bluuebunny/crossref_metadata_2025 huggingface dataset:
Nature‐Inspired, Computer‐Assisted Optimization of Hierarchically Structured Zeolites
Authors: Coppens Marc‐Olivier , Weissenberger Tobias , Zhang Qunfeng , Ye Guanghua
Published: December 2020

Zeolite catalysis is often affected by transport limitations, which significantly influence overall performance. Introducing wide pores as molecular transport highways can reduce transport limitations, control the product distribution, and mitigate effects of catalyst deactivation. Nevertheless, the importance to rationally design the meso‐ and macropore space remains underappreciated. This article reviews multiscale modelling approaches to optimize overall catalytic performance. It provides a general methodology and rules of thumb to guide catalyst synthesis with optimal pore network characteristics. Inspiration is taken from nature, such as the structure of leaves and tissues, with similar requirements and associated features. In optimal hierarchically structured zeolites, the added macro‐/mesopore volume fraction, connectivity, crystal size, and minimum wide pore size are crucial. The broad pore size distribution is secondary. No uncontrolled diffusion limitations should exist within the zeolite crystals. Surface barriers, however, can significantly affect, even dominate overall transport. Understanding their origin and ways to control them is an emergent research area. Synthesis methods to realize hierarchically structured zeolites are briefly reviewed. Significant gaps exist between laboratory synthesis methods and industrial requirements. Zeolite catalysis could benefit from computer‐assisted design of their hierarchical pore network, embracing principles used by natural transport networks for scalable efficiency, selectivity, and robustness.
Electrogyration in Metamaterials: Chirality and Polarization Rotatory Power that Depend on Applied Electric Field
Authors: Zhang Qiang , Plum Eric , Ou Jun‐Yu , Pi Hailong , Li Junqing , MacDonald Kevin F. , Zheludev Nikolay I.
Published: December 2020

One of the most fascinating properties of chiral molecules is their ability to rotate the polarization of light. Since Faraday's experiments in 1845, it has been known that nonreciprocal polarization rotatory power can be induced by a magnetic field. But can reciprocal polarization rotation in chiral molecules be influenced by an electric field? In the 1960s, Aizu and Zheludev introduced the phenomenon of electrogyration. While the linear (Pockels) and quadratic (Kerr) electro‐optical effects describe how an external electric field changes linear birefringence and dichroism, electrogyration describes how a field changes the circular birefringence and dichroism of a medium. Electrogyration is observed in dielectrics, semiconductors, and ferroelectrics, but the effect is small. This work demonstrates a nanostructured photonic metamaterial that exhibits quadratic electrogyration—proportional to the square of the applied electric field—six orders of magnitude stronger than in any natural medium. Giant quadratic electrogyration emerges as electrostatic forces acting against forces of elasticity change the chiral configuration of the metamaterial's nanoscale building blocks and consequently its polarization rotatory power. This observation of giant electrogyration alters the perception of the effect from that of an esoteric phenomenon into a functional part of the electro‐optic toolkit with application potential.
Nitrogen‐Doping‐Regulated Electromagnetic Wave Absorption Properties of Ultralight Three‐Dimensional Porous Reduced Graphene Oxide Aerogels
Authors: Shu Ruiwen , Zhang Gengyuan , Zhang Chao , Wu Yue , Zhang Jiabin
Published: December 2020

Heteroatom nitrogen doping is considered an effective strategy to enhance the electromagnetic wave (EMW) absorption capacity of reduced graphene oxide (RGO). Herein, nitrogen‐doped RGO aerogels (NGAs) are synthesized via hydrothermal self‐assembly followed by lyophilization processes. Results of micromorphology analysis show that the as‐prepared NGAs display unique 3D porous and netlike structure. Moreover, the effects of nitrogen doping and filler contents on EMW absorption properties of NGAs are studied. The as‐synthesized NGA with nitrogen content of 9.41 at% and a bulk density of 8.7 mg cm–3 presents the integrated optimal EMW absorption performance. Specifically, the minimum reflection loss of –56.4 dB is achieved and maximum absorption bandwidth of 6.8 GHz is reached, covering the whole Ku band. In addition, the possible EMW absorption mechanisms of obtained NGAs are proposed. Therefore, the as‐synthesized NGAs can be exploited as promising high‐efficiency and lightweight EMW absorbers.
Recent Advances and Prospects of Atomic Substitution on Layered Positive Materials for Lithium‐Ion Battery
Authors: Oh Pilgun , Yun Jeongsik , Park Seohyeon , Nam Gyutae , Liu Meilin , Cho Jaephil
Published: December 2020

