bluuebunny/crossref_metadata_2025_split huggingface dataset:
Enhancing the CO2 Electroreduction of Fe/Ni‐Pentlandite Catalysts by S/Se Exchange
Authors: Pellumbi Kevinjeorjios , Smialkowski Mathias , Siegmund Daniel , Apfel Ulf‐Peter 
Published: May 2020

AbstractThe electrochemical reduction of CO2 is an attractive strategy towards the mitigation of environmental pollution and production of bulk chemicals as well as fuels by renewables. The bimetallic sulfide Fe4.5Ni4.5S8 (pentlandite) was recently reported as a cheap and robust catalyst for electrochemical water splitting, as well as for CO2 reduction with a solvent‐dependent product selectivity. Inspired by numerous reports on monometallic sulfoselenides and selenides revealing higher catalytic activity for the CO2 reduction reaction (CO2RR) than their sulfide counterparts, the authors investigated the influence of stepwise S/Se exchange in seleno‐pentlandites Fe4.5Ni4.5S8‐YSeY (Y=1–5) and their ability to act as CO2 reducing catalysts. It is demonstrated that the incorporation of higher equivalents of selenium favors the CO2RR with Fe4.5Ni4.5S4Se4 revealing the highest activity for CO formation. Under galvanostatic conditions in acetonitrile, Fe4.5Ni4.5S4Se4 generates CO with a Faradaic Efficiency close to 100 % at applied current densities of −50 mA cm−2 and −100 mA cm−2. This work offers insight into the tunability of the pentlandite based electrocatalysts for the CO2 reduction reaction.
1,2,4,5‐Tetrakis(tetramethylguanidino)‐3,6‐diethynyl‐benzenes: Fluorescent Probes, Redox‐Active Ligands and Strong Organic Electron Donors
Authors: Wagner Conrad , Kreis Franka , Popp Dennis , Hübner Olaf , Kaifer Elisabeth , Himmel Hans‐Jörg 
Published: May 2020

AbstractIn this work, the change of reactivity induced by the introduction of two para‐ethynyl substituents (CCSi(iPr)3 or CCH) to the organic electron‐donor 1,2,4,5‐tetrakis(tetramethylguanidino)‐benzene is evaluated. The redox‐properties and redox‐state dependent fluorescence are evaluated, and dinuclear CuI and CuII complexes synthesized. The Lewis‐acidic B(C6F5)3 substitutes the proton of the ethynyl −CCH groups to give new anionic −CCB(C6F5)3− substituents, leading eventually to a novel dianionic strong electron donor in its diprotonated form. Its two‐electron oxidation with dioxygen in the presence of a copper catalyst yields the first redox‐active guanidine that is neutral (instead of cationic) in its oxidized form.
Design, Synthesis and Biological Evaluation of Bengamide Analogues as ClpP Activators
Authors: Kong Xue‐Qing , Wei Bing‐Yan , Yu Chen‐Xi , Guan Xiang‐Na , Ma Wei‐Ping , Liu Gang , Yang Cai‐Guang , Nan Fa‐Jun 
Published: May 2020

Summary of main observation and conclusionTo combat multidrug‐resistant Gram‐positive bacteria, new antimicrobials particularly those with novel mechanism of action are badly needed. Different with conventional antibiotics which are typical inhibitors, small‐molecule activators of bacterial ClpP represent a new class of antibiotics. No ClpP activator has been developed for clinical trial. Herein, we conducted a screening on our library of bengamide‐like ring‐opened analogues and found that L472‐2 possesses a low minimum inhibitory concentration (MIC) against S.aureus and shows no activity for ClpP activation in vitro, but it displayed reduced antibacterial activity against S. aureus with clpP deletion. In order to obtain bengamide analogues that activate ClpP in vitro as well as possess antibacterial activity, we perform further structural modifications starting from L472‐2. Compound 37 remains the antimicrobial activity and activation of ClpP protein in vitro, which could be viewed as a new chemical scaffold for ClpP activators and worthy of further investigation.
Arenesulfonyl Fluoride Synthesis via Copper‐free Sandmeyer‐type Fluorosulfonylation of Arenediazonium Salts
Authors: Lin Qiongzhen , Ma Zhanhu , Zheng Changge , Hu Xiao‐Jun , Guo Yong , Chen Qing‐Yun , Liu Chao 
Published: May 2020

