bluuebunny/crossref_metadata_2025 huggingface dataset:
Interfacially Polymerized Polyamide Interlayer onto Ozonated Carbon Nanotube Networks for Improved Stability of Sulfur Cathodes
Authors: Rana Harpalsinh H. , Jana Milan , Yeon Jeong Seok , Park Jeong Hee , Qing Liu , Park Ho Seok
Published: November 2019

Lithium–sulfur (Li–S) batteries are considered promising energy‐storage devices owing to the high specific capacity and low cost of the S cathode. However, they suffer from capacity decay and poor coulombic efficiency arising from the dissolution of long‐chain polysulfides and their shuttling. A facile and scalable method was developed to directly coat a thin (≈57.3 nm) and porous polyamide (PA) interlayer onto a S cathode by interfacial polymerization. This PA interlayer prevented the shuttling of polysulfides by creating a physical barrier and, through chemical interactions between the amide functionalities of PA and the polysulfides, allowing access to the S electrode by the Li ions. The resulting PA‐coated cathode exhibited approximately 64.2 % capacity retention over 1000 cycles at 1 C with only 0.0358 % decay per cycle and a moderate capacity of 1008 mAh g−1 at 0.1 C.
Open‐Close Strategy toward the Organocatalytic Generation of 2‐Deoxyribosyl Oxocarbenium Ions: Pyrrolidine‐Salt‐Catalyzed Synthesis of 2‐Deoxyribofuranosides
Authors: Ghosh Titli , Mukherji Ananya , Kancharla Pavan K.
Published: November 2019

The reaction of secondary amine salts with 2‐deoxy‐ribofuranoses under forcible conditions leads to the putative furanosyl oxocarbenium ion that is trapped with various alcohols to provide 2‐deoxy‐ribofuranosides. The observed anomeric selectivities range from an equimolar mixture to complete α‐selectivity in the case of bulky sugar acceptors. Owing to the mechanism and temperature of the transformation, the generated oxocarbenium ion shows little or no facial preference towards the nucleophilic attack of non‐carbohydrate acceptors and leads to a mixture of anomers in the case of benzyl and acetyl protected donors. However, the conformationally less flexible tetraisopropylsilyl protected donor reacted with both sugar and non‐sugar acceptors in a stereoselective fashion. Besides, the glycosylation with 2‐cyanoethanol gave the product with unexpected beta‐selectivity presumably due to nitrile effect. The operationally simple organocatalytic protocol provides easy access to otherwise difficult 2‐deoxy‐ribofuranosides/disaccharides.
Production of a NiO/Al primary battery employing powder‐based electrodes
Authors: Burrola Samantha , Horii Maya , Gonzalez‐Guerrero Maria Jose , Bachman John Christopher , Gomez Frank A.
Published: November 2019

This paper describes the use of aluminum and zinc as anodic materials for a battery employing nickel (II) oxide (NiO) as cathode. Comparison of both materials resulted in the development of a compact, cost effective, and easy to use primary NiO/Al battery employing an alkaline electrolyte. The system features electrodes composed of powder forms of the active materials on modified paper substrates that are contained in a simple multilayer design utilizing thin laminated plastic materials to provide structure and flexibility to the battery as well as a paper separator. Various concentrations of potassium hydroxide (KOH) electrolyte were examined and maximum performance was observed at 6 M KOH. A maximum current density and power density of 1.94 mA/cm2 and 1 mW/cm2, respectively was achieved. This user‐friendly device was able to produce a maximum capacity of 2.33 mAh/g when 2 mA/g was applied. This work demonstrates the viability of a paper‐based battery featuring powder electrodes as a possible power source for microelectronic devices.
Recent Advances and Prospects of Metal‐Based Catalysts for Oxygen Reduction Reaction
Authors: Lang Peng , Yuan Nannan , Jiang Qianqian , Zhang Yichi , Tang Jianguo
Published: November 2019

Fuel cells, as one of the most promising technologies in sustainable energy conversion systems, hold great expectations for commercial applications. Cathode oxygen reduction reaction (ORR) kinetics of fuel cells are very slow and require a large overpotential to make the reaction occur, which greatly limits the energy output of fuel cells. Therefore, designing and preparing a highly active and stable ORR catalyst has become a great challenge. Herein, recent advances in platinum‐based and platinum‐free materials in metal‐based catalysts are focused on, including structural properties, synthesis methods, performance characterization, and catalytic mechanisms. Although platinum‐based precious metal catalysts have excellent performance, high prices limit the scale of commercial fuel cells. Nonprecious metal catalysts (e.g., transition metal nitrogen‐doped carbon‐based catalysts (M‐N/C), transition metal compounds (transition metal oxides—TMOs, transition metal carbides—TMCs, transition metal nitrides/transition metal oxynitrides—TMNs/TMNOs), layered double hydroxides—LDHs) completely eliminate dependence on precious metals and exhibit excellent ORR catalytic activity and stability. Finally, the ideas for future design and preparation of new ORR catalysts and challenges in the future of research work are discussed.
Formation of Nitrogen‐Doped Carbon‐Coated CoP Nanoparticles Embedded within Graphene Oxide for Lithium‐Ion Batteries Anode
Authors: Sun Shuo , Xie Tianhuan , Tao Shi , Sheng Peng , Han Zhengsi , Qian Bin , Jiang Xuefan
Published: November 2019