This work not only summarizes the previous doping research that focused on the optimization of a bulk doping composition but also introduces a new doping strategy, namely, “electrochemical reaction mechanism control doping.” The new electrochemical mechanism control technology enables the study of the precise deterioration mechanism of layered cathode materials for Li‐ion batteries (LIBs). Accordingly, tremendous efforts have been devoted to the development of various types of layered cathode materials, such as lithium‐rich, nickel‐rich, and cobalt‐rich materials, by using an electrochemical functioning doping method. This progress report also gives a perspective on potential future directions for this field. In this context, detailed methodological approaches are suggested for advanced doping studies, where the consideration of the doping method takes significance as great as designing doping configurations, e.g., chemical composition, doping depth, and doping site control, for the modification of battery material properties. As an instance of the methodological approaches for doping studies, a new “secondary doping” is shown with exemplary experimental results showing that functioning dopants (primary dopants) are homogeneously dispersed on the layered cathode materials by using supporting dopants (secondary dopants). This study will provide insights into the future direction of doping research of LIBs, as well as the history of the development of atomic substitution in layered cathode materials.
Liquid‐State Templates for Constructing B, N, Co‐Doping Porous Carbons with a Boosting of Potassium‐Ion Storage Performance
Authors: Feng Wenting , Feng Nianyun , Liu Wei , Cui Yongpeng , Chen Chen , Dong Tiantian , Liu Shuang , Deng Weiqiao , Wang Huanlei , Jin Yongcheng
Published: December 2020

Template‐assistant design and fabrication of porous carbon electrode materials has experienced great progress throughout the past decades and yielded lots of successes via various gas or solid state templates. Nevertheless, liquid‐state templates are rather rare in preparing porous carbon materials to date. In this work, melting B2O3 beads are used as both templates and a B dopant, leading to unique B, N co‐doping hierarchically porous carbons containing a “bubble pool”‐like skeleton built of interconnected carbon nanobubbles. Notably, an interesting amending effect of doped B atoms on the N‐doped carbon network can be identified for the first time, which creates a “paddy field”‐like hybrid microstructure with the co‐existence of sp2 short‐range order and sp3 defective areas, leading to an ideal model of carbon materials with both good conductivity and high capacity. Together with the rich ion diffusing pathways and the structural integrity of the “bubble pool”‐like skeleton, the resultant electrode delivers a comprehensive K‐ion storage performance. Therefore, the findings demonstrate the unique pore‐making merits of liquid state templates, which may open the door for exploring porous carbons with more innovations of microstructures and functionalities for applications in energy storage and other fields.
2D Doping of Proton Conductors: BaZrO3‐Based Heterostructures
Authors: Ngabonziza Prosper , Merkle Rotraut , Wang Yi , van Aken Peter A. , Bjørheim Tor S. , Maier Joachim , Mannhart Jochen
Published: December 2020