Summary of main observation and conclusionThe limited availability of highly valuable arenesulfonyl fluorides seriously hinders their further application in many research fields including medicinal chemistry and chemical biological, organic synthesis, polymer preparation, etc. We report herein a mild and efficient copper‐free Sandmeyer‐type fluorosulfonylation reaction of various arenediazonium salts to prepare valuable arenesulfonyl fluorides using K2S2O5 as both a reductant and a practical sulfonyl source in combination with N‐fluorobenzenesulfonimide as an effective fluorine source. This methodology provides an attractive route to diverse important arenesulfonyl fluorides given the overall practicality and scope.
Synthetic Guaiacol Derivatives as Promising Myeloperoxidase Inhibitors Targeting Atherosclerotic Cardiovascular Disease
Authors: Premkumar Jayaraj , Sampath Parthasarathy , Sanjay Rajagopalan , Chandrakala Aluganti , Rajagopal Desikan 
Published: May 2020

AbstractMyeloperoxidase (MPO) is known to cause oxidative stress and inflammation leading to cardiovascular disease (CVD) complications. MPO‐mediated oxidation of lipoproteins leads to dysfunctional entities altering the landscape of lipoprotein functionality. The specificity of guaiacol derivatives toward preventing MPO‐mediated oxidation to limit MPO's harmful effects is unknown. Diligent in silico studies were accomplished for a portfolio of compounds with guaiacol as a building block. The compounds’ activity toward MPO inhibition was also validated. The role of these chemical entities in controlling MPO‐mediated oxidation of lipoproteins (LDL and HDL) was shown to agree with our approach of developing powerful MPO inhibitors. The mechanism of MPO inhibition was demonstrated to be reversible in nature. This study reveals that there is great potential for guaiacol derivatives as therapeutics for CVD by modulating lipid profiles, reducing atherosclerotic plaque burden, and subsequently optimizing cardiovascular functions.
Synthesis and Biological Evaluation of Endocannabinoid Uptake Inhibitors Derived from WOBE437
Authors: Mäder Patrick , Bartholomäus Ruben , Nicolussi Simon , Baumann Alice , Weis Melanie , Chicca Andrea , Rau Mark , Simão Ana Catarina , Gertsch Jürg , Altmann Karl‐Heinz 
Published: May 2020

AbstractWOBE437 ((2E,4E)‐N‐(3,4‐dimethoxyphenethyl)dodeca‐2,4‐dienamide, 1) is a natural product‐derived, highly potent inhibitor of endocannabinoid reuptake. In this study, we synthesized almost 80 analogues of 1 with different types of modifications in the dodecadienoyl domain as well as the dimethoxyphenylethyl head group, and we investigated their effects on anandamide uptake into U937 cells. Intriguingly, none of these analogues was a more potent inhibitor of anandamide uptake than WOBE437 (1). At the same time, a number of WOBE437 variants exhibited potencies in the sub‐100 nM range, with high selectivity over inhibition of the endocannabinoid‐degrading enzyme fatty acid amide hydrolase; two compounds were virtually equipotent with 1. Interestingly, profound activity differences were observed between analogues in which either of the two methoxy substituents in the head group had been replaced by the same bulkier alkoxy group. Some of the compounds described here could be interesting departure points for the development of potent endocannabinoid uptake inhibitors with more drug‐like properties.
Supervised machine learning for coronary artery lumen segmentation in intravascular ultrasound images
Authors: Cui Hengfei , Xia Yong , Zhang Yanning 
Published: May 2020