Due to its high electrochemical activities and low intercalation potential for Li/Li+, transition metal phosphides (TMPs) are booming as commerciogenic anode for lithium‐ion batteries (LIBs). Herein, the reasonable devise of nitrogen‐doped carbon‐coated CoP (CoP@NC) nanocomposites, which is derived from metal–organic frameworks (MOF‐Co) precursors, combining with graphene modification, is presented. The ultrafine CoP@NC nanoparticles are strongly incorporated with graphene networks (CoP@NC/GO). When assessed as anode electrode for LIBs, novel dual carbon encapsulation architectures of CoP@NC/GO hybrid composites exhibit superior cyclability (345 mAh g−1 at 1500 mA g−1 after 1000 cycles) and prominent rate ability (404 mAh g−1 at 3000 mA g−1). It is believed that this strategy can be helpful for boosting the electrochemical performance of the TMPs family as advance anode materials for energy storage systems.
Holocene climate in arid central Asia and timing of sand dunes accumulation in Balikun Basin, Northwest China
Authors: Ji Junliang , Wang Guocan , Yang Lirong , Li Jie , Xu Yang , Liu Zihan
Published: November 2019

Westerlies‐dominated arid central Asia (ACA) has a very fragile ecological environment that highly depends on the available moisture sources. However, the moisture history of this region during the Holocene has been a controversial topic for several decades. Here, we performed optically stimulated luminescence (OSL) dating and grain‐size analysis of aeolian sediments from the eastern Balikun Basin. Our results demonstrated that the early Holocene climate in the Balikun Basin was dry (before ~6.5 ka) and then became wetter during the mid–late Holocene. This Holocene climate pattern correlates well with other climatic inferences from various proxies acquired at various ACA locations, further supporting an earlier view that the Holocene climate in ACA was out of phase with that of the East Asia summer monsoon. Furthermore, an extremely dry event at 4.3–2.6 ka correlated well with pollen records and a decrease of ~4°C in temperature in the western Balikun Lake, but this event was not evident in other ACA regions. Finally, Mingsha Shan Sand Dunes in the eastern Balikun Basin initially accumulated in the earliest Holocene. We suggest that the early Holocene dry climate in the ACA region and the local geomorphology are responsible for the formation of the Mingsha Shan Sand Dunes.
Late Palaeozoic tectonic evolution of North Tianshan Orogenic Belt: Perspectives from geochronology and geochemistry of the Tulasu pluton in the Tulasu Basin
Authors: Zhang Jingbo , An Fang , Wei Shaoni , Cai Guangyao
Published: November 2019

The Tulasu pluton is located in the northeast of the Tulasu Basin, North Tianshan, which is composed of three rock types including quartz diorite porphyry, pyroxene diorite porphyry, and granite. Zircon U‐Pb dating indicates that the quartz diorite porphyry and pyroxene diorite porphyry were crystallized in the Late Devonian (with ages at 360.3 ± 7.8 and 375.4 ± 6.2 Ma, respectively), while the granitic rocks was formed in the Late Carboniferous (at 305.9 ± 5.9 Ma), suggesting that the Tulasu pluton was the product of two magmatic episodes. The Late Devonian quartz diorite and pyroxene diorite porphyry are metaluminous and belong to calc‐alkaline to high‐K calc‐alkaline series. Quartz diorite porphyry and pyroxene diorite porphyry are characterized by the prominent enrichment in LILEs, such as Rb, Th, U, and K, and depletion in HFSEs, such as Nb, Ta, P, and Ti, which is similar to typical subduction‐related arc magma. The εHf(t) values of quartz diorite porphyry and pyroxene diorite porphyry are +4.5–+8.8 and +2.0–+6.4, respectively, indicating that they are derived from depleted mantle wedge. Their TDM2 ages are 814–1,087 Ma and 955–1,227 Ma, respectively, which shows that the Mesoproterozoic to the Neoproterozoic crustal materials were involved. Their high Ba/La (10.26–17.92), low Th/Yb (1.96–5.80), and relatively low Ce/Th (3.16–7.34) and Ba/Th (18.29–38.92) ratios indicate that they were probably produced by partial melting of depleted mantle wedge metasomatized by slab‐derived aqueous fluids, with involvement of subducted sediment. Geochemical characteristics indicate that the Late Devonian dioritic magma was generated in an arc‐related tectonic setting. The Late Carboniferous granitic rocks were composed of granodiorite porphyry and granite porphyry. The granodiorite porphyry samples are high‐K calc‐alkaline and peraluminous, while the granite porphyry samples are in the boundary zones of shoshonite and high‐K calc‐alkaline, as well as metaluminous and weakly peraluminous. Granodiorite porphyry shows features of I‐type granite, while granite porphyry has the characteristics of A‐type granite. High 176Hf/177Hf ratios (0.282600–0.282833) and εHf(t) values (+0.4–+8.7) indicate that granitic rocks have affinities with both depleted mantle and crust. Geochemical characteristics suggest that the Late Carboniferous granitic magma was formed in post‐collisional setting.
Geochemical characterization of mineralized albitite from Paleoproterozoic Bhukia IOCG‐IOA deposit of Aravalli‐Delhi Fold Belt, Rajasthan, western India: Genetic linkage to the gold (±Cu ± U) mineralization
Authors: Mukherjee Rahul , Venkatesh Akella Satya , Fareeduddin
Published: November 2019