Ionically conducting oxide heterostructures provide ideal geometries for revealing interfacial effects in solid state ionics. Beyond that, they can provide a high density of heterointerfaces and thus allow for reliable studies of interfacial phenomena with respect to fundamental understanding as well as with respect to nanoionic applications. Substituting an entire single layer rather than random single ions by aliovalent impurities enables the possibility of 2D doping rather than conventional 0D doping. To the best of the authors’ knowledge, this technique has never been applied to ionically conducting systems. Acceptor‐doped barium zirconate has been widely investigated, particularly for applications in clean energy technologies, most importantly for intermediate temperature fuel cells. Here, epitaxial BaZrO3–BaYOx heterostructures and in particular 2D doping of BaZrO3 by yttrium are reported. The effects on proton conductivity are studied. The results not only lead to fundamental insight into the pros and cons of 2D doping of ion conductors, but may also help improve protonic devices.
Predictive model for postoperative pleural effusion after hepatectomy
Authors: Nitta Hidetoshi , Mitsuura Chisho , Shiraishi Yuta , Miyata Tatsunori , Shimizu Kenji , Harada Kazuto , Karashima Ryuichi , Masuda Toshiro , Matsumoto Katsutaka , Okino Tetsuya , Yamashita Yo‐ichi , baba Hideo , Takamori Hiroshi
Published: December 2020

Aim

Severe postoperative pleural effusion (sPOPE) after hepatectomy can lead to respiratory distress and may require thoracic drainage, leading to prolonged hospitalization. Preventive chest tube insertion may be useful for patients at high risk for sPOPE. We aimed to develop a predictive model for sPOPE after hepatectomy and evaluate indications for preventive chest tube insertion using our model.

Methods

We evaluated all patients who underwent hepatectomy from 2013 to 2020. Risk factors for sPOPE were used to develop a predictive model for sPOPE, which was validated in a cohort that received preventative chest tube placement postoperatively.

Results

A total of 325 patients were analyzed. Thirty‐one (9.5%) patients had a preventive chest tube placed at the end of their operation. Twenty‐one patients out of the remaining 294 patients developed sPOPE. Multivariate analysis identified resection containing segment 8 [relative risk (RR) 3.24, P = .022], intraoperative bleeding ≥ 500 g (RR 4.02, P = .008), intraoperative diaphragmatic incision (RR 6.96, P = .042) and open hepatectomy (RR 7.51, P = .016) as independently associated with sPOPE. The estimated probability of sPOPE ranged from 0.4% in patients with none of these factors to 73.4% in the presence of all factors. Among the 31 patients who received a preventive chest tube, more patients in the high‐risk group defined by the model had postoperative pleural effusions compared to the low‐risk group (P = .012).

Conclusion

Our predictive model for sPOPE using four risk factors allows for reliable prediction and may be useful for selection of preventive chest tube in patients undergoing hepatectomy.
Pathways to Well‐being among LGBT adults: Sociopolitical Involvement, Family Support, Outness, and Community Connectedness with Race/Ethnicity as a Moderator
Authors: Roberts Leah Marion , Christens Brian D.
Published: December 2020

People who identify as lesbian, gay, bisexual, and/or transgender (LGBT) experience disparate levels of psychological distress due to marginalization, yet there are also opportunities for community connectedness and sociopolitical involvement in identify‐specific issues and organizations, which may improve psychological well‐being. This study contributes to intersectional research on LGBT psychological well‐being by locating LGBT community connectedness as a mediator of the associations between well‐being and (a) LGBT sociopolitical involvement and (b) being out as LGBT among a sample of predominately LGBT‐identified adults in the United States and Puerto Rico (n = 4940) across four racial/ethnic identity groups: non‐Hispanic Black, Latinx/Hispanic, non‐Hispanic White, and other races/ethnicities. Analyses revealed that separate models were operating across racial/ethnic identity groups. Path analysis further showed that LGBT community connectedness mediated (either partially or fully) the effects of both LGBT sociopolitical involvement and outness on well‐being. Direct effects on well‐being were also found for family support across all groups and for outness only among the non‐Hispanic White and other races/ethnicities groups. Community leaders and practitioners should seek to create opportunities for LGBT sociopolitical involvement and other activities that may facilitate feeling connected to LGBT community as part of efforts to promote LGBT well‐being.
Synthesis, structural characterization, and biological studies of ATBS–M complexes (M(II) = Cu, Co, Ni, and Mn): Access for promising antibiotics and anticancer agents
Authors: Ismael Mohamed , Abdel‐Rahman Laila H. , Abou El‐ezz Doaa , Ahmed Ebtehal A.‐H. , Nafady Ayman
Published: December 2020