AbstractIntravascular ultrasound (IVUS) has been widely used to capture cross sectional lumen frames of inner wall of coronary arteries. This kind of medical imaging modalities is capable of providing detailed and significant information of lumen contour shape, which is very important for clinical diagnosis and analysis of cardiovascular diseases. Numerous learning based techniques have recently become very popular for coronary artery segmentation due to their impressive results. In this work, a supervised machine learning method for coronary artery lumen segmentation with high accuracy and minimal user interaction is designed. The fully discriminative lumen segmentation method jointly learning a classifier the weak learners rely on and the features of the classifier is developed. Additionally, the theoretical supports of the Gradient Boosting framework used in this work and its quadratic approximation are presented. The proposed algorithm is tested on the public datasets of boundary detection of lumen in IVUS challenge held in MICCAI 2011 and achieves a higher average Jaccard similarity of 96.8% and a lower mean error distance of 0.55 (in Cartesian coordinates), which shows higher accuracy compared to the existing learning based methods. Moreover, three real patient IVUS datasets are used to evaluate the performance of the proposed coronary artery lumen segmentation algorithm, which is shown to achieve lower percent error of lumen area of 1.861% ± 0.965%, 1.968% ± 0.864%, and 1.671% ± 0.584%, respectively, compared to the manually measured lumen area (ground truth). The proposed lumen segmentation method is found to be superior to the latest learning based segmentation techniques. Given the efficiency and robustness, our method has great potential in IVUS images processing and coronary artery segmentation and quantification.Novelty StatementThe main contributions are summarized in the following aspects:
A detailed review of related work about learning based coronary artery lumen segmentation in intravascular ultrasound images is presented.
A fully discriminative lumen segmentation method jointly learning a classifier our weak learners rely on and the features of the classifier is developed.
The theoretical supports of the Gradient Boosting framework and its quadratic approximation used in this work are presented.
Severe infusion reaction due to nivolumab: A case report
Authors: Kumari Seema , Yun James , Soares James R. , Ding Pei N. 
Published: May 2020

AbstractBackgroundNivolumab is an anti‐PD1 immune checkpoint inhibitor commonly used for the treatment of solid organ and hematological malignancies. Severe infusion reaction due to nivolumab is quite rare.CaseWe report a case of severe infusion reaction due to nivolumab necessitating ICU admission and withdrawal of further nivolumab use in a patient with metastatic non‐small cell lung cancer.ConclusionOur knowledge and expertise with the use of immune checkpoint inhibitors are still evolving. This report highlights one of the rare possible side‐effects that clinicians and patients may have to face with increasing indications and use of nivolumab in day to day practice.
Simultaneous and Significant Improvements in Efficiency and Stability of Deep‐Blue Organic Light Emitting Diodes through Friedel‐Crafts Arylmethylation of a Fluorophore
Authors: Feng Quanyou , Tan Kesheng , Zheng Xiaojun , Xie Songlin , Xue Kai , Bo Yifan , Zhang He , Lin Dongqing , Rao Junfeng , Xie Xinmiao , Xie Linghai , Cao Hongtao , Zhang Hongmei , Wei Ying , Huang Wei 
Published: May 2020

AbstractThe front cover artwork is provided by the Huang Group at the Institute of Advanced Materials (IAM) at Nanjing University of Posts and Telecommunications (China). The image shows how comprehensive performances of deep‐blue organic light‐emitting diodes can be achieved through Friedel–Crafts arylmethylation of a fluorophore. Read the full text of the Communication at 10.1002/cptc.201900268.
Oxygen‐Vacancy‐Enhanced Singlet Oxygen Production for Selective Photocatalytic Oxidation
Authors: Wang Jiajia , Xu Xilong , Liu Yuanyuan , Wang Zeyan , Wang Peng , Zheng Zhaoke , Cheng Hefeng , Dai Ying , Huang Baibiao 
Published: May 2020

AbstractOxygen vacancies are usually thought to be beneficial for photogenerated charge separation. In this work, the oxygen vacancies in ov‐Bi2O3 (Bi2O3 with oxygen vacancy) were found to be able to produce 1O2 in the dark owing to chemical adsorption. The oxygen vacancies were further found to be responsible for ov‐Bi2O3 exhibiting higher 1O2 generation under light irradiation with 1O2 as the only reactive oxygen species (ROS) than Bi2O3 with 1O2, H2O2, and others as the ROS. The photocatalytic activity was investigated for the selective photo‐oxidation of phenyl methyl sulfide to phenyl methyl sulfoxide and phenyl alcohol to benzaldehyde. In either case, ov‐Bi2O3 displayed better performance than Bi2O3, suggesting the significant role of oxygen vacancies in modulating the photocatalytic oxidation properties. This work provides an alternative approach to obtain singlet oxygen, which may guide further design of photocatalysts with high efficiency and selectivity towards photocatalytic organic synthesis.
Molecular‐Level Overhaul of γ‐Aminopropyl Aminosilicone/Triethylene Glycol Post‐Combustion CO2‐Capture Solvents
Authors: Cantu David C. , Malhotra Deepika , Nguyen Manh‐Thuong , Koech Phillip K. , Zhang Difan , Glezakou Vassiliki‐Alexandra , Rousseau Roger , Page Jordan , Zheng Richard , Perry Robert J. , Heldebrant David J. 
Published: May 2020