Paleoproterozoic Bhukia gold deposit is located within the Debari Group of Aravalli Supergroup, Rajasthan, northwestern India. The major lithounits that are associated with gold–graphite (±Cu ± U) mineralization exposed in Bhukia are albitite, carbonates, and quartzite which have undergone upper greenschist to amphibolite facies metamorphism. Ore mineralization viz. pyrrhotite, arsenopyrite, chalcopyrite, pyrite, graphite, magnetite, and goethite in the study area are associated with NNW–SSE trending shear zone. Nuggets of gold are identified in the thick gossan zones that occurs parallel to the shear zone. The gold–sulfide lodes of the Bhukia deposits are largely confined either to marble or albitized marble and pure monomineralic albitite. The mineralization that is associated with the albitite, follows the boundaries of albite grains which confirms the role of these weak zones for the mobilization of mineralizing fluid and concentration of metal ions. Hence, geochemical studies of albitite would help to evaluate the petrogenesis, likely magmatic affinity, tectonic setting, controls of the mineralizing fluid, source, and their linkage to the gold (±Cu ± U) metallogeny. Bhukia albitite is characterized by Na–Al–rich and K‐poor compositions along with metaluminous nature. Geochemical analysis of various key elements suggests that albitite is the product of low‐K calc‐alkaline magma series with variation in Nb/Ta ratio indicating their fractionation during the melt–rock interaction within the shear zone. Geochemical signatures suggest the role of upper continental crust in channelizing the mineralized fluids that generated albitite with felsic to intermediate composition in and around Bhukia deciphered from their low Nb/Y ratios. Lower concentration of compatible elements (Ni and Cr) and higher concentration of incompatible elements (Th, La, and Nd) with SiO2 suggest that evolution of albitite rock is related to the fractional crystallization process. Zr/Hf ratios of 9–35 with the average of 18 suggest that albitite formed under magmatic–hydrothermal transitional environment. Rare Earth Elements (REE) patterns of albitite samples are moderately fractionated showing Light Rare Earth Elements (LREE)‐enrichment with a rather steep slope and exhibit distinct negative Eu anomalies (0.42–0.71, average 0.57). The enrichment of LREE in comparison to the Heavy Rare Earth Elements (HREE) suggests a more evolved source, i.e., process of melting at shallow environments. Tectonic setting of albitite samples suggest their origin in a volcanic arc region that underwent rifting. Detailed geochemical characterization unravelled complex evolutionary history of albitite in the Bhukia area, which attests derivation of the parental melt possibly from an enriched SCLM (Sub‐continental lithospheric mantle) source similar to most of the IOCG‐IOA deposits worldwide.
Grade 1 Acute on Chronic Liver Failure Is a Predictor for Subsequent Grade 3 Failure
Authors: Mahmud Nadim , Sundaram Vinay , Kaplan David E. , Taddei Tamar H. , Goldberg David S.
Published: November 2019

Background and Aims

Acute on chronic liver failure (ACLF) results in extremely high short‐term mortality in patients with underlying cirrhosis. The European Association for the Study of the Liver criteria grade ACLF severity from 1 (least severe) to 3 (most severe) based on organ failures (OFs) that develop after an acute decompensation (AD). However, the implications of surviving low‐grade ACLF in terms of risk of subsequent high‐grade ACLF are unclear.

Approach and Results

We conducted a retrospective cohort study of patients with compensated cirrhosis in the Veterans Health Administration database from January 2008 to June 2016. Propensity matching for grade 1 (G1) ACLF, followed by Cox regression, was used to model risk of subsequent grade 3 (G3) ACLF. Stratified analyses of different ADs and OFs were also performed. We identified 4,878 patients with well‐matched propensity scores. G1 ACLF events conferred a significantly increased risk of subsequent G3 ACLF relative no previous G1 ACLF (hazard ratio, 8.69; P < 0.001). When stratified by AD, patients with ascites or hepatic encephalopathy were significantly more likely to develop G3 ACLF relative to those with gastrointestinal bleed or infection as an AD (P < 0.001). Risk of G3 ACLF also varied significantly by type of OF characterizing previous G1 ACLF, with liver, coagulation, and circulatory failure posing the highest increased risk.

Conclusions

Patients who recover from G1 ACLF have substantially increased risk of later developing G3 ACLF as compared to those who never have G1 ACLF. Moreover, reversible decompensations for G1 ACLF have a lower risk of G3 ACLF, and liver‐intrinsic OFs confer a much higher risk of G3 ACLF. These findings have implications for prognosis, future surveillance, and triaging early transplant evaluation.
Abdominal and gluteofemoral size and risk of liver cancer: The liver cancer pooling project
Authors: Florio Andrea A. , Campbell Peter T. , Zhang Xuehong , Zeleniuch‐Jacquotte Anne , Wactawski‐Wende Jean , Smith‐Warner Stephanie A. , Sinha Rashmi , Simon Tracey G. , Sesso Howard D. , Schairer Catherine , Rosenberg Lynn , Rohan Thomas E. , Robien Kim , Renehan Andrew G. , Purdue Mark P. , Poynter Jenny N. , Palmer Julie R. , Newton Christina C. , Lu Yunxia , Linet Martha S. , Liao Linda M. , Lee I‐Min , Koshiol Jill , Kitahara Cari M. , Kirsh Victoria A. , Hofmann Jonathan N. , Graubard Barry I. , Giovannucci Edward , Gaziano John M. , Gapstur Susan M. , Freedman Neal D. , Demuth Jane , Chong Dawn Q. , Chan Andrew T. , Buring Julie E. , Bradshaw Patrick T. , Beane Freeman Laura E. , McGlynn Katherine A. , Petrick Jessica L.
Published: November 2019