A new bidentate Schiff base ligand (ATBS [4‐bromo‐2‐(thiazole‐2‐yliminomethyl)phenol]) was synthesized via the condensation reaction of 2‐aminothiazole with 5‐bromosalicylaldehyde in ethanol. The reaction of ATBS with transition metal salts of Cu(II), Co(II), Ni(II), and Mn(II) afforded the corresponding ATBS–M complexes. Results from physicochemical and spectral analyses, such as elemental analysis, infrared, UV–Vis spectroscopy, magnetic susceptibility, and molar conductance, revealed a nonelectrolytic nature with octahedral (Oh) geometry and a metal/ligand ratio of 1:2 for Cu(II), Co(II), and Ni(II), but 1:1 for the Mn(II) complex. The density functional theory (DFT) calculations are correlated very well with the proposed structure and molecular geometry of the complexes as [M(ATBS)2] (M = Cu, Co, and Ni) and [Mn(ATBS)(H2O)2]. Significantly, the prepared compounds showed strong inhibition activity for a wide spectrum of bacteria (Escherichia coli, Bacillus subtilis, and Staphylococcus aureus) and fungi (Candida albicans, Aspergillus flavus, and Trichophyton rubrum), with the ATBS–Ni complex being the most promising antibiotic agent. Molecular docking studies of the binding interaction between the title complexes with the bacterial protein receptor CYP51 revealed clear insights about the inhibition nature against the studied microorganisms, with the following order: ATBS–Cu > ATBS–Mn > ATBS–Ni > ATBS–Co for complex stability. Moreover, the cytotoxicity measurements of all prepared metal complexes against the colon carcinoma (HCT‐116) and hepatocellular carcinoma (Hep‐G2) cell lines showed exceptional anticancer efficacy of the complexes as compared with the free ATBS Schiff base ligand. Significantly, the results attested that ATBS–Cu is the most effective complex against HCT‐116 cells, whereas ATBS–Mn has the highest cytotoxic efficiency against Hep‐G2 cells. Furthermore, electronic spectra, viscosity measurements, and gel electrophoresis techniques were employed to probe the interaction of all prepared ATBS–metal complexes with calf thymus (CT)‐DNA. Results confirmed that all complexes are strongly bound to CT‐DNA via intercalation mode, with the ATBS–Co complex having the highest binding ability.
Bifunctional Catalysts Containing Zn(II) and Imidazolium Salt Ionic Liquids for Chemical Fixation of Carbon Dioxide
Authors: Shang Hui , Bai Shiyang , Yao Jie , Ma Shuangshuang , Sun Jihong , Su Hongjing , Wu Xia
Published: December 2020

Zn(II) can efficiently promote the catalytic performance of imidazolium salt ionic liquids (imi‐ILs) for the chemical fixation of CO2 into epoxides. To obtain sustainability, immobilized bifunctional catalysts containing both imi‐ILs and Zn(II) were prepared using bimodal mesoporous silica (BMMs) as carrier, through grafting of Zn(OAc)2 and 1‐(trimethoxysilyl)propyl‐3‐methylimidazolium chloride (Si‐imi) separately in the nanopores. The catalysts, named as BMMs−Zn&ILs, were identified as efficient catalysts for cycloaddition reaction of CO2 into epoxides under solvent‐free conditions. BMMs−Zn&ILs showed good catalytic activity, which increased with the increase of the molar ratio of Zn(II) to Si‐imi. As a comparison, different catalytic systems including homogeneous imi‐IL, BMMs‐ILs and BMMs−Zn were studied to demonstrate different cooperation behaviors. Furthermore, the kinetics studies of homogeneous and heterogeneous bifunctional catalysts were employed to confirm the differences, as well as to support the proposed cooperative catalysis mechanism in the nanopores.
Modelle zur Vorhersage des Schwindens und Kriechens von Beton
Authors: Müller Harald S. , Acosta Urrea Fernando , Kvitsel Vladislav
Published: December 2020

