calculations and electrophile reactions of aminometalated intermediates has shown the advantages of using a mixed metal strategy. While potassium amides fail to add, the lithium amides are uncontrollable and eliminated, yet the mixed K/Li amides deliver the best of both systems. Aminopotassiation proceeds to form the alkylpotassium species which has enhanced stability over its lithium counterpart allowing for its isolation and thereby its further characterization.
Non‐Stationary Complementary Non‐Uniform Sampling (NOSCO NUS) for Fast Acquisition of Serial 2D NMR Titration Data
Authors: Romero Javier A. , Nawrocka Ewa K. , Shchukina Alexandra , Blanco Francisco J. , Diercks Tammo , Kazimierczuk Krzysztof 
Published: September 2020

AbstractNMR spectroscopy offers unique benefits for ligand binding studies on isotopically labelled target proteins. These benefits include atomic resolution, direct distinction of binding sites and modes, a lowest detectable affinity limit, and function independent setup. Yet, retracing protein signal assignments from apo to holo states to derive exact dissociation constants and chemical shift perturbation amplitudes (for ligand docking and structure‐based optimization) requires lengthy titration series of 2D heteronuclear correlation spectra at variable ligand concentration that may exceed the protein's lifetime and available spectrometer time. We present a novel method to overcome this critical limitation, based on non‐stationary complementary non‐uniform sampling (NOSCO NUS) combined with a robust particle swarm optimization algorithm. We illustrate its potential in two challenging studies with very distinct protein sizes and binding affinities, showing that NOSCO NUS can reduce measurement times by an order of magnitude to make such highly informative NMR titration studies more broadly feasible.
Design of a Single‐Atom Indiumδ+–N4Interface for Efficient Electroreduction of CO2to Formate
Authors: Shang Huishan , Wang Tao , Pei Jiajing , Jiang Zhuoli , Zhou Danni , Wang Yu , Li Haijing , Dong Juncai , Zhuang Zhongbin , Chen Wenxing , Wang Dingsheng , Zhang Jiatao , Li Yadong 
Published: September 2020

AbstractMain‐group element indium (In) is a promising electrocatalyst which triggers CO2reduction to formate, while the high overpotential and low Faradaic efficiency (FE) hinder its practical application. Herein, we rationally design a new In single‐atom catalyst containing exclusive isolated Inδ+–N4atomic interface sites for CO2electroreduction to formate with high efficiency. This catalyst exhibits an extremely large turnover frequency (TOF) up to 12500 h−1at −0.95 V versus the reversible hydrogen electrode (RHE), with a FE for formate of 96 % and current density of 8.87 mA cm−2at low potential of −0.65 V versus RHE. Our findings present a feasible strategy for the accurate regulation of main‐group indium catalysts for CO2reduction at atomic scale.
A New Mechanically‐Interlocked [Pd2L4] Cage Motif by Dimerization of two Peptide‐based Lemniscates
Authors: Schulte Thorben R. , Holstein Julian J. , Schneider Laura , Adam Abdulselam , Haberhauer Gebhard , Clever Guido H. 
Published: September 2020

AbstractMost metallo‐supramolecular assemblies of low nuclearity adopt simple topologies, with bridging ligands spanning neighboring metal centers in a direct fashion. Here we contribute a new structural motif to the family of host compounds with low metal count (two) that consists of a pair of doubly‐interlocked, Figure‐eight‐shaped subunits, also termed “lemniscates”. Each metal is chelated by two chiral bidentate ligands, composed of a peptidic macrocycle that resembles a natural product with two pyridyl‐terminated arms. DFT calculation results suggest that dimerization of the mononuclear halves is driven by a combination of 1) Coulomb interaction with a central anion, 2) π‐stacking between intertwined ligand arms and 3) dispersive interactions between the structure's compact inner core bedded into an outer shell composed of the cavitand‐type macrocycles. The resulting cage‐like architecture was characterized by NMR, MS and X‐ray structure analyses. This new mechanically bonded system highlights the scope of structural variety accessible in metal‐mediated self‐assemblies composed of only a few constituents.
Covalent surface functionalization of nonwoven fabrics with controlled hydrophobicity, water absorption, and pH regulation properties
Authors: Dan Yoav , Buzhor Marina , Raichman Daniel , Menashe Eti , Rachmani Oren , Amir Elizabeth 
Published: September 2020

AbstractA modular method for functionalization of nonwoven fabrics was developed using a two‐step process. In the first step, the fabrics were grafted with a linker molecule, 10‐undecenoyl chloride, via esterification, followed by attachment of a functional material under UV irradiation. Perfluorodecanethiol and 3‐mercaptopropionic acid (MPA) were connected to the linker‐modified fabrics using thiol‐ene click chemistry. Perfluorodecanethiol modified fabrics exhibited hydrophobicity with water contact angle of about 140° while MPA‐modified fabrics were able to lower the pH of a solution by about 1.6. We additionally demonstrated the possibility to connect functional polymers to the linker‐modified fabrics by radical graft polymerization of acrylic acid; this produced a thin layer of the polymer on the surface of the fabric. Fabrics modified with poly(acrylic acid) exhibited increased hydrophilicity with water contact angle of 0° for both cotton and viscose‐polyester fabrics, while the water absorption capability for polypropylene fabrics increased from about 50 to 1200%.
2020 Roadmap on Zinc Metal Batteries
Authors: Xu Chenxuan , Zhang Yu , Zhang Naiqing , Liu Xiaoyu , Yi Jin , Liu Xiaoqing , Lu Xihong , Ru Qiang , Lu Hao , Peng Xinwen , Zhao X. S. , Ma Jianmin 
Published: September 2020