Obesity is known to be associated with primary liver cancer (PLC), but the separate effects of excess abdominal and gluteofemoral size are unclear. Thus, we examined the association between waist and hip circumference with risk of PLC overall and by histologic type—hepatocellular carcinoma (HCC) and intrahepatic cholangiocarcinoma (ICC). The Liver Cancer Pooling Project is a consortium of prospective cohort studies that include data from 1,167,244 individuals (PLC n = 2,208, HCC n = 1,154, ICC n = 335). Multivariable‐adjusted hazard ratios (HRs) and 95% confidence intervals (CI) were estimated using proportional hazards regression. Waist circumference, per 5 cm increase, was associated with an 11% increased PLC risk (HR = 1.11, 95%CI: 1.09–1.14), including when adjusted for hip circumference (HR = 1.12, 95%CI: 1.08–1.17) and also when restricted to individuals in a normal body mass index (BMI) range (18.5 to <25 kg/m2; HR = 1.14, 95%CI: 1.07–1.21). Hip circumference, per 5 cm increase, was associated with a 9% increased PLC risk (HR = 1.09, 95%CI: 1.06–1.12), but no association remained after adjustment for waist circumference (HR = 0.99, 95%CI: 0.94–1.03). HCC and ICC results were similar. These findings suggest that excess abdominal size is associated with an increased risk of liver cancer, even among individuals considered to have a normal BMI. However, excess gluteofemoral size alone confers no increased risk. Our findings extend prior analyses, which found an association between excess adiposity and risk of liver cancer, by disentangling the separate effects of excess abdominal and gluteofemoral size through utilization of both waist and hip circumference measurements.
Abortion care in Ireland: Developing legal and ethical frameworks for conscientious provision
Authors: Donnelly Mary , Murray Claire
Published: November 2019

This article celebrates the remarkable changes which have occurred in the provision of abortion care in Ireland following the vote to remove the restrictive Eighth Amendment to the Constitution of Ireland in May 2018. However, it also identifies ways in which the emerging legal, ethical and clinical landscape is still impeding the conscientious provision of abortion care. It argues that in order to address these impediments, more attention needs to be paid to the ethical context for conscientious provision. This requires political leadership as well as ongoing leadership by professional bodies to develop both the clinical and the ethical guidance for conscientious provision.
Two are better than one: Volatility forecasting using multiplicative component GARCH‐MIDAS models
Authors: Conrad Christian , Kleen Onno
Published: November 2019

We examine the properties and forecast performance of multiplicative volatility specifications that belong to the class of generalized autoregressive conditional heteroskedasticity–mixed‐data sampling (GARCH‐MIDAS) models suggested in Engle, Ghysels, and Sohn (Review of Economics and Statistics, 2013,95, 776–797). In those models volatility is decomposed into a short‐term GARCH component and a long‐term component that is driven by an explanatory variable. We derive the kurtosis of returns, the autocorrelation function of squared returns, and theR2of a Mincer–Zarnowitz regression and evaluate the QMLE and forecast performance of these models in a Monte Carlo simulation. For S&P 500 data, we compare the forecast performance of GARCH‐MIDAS models with a wide range of competitor models such as HAR (heterogeneous autoregression), realized GARCH, HEAVY (high‐frequency‐based volatility) and Markov‐switching GARCH. Our results show that the GARCH‐MIDAS based on housing starts as an explanatory variable significantly outperforms all competitor models at forecast horizons of 2 and 3 months ahead.
Refining the workhorse oil market model
Authors: Zhou Xiaoqing
Published: November 2019

The Kilian and Murphy (Journal of Applied Econometrics, 2014, 29, 454–478) structural vector autoregressive model has become the workhorse model for the analysis of oil markets. I explore various refinements and extensions of this model, including the effects of (1) correcting an error in the measure of global real economic activity, (2) explicitly incorporating narrative sign restrictions into the estimation, (3) relaxing the upper bound on the impact price elasticity of oil supply, (4) evaluating the implied posterior distribution of the structural models, and (5) extending the sample. I demonstrate that the substantive conclusions of Kilian and Murphy (2014) are largely unaffected by these changes.
Political Conservatism and Anthropomorphism: An Investigation
Authors: Chan Eugene Y.
Published: November 2019

In the current research, we explore the possibility that politically conservative consumers may anthropomorphize consumer products more than their liberal counterparts. This is possibly because conservatives need to manage uncertainty in the marketplace. One way to do so might be by assigning more human‐like attributes to inanimate products. We test this hypothesis in three studies by measuring (Studies 1 and 2) and manipulating political ideology (Study 3). We find that avoidance of uncertainty (Study 1) and need for order (Study 2) can explain conservatives’ greater anthropomorphism. The effect is stronger for unpredictable than predictable products as the former are associated with greater uncertainty, which conservatives need to manage (Study 3). Also, we report that greater anthropomorphism of products can increase the perceived functionality of the products (Studies 2 and 3), offering implications for marketers. In all, the results offer support for our key hypothesis that conservatives anthropomorphize more; they also provide preliminary support for the role of uncertainty management in conservatives’ greater anthropomorphism of products. In our General Discussion, we discuss alternate explanations for the key effect and present some directions for further research in this area.
Catalytic activity of surface‐functionalized nanoscale nickel zinc multiferrites: potential vector for water purification
Authors: Tanwar Ruchika , Kumari Ritu , Mandal Uttam K , Kar Kamal K
Published: November 2019

BACKGROUND

Decontamination of water by means of photocatalysis is seen as a sustainable solution. However, catalysts with low recovery from liquid suspension remain the main predicament that obstructs their industrial applications. To overcome this shortcoming, a methodology is reported here for the functionalization of nanospinel nickel zinc ferrite by cystamine ligand to develop Ni0.5Zn0.5Fe2O4@cystamine magnetic recyclable catalyst for water decontamination applications.