AbstractCapturing carbon dioxide from post‐combustion gas streams is an energy‐intensive process that is required prior to either converting or sequestering CO2. Although a few commercial 1st and 2nd generation aqueous amine technologies have been proposed, the cost of capturing CO2 with these technologies remains high. One approach to decrease costs of capture has been the development of water‐lean solvents that aim to increase efficiency by reducing the water content in solution. Water‐lean solvents, such as γ‐aminopropyl aminosilicone/triethylene glycol (GAP/TEG), are promising technologies, with the potential to halve the parasitic load to a coal‐fired power plant, albeit only if high solution viscosities and hydrolysis of the siloxane moieties can be mitigated. This study concerns an integrated multidisciplinary approach to overhaul the GAP/TEG solvent system at the molecular level to mitigate hydrolysis while also reducing viscosity. Cosolvents and diluents are found to have negligible effects on viscosity and are not needed. This finding allows for the design of single‐component siloxane‐free diamine derivatives with site‐specific incorporation of selective chemical moieties for direct placement and orientation of hydrogen bonding to reduce viscosity. Ultimately, these new formulations are less susceptible to hydrolysis and exhibit up to a 98 % reduction in viscosity compared to the initial GAP/TEG formulation.
Bimetallic Pairs Supported on Graphene as Efficient Electrocatalysts for Nitrogen Fixation: Search for the Optimal Coordination Atoms
Authors: Hu Riming , Li Yongcheng , Zeng Qingwen , Wang Fuhe , Shang Jiaxiang 
Published: May 2020

AbstractThe electrocatalytic nitrogen reduction reaction (NRR) is a most attractive approach to ammonia synthesis, and the development of catalysts with excellent activity, high NRR selectivity, and long‐term durability is crucial but remains a great challenge. Herein, by means of density functional theory calculations, the stability and catalytic performance of anchored bimetals was systematically investigated by pairing different transition‐metal atoms (Mo, Cr, Ti, V, Ru, and W) on graphene with different coordination atoms (C, N, O, P, and S) for N2 fixation. By screening the stability, limiting potential, and selectivity of 105 candidates, carbon was found to be the optimal coordination atom for bimetallic pairs, whereas the other four coordination atoms were unsatisfactory owing to either thermodynamically unstable anchor sites for bimetallic pairs (O, P, and S atoms) or relatively low catalytic activity (N atom). Notably, the bimetallic compound of Mo and Ti supported on C‐coordinated graphene (MoTi‐CG) and TiV‐CG were predicted as effective NRR catalysts with the attractive limiting potentials of −0.34 and −0.30 V. Furthermore, the volcano curve between the limiting potential and the adsorption free energy of NH2* [ΔG(NH2*)] was revealed, in which a moderate ΔG(NH2*) was required for high‐activity NRR catalysts. This study not only provides a theoretical basis for the rational design of bimetallic compounds anchored on graphene as effective NRR catalysts under ambient conditions but also opens up a new way to accelerate the screening of NRR catalysts.
Photoelectrochemical Decomposition of Lignin Model Compound on a BiVO4 Photoanode
Authors: Li Tengfei , Mo Jia Yi , Weekes David M. , Dettelbach Kevan E. , Jansonius Ryan P. , Sammis Glenn M. , Berlinguette Curtis P. 
Published: May 2020

AbstractThe photoelectrochemical decomposition of lignin model compounds at a BiVO4 photoanode is demonstrated with simulated sunlight and an applied bias of 2.0 V. These prototypical lignin model compounds are photoelectrochemically converted into the corresponding aryl aldehyde and phenol derivatives in a single step with conversion of up to ≈64 % over 20 h. Control experiments suggest that vanadium sites are electrocatalytically active, which precludes the need for a redox mediator in solution. This feature of the system is corroborated by a layer of V2O5 deposited on BiVO4 serving to boost the conversion by 10 %. Our methodology capitalizes on the reactive power of sunlight to drive reactions that have only been studied previously by electrochemical or catalytic methods. The use of a BiVO4 photoanode to drive lignin model decomposition therefore provides a new platform to extract valuable aromatic chemical feedstocks using solar energy, electricity and biomass as the only inputs.
RISC32‐E: Field programmable gate array based sensor node with queue system to support fast encryption in Industrial Internet of Things applications
Authors: See Jin‐Chuan , Mok Kai‐Ming , Lee Wai‐Kong , Goh Hock‐Guan 
Published: May 2020