AbstractMetallic zinc (Zn) is considered to be a safe and low‐cost anode for rechargeable batteries. Thus, several zinc metal batteries (ZMBs) have been well developed, i. e., zinc silver batteries, Zn−MnO2 batteries, nickel‐zinc batteries, zinc‐air batteries and other kinds of zinc ion batteries. ZMBs are strongly correlated with electrochemistry, electrodes, electrolytes and battery structures. To support the development of this field, we herein invite some famous research experts to write this roadmap for giving some guidance in future research. The roadmap will include their research status, challenge, opportunities, and the technology advance in their fields. We expect this roadmap will produce active influence in developing green, low‐cost, safe ZMBs for our bright life in future.
Folic acid antagonist use before and during pregnancy and risk for selected birth defects
Authors: Kerr Stephen M. , Parker Samantha E. , Mitchell Allen A. , Tinker Sarah C. , Werler Martha M. 
Published: September 2020

AbstractBackgroundMaternal folic acid (FA) intake before and during early pregnancy reduces the risk for neural tube defects (NTDs); evidence suggests it may also reduce the risk for oral clefts, urinary defects, and cardiac defects. We sought to re‐examine the use of drugs, which affect folate metabolism, dihydrofolate reductase inhibiting (DHFRI) medications, and anti‐epileptic drugs (AEDs), in data collected in the post‐FA fortification era (1998+) in the Slone Birth Defects Study.MethodsWe assessed maternal DHFRI and AED use and risk for NTDs, oral clefts, and urinary and cardiac defects. We estimated odds ratios (ORs) and 95% confidence intervals (CIs) using logistic regression. We assessed daily average FA intake of ≥400 mcg as a potential effect modifier.ResultsWe analyzed data from 10,209 control and 9,625 case mothers. Among controls, the prevalence of exposure to DHFRI medications was 0.3% and to AEDs was 0.5%. Maternal use of AEDs was associated with increased risks for NTDs (OR: 3.4; 95% CI: 1.5, 7.5), oral clefts (OR: 2.3; 95% CI: 1.3, 4.0), urinary defects (OR: 1.6; 95% CI: 1.0, 2.7), and cardiac defects (OR: 1.6; 95% CI: 1.1, 2.3); similar or further increased risks were found among those with FA intake ≥400 mcg per day. DHFRI use was rare and relative risk estimates were imprecise and consistent with the null.ConclusionsSimilar to our previous analyses, we observed associations between AED use and these defects. For DHFRI exposure, we found no evidence for increased risk of these defects. Though statistical power to examine FA effect modification was low, we found no evidence of further protection among those with FA intake ≥400 mcg, with some associations somewhat stronger in this group.
Regulatory interventions improve the biosynthesis of limiting amino acids from methanol carbon to improve synthetic methylotrophy in Escherichia coli
Authors: Kyle Bennett Robert , Agee Alec , Har Jie R. G. , von Hagel Bryan , Antoniewicz Maciek R. , Papoutsakis Eleftherios T. 
Published: September 2020

AbstractSynthetic methylotrophy aims to engineer methane and methanol utilization pathways in platform hosts like Escherichia coli for industrial bioprocessing of natural gas and biogas. While recent attempts to engineer synthetic methylotrophs have proved successful, autonomous methylotrophy, that is, the ability to utilize methane or methanol as sole carbon and energy substrates, has not yet been realized. Here, we address an important limitation of autonomous methylotrophy in E. coli: the inability of the organism to synthesize several amino acids when grown on methanol. We targeted global and local amino acid regulatory networks. Those include removal of amino acid allosteric feedback inhibition (argAH15Y, ilvAL447F, hisGE271K, leuAG462D, proBD107N, thrAS345F, trpES40F), knockouts of transcriptional repressors (ihfA, metJ); and overexpression of amino acid biosynthetic operons (hisGDCBHAFI, leuABCD, thrABC, trpEDCBA) and transcriptional regulators (crp, purR). Compared to the parent methylotrophic E. coli strain that was unable to synthesize these amino acids from methanol carbon, these strategies resulted in improved biosynthesis of limiting proteinogenic amino acids (histidine, leucine, lysine, methionine, phenylalanine, threonine, tyrosine) from methanol carbon. In several cases, improved amino acid biosynthesis from methanol carbon led to improvements in methylotrophic growth in methanol minimal medium supplemented with a small amount of yeast extract. This study addresses a key limitation currently preventing autonomous methylotrophy in E. coli and possibly other synthetic methylotrophs and provides insight as to how this limitation can be alleviated via global and local regulatory modifications.