RESULTS

The diffraction patterns of bare and functionalized nanoferrites indicated that the cubic inverse spinel structure of the particles was not changed after cystamine functionalization. X‐ray photoelectron spectroscopy (XPS) and Raman spectroscopy analyses confirmed the chemical bonding between cystamine and spinel ferrites. The spherical morphology and elemental composition were studied through high‐resolution transmission electron spectroscopy (HRTEM) images and energy‐dispersive X‐ray (EDX) analysis respectively. Deeper understanding of the catalyst's optical behavior and calculation of the energy band gap were achieved by means of photoluminescence spectroscopy. Magnetic saturation values were calculated from vibrating sample magnetometer (VSM) analysis, and almost negligible change was found. A possible photocatalytic mechanism for the removal of organic dye is proposed.

CONCLUSION

The present findings imply that the presence of amine groups on the catalyst surface, good dispersibility stability and outstanding catalytic activity make functionalized nanoferrite a suitable candidate for industrial wastewater treatment. Easy synthesis, easy work‐up and short reaction times are some of the advantages of the methodology. © 2019 Society of Chemical Industry
A sustainable system for maleic acid synthesis from biomass‐derived sugar
Authors: Yu Qiang , Bai Ruxue , Wang Fan , Zhang Qinghua , Sun Yongming , Zhang Yu , Qin Lei , Wang Zhongming , Yuan Zhenhong
Published: November 2019

BACKGROUND

The preparation of maleic acid from the oxidation of renewable furfural has attracted significant attention, but research regarding the direct transformation of biomass‐derived sugar to maleic acid is rare. The research regarding the direct transformation of xylose to maleic acid would further promote its industrial applications.

RESULTS

The direct synthesis of maleic acid from xylose was investigated based on a sustainable system of deep eutectic solvents (DESs). Four DESs were screened to evaluate their abilities for the dehydration of xylose. Hydrogen peroxide (H2O2) was then loaded to realize the oxidation of furfural without the separation of intermediates. A good maleic acid yield of 20.8%, along with 5.0% of fumaric acid, based on the xylose content were obtained under the initial xylose loading of 50 mM, a tin(IV) chloride (SnCl4)–xylose molar ratio of 4:1, in a monophase choline chloride (ChCl)–formic acid (Fa) (molar ratio of 1:6) system at 120 °C for 2 h. Then, 4 mL of H2O2 per mmol furfural was loaded for a further 10 min at 120 °C.

CONCLUSION

This ChCl–Fa–SnCl4–H2O2 system possesses a higher oxidation selectivity to maleic acid with no furanone and succinic acid. Moreover, it was interesting that ChCl and SnCl4 could be recovered through natural recrystallization. © 2019 Society of Chemical Industry
In situ construction of hierarchical graphitic carbon nitride homojunction as robust bifunctional photoelectrocatalyst for overall water splitting
Authors: Luo Leng , Zhang Hua‐Wei , Han Er‐Xun , Zhou Bin‐Xin , Huang Wei‐Qing , Hu Wangyu , Huang Gui‐Fang
Published: November 2019

BACKGROUND

Sustainable production of oxygen and hydrogen via catalyst‐aided water splitting utilizing solar energy has attracted increasing interest. The primary issue in this field is the development of earth‐abundant and active photoelectrocatalytic materials. Herein, a novel hierarchical g‐C3N4/g‐C3N4 metal‐free homojunction catalyst is synthesized through partial hydrolysis of melamine in alkali and subsequent thermal treatment.

RESULTS

The hierarchical g‐C3N4/g‐C3N4 metal‐free homojunction composed of lamellas features large exposed surface area, abundant interface contact and more channels for mass transfer, making it highly effective for water splitting with a small overpotential of 500 mV at 10 mA cm−2 and low Tafel slope of 93.1 mV dec−1 for oxygen evolution reaction (OER) in 1.0 mol L−1 potassium hydroxide (KOH) solution, as well as 259 mV at 10 mA cm−2 and 109.33 mV dec−1 for hydrogen evolution reaction (HER) in 0.5 mol L−1 sulfuric acid (H2SO4) solution. Furthermore, the overpotential and Tafel slope further decrease to 383.4 mV and 69.52 mV dec−1 for OER, 150.1 mV and 67.93 mV dec−1 for HER upon visible light irradiation, demonstrating the exceptional photo‐responsive catalytic performance, which can be attributed to the direct Z‐scheme homojunction resulting in effective charge transfer and •OH and superoxide free radicals produced under visible light irradiation.

CONCLUSION

This work provides a facile but effective approach for the construction of metal‐free OER/HER bifunctional catalyst with high photo‐responsive performance, achieving higher activity for catalyst‐assisted water splitting. © 2019 Society of Chemical Industry
Synthesis and evaluation of a radioiodinated BODIPY derivative as a thiol‐labeling agent
Authors: Watanabe Hiroyuki , Itagaki Futa , Shimizu Yoichi , Iikuni Shimpei , Ono Masahiro
Published: November 2019

Labeling agents with radioisotopes or fluorescent dyes are useful for investigating the biodistributions of biologically active proteins and peptides. Compared with molecular imaging with a single modality, dual imaging probes provide complementary information for each modality. The development of a dual radioisotope/fluorescence agent for protein labeling would thus be valuable for both preclinical and clinical applications. In this study, we designed and synthesized a radioiodinated BODIPY derivative (BODIPY‐ML) with a maleimide group as a thiol‐labeling agent. In the presence of N‐chlorosuccinimide and 1% acetic acid, [125I]BODIPY‐ML was successfully obtained at a radiochemical yield of 42%. In conjugation studies, model proteins including RGD peptides and anti‐HER2 VHH were successfully labeled with BODIPY‐ML via covalent bonds. The results demonstrated the feasibility of the radioiodinated BODIPY as a dual‐labeling agent via thiol groups.
Elevation‐dependent cooling caused by volcanic eruptions during the last millennium
Authors: Ning Liang , Liu Jian , Bradley Raymond S. , Yan Mi , Chen Kefan , Sun Weiyi , Jin Chunhan
Published: November 2019