SummaryIndustrial Internet of Things (IIoT) is an emerging technology that relies on the use of massively connected sensor nodes to gather industrial‐related data. The collected data are used for postanalysis to generate insights for reducing production down time, cost optimization, and predictive maintenance. One of the key requirements for sensor node in such application is the data confidentiality; as such sensor data may potentially leak the manufacturing and industrial secret to their competitors. In this paper, a field programmable gate array (FPGA)‐based sensor node with Advanced Encryption Standard (AES) crypto‐processor is proposed to safeguard the sensor data. A novel queue system is proposed to further reduce the data processing time and energy consumption. The proposed queue system is able to achieve 1.48× speed up and ∼16% energy reduction, which makes it a competitive candidate for Industrial IoT applications. The technique developed in this paper can also be extended to implement FPGA‐based gateway with encryption feature, which is very useful for edge computing in IoT applications.
TAS2R20 variants confer dietary adaptation to high‐quercitrin bamboo leaves in Qinling giant pandas
Authors: Hu Xiangxu , Wang Guan , Shan Lei , Sun Shuyan , Hu Yibo , Wei Fuwen 
Published: May 2020

AbstractSensitivity to bitter tastes provides animals with an important means of interacting with their environment and thus, influences their dietary preferences. Genetic variants encoding functionally distinct receptor types contribute to variation in bitter taste sensitivity. Our previous study showed that two nonsynonymous sites, A52V and Q296H, in the TAS2R20 gene are directionally selected in giant pandas from the Qinling Mountains, which are speculated to be the causative base‐pair changes of Qinling pandas for the higher preference for bamboo leaves in comparison with other pandas. Here, we used functional expression in engineered cells to identify agonists of pTAS2R20 (i.e., giant panda's TAS2R20) and interrogated the differences in perception in the in vitro responses of pTAS2R20 variants to the agonists. Our results show that pTAS2R20 is specifically activated by quercitrin and that pTAS2R20 variants exhibit differences in the sensitivity of their response to the agonist. Compared with pTAS2R20 in pandas from other areas, the receptor variant with A52V and Q296H, which is most commonly found in Qinling pandas, confers a significantly decreased sensitivity to quercitrin. We subsequently quantified the quercitrin content of the leaves of bamboo distributed in the Qinling Mountains, which was found to be significantly higher than that of the leaves of bamboo from panda habitats in other areas. Our results suggest that the decreased sensitivity to quercitrin in Qinling pandas results in higher‐quercitrin‐containing bamboo leaves to be tasting less bitter to them and thus, influences their dietary preference. This study illustrates the genetic adaptation of Qinling pandas to their environments and provides a fine example of the functional effects of directional selection in the giant panda.
Total devastation of river macroinvertebrates following a volcanic eruption in southern Chile
Authors: Fuentes Norka , Goméz Lorna , Venegas Héctor , Rau Jaime R. 
Published: May 2020

AbstractAlthough explosive volcanic eruptions are natural disturbances that cause significant environmental repercussions and impose multiple changes on ecosystems, post‐eruption studies of rivers and streams are not common. The most recent eruption of the Puyehue‐Cordón Caulle volcanic complex (PCCVC) began on 4 June 2011 with a large explosion and the emission of a column of gas and volcanic ash (particle size <0.001–2 mm) followed by the release of silica magma, and lasted approximately until June 2012. The wind‐dispersed volcanic ash affected the area surrounding the PCCVC in southern Chile and, subsequently, most of South America, but local effects on streams and rivers in the vicinity were more drastic. We collected water, ash, and benthic macroinvertebrate samples four months after the eruption from four rivers: Two were visibly impacted (Gol‐Gol and Nilahue) in areas where volcanic ash thickness ranged between 1 and 5 cm, in the vicinity of the PCCVC fissure (8–15 km), and two adjacent rivers (Calcurrupe and Chanleufu) were located 20–40 km from the PCCVC fissure where ash thickness was <1 cm and did not present visible impacts. Results were then compared with data obtained from previous research projects. This study reports that this natural disaster induced an increase in concentrations of total suspended solids and of phosphorous in the rivers Gol‐Gol and Nilahue, as well as habitat destruction, deterioration of environmental quality, and the consequent devastation of macroinvertebrate assemblages inhabiting these rivers directly following the eruption. We conclude that volcanic eruptions can generate local extinctions of benthic macroinvertebrates in the short term, compared with rivers that were not affected by volcanic ash.