Amplified warming over high‐elevation regions has been observed in recent decades, affecting mountain hydrological systems, ecosystems, and socioeconomic development. However, whether natural forcing in the past caused similar elevation‐dependent temperature changes is unclear. Because limited observational data constrain our understanding of such elevation‐dependent temperature changes and the corresponding mechanisms, here we use multi‐model long‐term simulations to show that elevation‐dependent cooling (EDC) occurred after major volcanic eruptions during the last millennium. We propose two physical mechanisms responsible for the EDC: a reduction in latent heat release related to the tropical deep convection, serving as the large‐scale background climate change; feedbacks involving snow albedo and surface received short‐wave radiation, serving as the local processes. These findings improve our understanding of the physical mechanisms behind elevation‐dependent temperature changes, and provide insights for future climate projections considering both natural forcing and greenhouse gas increases.
Quantifying relationships between environmental factors and power dissipation on the most prolific days in the largest tornado “outbreaks”
Authors: Schroder Zoe , Elsner James B.
Published: November 2019

Studies show an increasing tendency for tornadoes in the United States to occur in larger outbreaks. To shed light on the reason for this, the authors use a regression model to quantify the relationship between convective environmental variables and accumulated tornado power (ATP). They consider only days with many tornadoes that occur as part of an outbreak. Results show an average upward trend in ATP at 5% ([2.5%, 12%], 95% uncertainty interval) per year. ATP increases by 125% for every 10 m⋅s−1 increase in bulk shear (on average)and by 33% for every 1,000 J⋅kg−1 increase in convective available potential energy holding the other variables constant. Changes in bulk shear, which has the largest effect on ATP, might help explain the documented changes in tornado activity.
Baltic Sea Hypoxia Takes Many Shapes and Sizes
Authors: Carstensen Jacob , Conley Daniel J.
Published: November 2019

The Baltic Sea is naturally prone to hypoxia, but the frequency and extent have increased multifold over the last century. Hypoxia manifests itself as perennial in the open central part, seasonal at the entrance area, and episodic at many coastal sites, and the expression of hypoxia is largely driven by differences in bottom water residence times and stratification patterns. Enhanced nutrient inputs from land and atmosphere are the main drivers of expanding hypoxia in the Baltic Sea although deoxygenation has also been exacerbated by increasing temperature over the past 3–4 decades. Hypoxia severely influences ecosystem functions such as fish production through reduced trophic efficiency and harmful cyanobacteria blooms sustained by phosphorus release from sediments. Nutrient inputs from land have created the largest man‐made hypoxic area in the world and the only viable long‐term solution to mitigation is to continue efforts to reduce nutrient loading.
Acetylome analysis of lysine acetylation in the plant pathogenic bacterium Brenneria nigrifluens
Authors: Li Yong , Xue Han , Bian Dan‐ran , Xu Guantang , Piao Chungen
Published: November 2019

Protein lysine acetylation, a dynamic and reversible posttranslational modification, plays a crucial role in several cellular processes, including cell cycle regulation, metabolism, enzymatic activities, and protein interactions. Brenneria nigrifluens is a pathogen of walnut trees with shallow bark canker and can cause serious disease in walnut trees. Until now, a little has been known about the roles of lysine acetylation in plant pathogenic bacteria. In the present study, the lysine acetylome of B. nigrifluens was determined by high‐resolution LC‐MS/MS analysis. In total, we identified 1,866 lysine acetylation sites distributed in 737 acetylated proteins. Bioinformatics results indicated that acetylated proteins participate in many different biological functions in B. nigrifluens. Four conserved motifs, namely, LKac, Kac*F, I*Kac, and L*Kac, were identified in this bacterium. Protein interaction network analysis indicated that all kinds of interactions are modulated by protein lysine acetylation. Overall, 12 acetylated proteins were related to the virulence of B. nigrifluens.
Isolation of time‐dependent DNA damage induced by energetic carbon ions and their fragments using fluorescent nuclear track detectors
Authors: McFadden Conor H. , Rahmanian Shirin , Flint David B. , Bright Scott J. , Yoon David S. , O’Brien Daniel J. , Asaithamby Aroumougame , Abdollahi Amir , Greilich Steffen , Sawakuchi Gabriel O.
Published: November 2019

Purpose

High energetic carbon (C‐) ion beams undergo nuclear interactions with tissue, producing secondary nuclear fragments. Thus, at depth, C‐ion beams are composed of a mixture of different particles with different linear energy transfer (LET) values. We developed a technique to enable isolation of DNA damage response (DDR) in mixed radiation fields using beam line microscopy coupled with fluorescence nuclear track detectors (FNTDs).

Methods

We imaged live cells on a coverslip made of FNTDs right after C‐ion, proton or photon irradiation using an in‐house built confocal microscope placed in the beam path. We used the FNTD to link track traversals with DNA damage and separated DNA damage induced by primary particles from fragments.

Results

We were able to spatially link physical parameters of radiation tracks to DDR in live cells to investigate spatiotemporal DDR in multi‐ion radiation fields in real time, which was previously not possible. We demonstrated that the response of lesions produced by the high‐LET primary particles associates most strongly with cell death in a multi‐LET radiation field, and that this association is not seen when analyzing radiation induced foci in aggregate without primary/fragment classification.

Conclusions

We report a new method that uses confocal microscopy in combination with FNTDs to provide submicrometer spatial‐resolution measurements of radiation tracks in live cells. Our method facilitates expansion of the radiation‐induced DDR research because it can be used in any particle beam line including particle therapy beam lines.

Category

Biological Physics and Response Prediction.
A novel segmentation framework dedicated to the follow‐up of fat infiltration in individual muscles of patients with neuromuscular disorders
Authors: Ogier Augustin C. , Heskamp Linda , Michel Constance P. , Fouré Alexandre , Bellemare Marc‐Emmanuel , Le Troter Arnaud , Heerschap Arend , Bendahan David
Published: November 2019

Purpose

To propose a novel segmentation framework that is dedicated to the follow‐up of fat infiltration in individual muscles of patients with neuromuscular disorders.

Methods

We designed a semi‐automatic segmentation pipeline of individual leg muscles in MR images based on automatic propagation through nonlinear registrations of initial delineation in a minimal number of MR slices. This approach has been validated for the segmentation of individual muscles from MRI data sets, acquired over a 10‐month period, from thighs and legs in 10 patients with muscular dystrophy. The robustness of the framework was evaluated using conventional metrics related to muscle volume and clinical metrics related to fat infiltration.

Results

High accuracy of the semi‐automatic segmentation (mean Dice similarity coefficient higher than 0.89) was reported. The provided method has excellent reliability regarding the reproducibility of the fat fraction estimation, with an average intraclass correlation coefficient score of 0.99. Furthermore, the present segmentation framework was determined to be more reliable than the intra‐expert performance, which had an average intraclass correlation coefficient of 0.93.

Conclusion

The proposed framework of segmentation can successfully provide an effective and reliable tool for accurate follow‐up of any MRI biomarkers in neuromuscular disorders. This method could assist the quantitative assessment of muscular changes occurring in such diseases.
Functional outcomes and safety of GreenLight photovaporization of the prostate in the high‐risk patient with lower urinary tract symptoms due to benign prostatic enlargement
Authors: Barco‐Castillo Catalina , Plata Mauricio , Zuluaga Laura , Santander Jessica , Trujillo Carlos Gustavo , Caicedo Juan Ignacio , Serrano Adolfo , Fernández Nicolás , Azuero Julián
Published: November 2019

Aims

Photovaporization of the prostate (PVP) with GreenLight Laser is a surgical treatment for lower urinary tract symptoms. It is considered safe in elderly patients with comorbidities, however, the evidence is inconclusive. The objective of this study is to evaluate the efficacy and safety outcomes of PVP according to the American Society of Anesthesiologists Physical Status (ASAPS).

Methods

A cohort of 675 patients who underwent PVP between 2012 and 2018 was evaluated. Patients were classified according to their ASAPS as low (I and II) and high risk (III and IV). Surgical characteristics and improvement of symptoms and Quality of Life (QoL) were evaluated.

Results

The median age of high‐risk group was higher than low‐risk group. The high‐risk group had more history of anticoagulation, antiaggregation, urinary catheterization, urinary retention and urethral stricture. Longer times of hospitalization (23.7 [interquartile range {IQR} = 18.9‐41.35] vs 21.8 hours [IQR = 18.7‐26.6], P = .008) and catheterization (19.55 [IQR = 15.6‐35.57] vs 17.67 hours [IQR = 14.76‐22.5], P = .004) were found in the high‐risk group. Conversion and bleeding control were not different between groups. In the follow‐up, improvement of International Prostate Symptoms Score (IPSS) and QoL was significant in all patients when compared before and after surgery scores (P < .001). There were no difference between groups for QoL, however, IPSS was lower for the low‐risk group (8 [IQR = 4‐14.5] vs 5 [2‐12], P = .001).

Conclusion

PVP with GreenLight Laser is a safe and efficient procedure for all patients despite their comorbidities, with comparable middle‐term outcomes which makes it a standard treatment for the entire aging population, improving their QoL.
The association of patients' daily summarized self‐rated “real‐time” pain scores with physical recovery after major surgery – A repeated measurement design
Authors: Wikström Lotta , Nilsson Mats , Eriksson Kerstin
Published: November 2019

Aim

To determine the associations of patients' documented self‐rated pain with self‐rated early postoperative physical recovery.

Design

Observational with repeated measures.

Methods

General and orthopaedic inpatients (N = 479) were during the period 2012–2015 screened for pain. Individual daily median pain scores at rest and during activity were based on 4–9 self‐ratings on postoperative days 1 and 2, using the Numeric Rating Scale. Nine items reflecting physical recovery from the “Postoperative Recovery Profile” were used in a questionnaire.

Results

Associations between median pain scores on postoperative day 1 and physical recovery (fatigue, sleeping difficulties, bladder function, mobilization, muscle weakness and personal hygiene) the same day were found. Additionally, associations were found between median pain scores on day 1 and physical recovery (fatigue, sleeping difficulties, mobilization and muscle weakness) on day 2.
A homoisoflavonoid and a fatty acid in common purslane (Portulaca oleracea L.) synergistically inhibit growth of Spodoptera litura larvae
Authors: Wang Zhenzhen , Yang Renyue , Li Ping , Yang Zhongyan , Ling Ruimei , Shen Tunkai , Peng Weiyao , Yang Quan , Yan Jian
Published: November 2019

BACKGROUND

Portulaca oleracea L., common purslane, is an insecticidal plant that has been documented as a ‘Chinese indigenous pesticide’, and it is seldom visited by insects in the field. However, identification of anti‐insect compounds and mechanisms of action are still unclear.

RESULTS

Interplanting purslane with Chinese cabbage demonstrated that purslane may contain secondary compounds that S. litura avoids eating. Four compounds were isolated from P. oleracea by directed anti‐insect activity, and their chemical structures were identified by NMR spectra as (9Z,11E,15Z)‐13‐hydroxyoctadeca‐9,11,15‐trienoic acid (1), portulacanone A (2), portulacanone D (3), and a new natural product 2,4′‐dihydroxy‐3′,5′‐dimethoxychalcone (4). A combination of compound 1 and 2 possessed stronger activity than other combinations (compounds 1 + 3; 1 + 4; 2 + 3; 2 + 4; 3 + 4). Both active compounds were detected in all samples from 23 regions in China, and concentrations in samples collected from 17 regions were generally above 500 μg/kg. Concentrations of compounds 1 and 2 fluctuated greatly from April to November, and reached maximum concentrations of 45 951.44 μg/kg for compound 1 and 3739.09 μg/kg for compound 2 in November. The combination of these compounds (1 + 2) caused mid‐gut structural deformation and tissue decay as determined by mid‐gut histopathology of S. litura.

CONCLUSION

In general, these active compounds coexisting contributed to partly protect purslane from insects. This research also provides new insights into the use of purslane as important ingredient of botanical pesticide alternatives to traditional chemical pesticides. © 2019 Society of Chemical Industry
Development of analytical method of melamine in placenta from pregnant women by isotope‐dilution liquid chromatography/tandem mass spectrometry
Authors: Wu Chia‐Fang , Cheng Ching‐Mei , Hsu Yu‐Ming , Li Sih‐Shyan , Huang Chung‐Yi , Chen Yung‐Hung , Kuo Fu‐Chen , Wu Ming‐Tsang
Published: November 2019

Rationale

Melamine is ubiquitously present in our daily life. It has a known effect on the kidneys, but it may also adversely affect the reproduction system. We have developed an analytical method for measuring melamine levels in maternal placenta and correlated these levels with melamine concentrations in urine, a necessary step in finding out if melamine might cross the placenta and enter the circulation of the fetus.

Methods

We used liquid–liquid extraction, clean up by solid‐phase extraction (SPE), and isotope‐dilution liquid chromatography/tandem mass spectrometry (LC/MS/MS) to measure melamine in placenta specimens. The results of this method were assessed for linearity, limits of quantitation (LOQs), and intra‐ and inter‐assay precision as well as accuracy, matrix effect, and recovery rate.

Results

Calibration curves indicated good linearity (r >0.995) over concentrations ranging from 5 to 500 ng/mL in placenta specimens, intra‐ and inter‐assay precision from 0.89% to 27.07%, and accuracy from 92.4% to123.5%. Recovery ranged from 63.9 to 83.9%, and the LOQ was 5 ng/mL in placenta (0.2 g). Placental melamine levels ranged from 7.87 to19.64 ng/mL, all detectable (n = 8). Pregnant women with higher levels of urinary melamine had higher placenta melamine levels than those with non‐detectable urinary melamine, though the results were not significantly different (p = 0.149, n = 4 in each group).

Conclusions

The results of this study suggest that pregnant women were exposed to low doses of melamine in their daily lives as measured in urine samples and placenta specimens. It is unclear whether placenta melamine concentrations can better represent long‐term exposure than urine or whether melamine in the uterus can enter the fetus via this route.
Untargeted characterisation of dissolved organic matter contributions to rivers from anthropogenic point sources using direct‐infusion and high‐performance liquid chromatography/Orbitrap mass spectrometry
Authors: Pemberton Jonathan A. , Lloyd Charlotte E.M. , Arthur Christopher J. , Johnes Penny J. , Dickinson Michael , Charlton Adrian J. , Evershed Richard P.
Published: November 2019

Rationale

Anthropogenic organic inputs to freshwaters can exert detrimental effects on aquatic ecosystems, raising growing concern for both environmental conservation and water security. Current regulation by the EU water framework directive (European Union, 2000/60/EC) relates to organic pollution by monitoring selected micropollutants; however, aquatic ecosystem responses require a comprehensive understanding of dissolved organic matter (DOM) composition. The introduction of high‐resolution mass spectrometry (HRMS) is set to greatly increase our understanding of the composition of DOM of both natural and anthropogenic origin derived from diffuse and point sources.

Methods

DOM was extracted from riverine and treated sewage effluent using solid‐phase extraction (SPE) and analysed using dissolved organic carbon analysis, direct‐infusion high‐resolution mass spectrometry (DI‐HRMS) and high‐performance liquid chromatography (HPLC)/HRMS. The data obtained were analysed using univariate and multivariate statistics to demonstrate differences in background DOM, anthropogenic inputs and in‐river mixing. Compound identifications were achieved based on MS2 spectra searched against on‐line databases.

Results

DI‐HRMS spectra showed the highly complex nature of all DOM SPE extracts. Classification and visualisation of extracts containing many thousands of individual compounds were achieved using principal component analysis (PCA) and hierarchical cluster analysis. Kruskal‐Wallis analyses highlighted significant discriminating ions originating from the sewage treatment works for more in‐depth investigation by HPLC/HRMS. The generation of MS2 spectra in HPLC/HRMS provided the basis for identification of anthropogenic compounds including; pharmaceuticals, illicit drugs, metabolites and oligomers, although many thousands of compounds remain unidentified.

Conclusions

This new approach enables comprehensive analysis of DOM in extracts without any preconceived ideas of the compounds which may be present. This approach has the potential to be used as a high throughput, qualitative, screening method to determine if the composition of point sources differs from that of the receiving water bodies, providing a new approach to the identification of hitherto unrecognised organic contribution to water bodies.