Im Herbst dieses Jahres wurde die Überarbeitung der EN 1992‐1‐1:2004 (Eurocode 2) abgeschlossen und damit der Entwurf prEN 1992‐1‐1:2020 vorgelegt. Er stellt der Praxis zahlreiche neue und bessere Konzepte und Modelle zur Verfügung. Dies gilt auch für die Modelle zum Kriechen und Schwinden von Konstruktionsbeton, die zum Teil erhebliche Veränderungen erfahren haben. In diesem zweiteiligen Aufsatz (Teil 1 Schwinden, Teil 2 Kriechen) werden die neuen Modelle zur Prognose des Verformungsverhaltens von Beton vorgestellt. Er beleuchtet auch die Hintergründe, die zur Entwicklung der verbesserten Ansätze geführt haben.

Dieser Beitrag befasst sich mit dem Schwinden von Beton. In einem Überblick werden zunächst die wesentlichen Schwindarten und ihre Merkmale dargestellt. Danach werden die normativen Entwicklungen aufgezeigt, die zum heute gültigen Schwindmodell in DIN EN 1992‐1‐1:2011 geführt haben. Im Mittelpunkt steht die Analyse der Zuverlässigkeit und Genauigkeit dieses Modells. Sie ergab erhebliche Defizite, die Anlass für eine wesentliche Korrektur und Weiterentwicklung im Zuge der Erarbeitung der prEN 1992‐1‐1:2020 waren. Zahlreiche Untersuchungsergebnisse untermauern den neuen Ansatz, der hier vorgestellt und begründet wird. Statistische Betrachtungen zur Zuverlässigkeit des neuen Modells und die Darstellung eines Konzepts für den Einbezug von Laborversuchsdaten zur Verbesserung des Modells bilden den Abschluss des Beitrags.
Single‐Molecule Sensing by Grating‐based Spectrally Resolved Super‐Resolution Microscopy
Authors: Kim Geun‐ho , Chung Jinkyoung , Park Hyunbum , Kim Doory
Published: December 2020

Recent advances in single‐molecule spectroscopic imaging techniques, such as spectrally resolved stochastic optical reconstruction microscopy (SR‐STORM), have been effective for obtaining detailed spectral information at the molecular level. However, its application for single‐molecule sensing is highly challenging owing to its complicated configuration and limited spectral information. In this study, we demonstrated single‐molecule polarity sensing by combining grating‐based SR‐STORM with the solvatochromic dye, Nile red. The spatial and spectral resolutions of the custom‐built grating‐based SR‐STORM were examined for various color ranges of fluorescent dyes, and this approach was successfully applied for sensing nanoscale local polarity of various organic solvent molecules and surfactant molecules. Furthermore, we demonstrated that the proposed method effectively distinguished the different polarities of functional groups within surfactant molecules at the single‐molecule level. We anticipate that the proposed approach can be combined with other chromic molecules for application to many other chemical systems.
Do financial penalties for environmental violations facilitate improvements in corporate environmental performance? An empirical investigation
Authors: Shevchenko Anton
Published: December 2020

Environmental regulations play an essential role in managing firm behavior and providing a reference point for the minimum standards of corporate environmental performance, yet certain firms fail to ensure their environmental performance meets these standards. This research focuses on public firms that the US government has penalized for violating environmental regulations and investigates whether these firms subsequently improved their environmental performance. Surprisingly, neither the receipt of a penalty for an environmental violation nor the imposition of a greater penalty was associated with improvements in environmental performance. Instead, a penalty for environmental violation predicted further, albeit mild, deterioration in environmental performance. While the existing literature has established that financial penalties deter most firms from committing environmental violations, this research contributes to this literature by revealing that these penalties fail to motivate firms that have violated environmental regulations to improve their environmental performance.
Looking for sustainable development: Socially responsible mutual funds and the low‐carbon economy
Authors: Soler‐Domínguez Amparo , Matallín‐Sáez Juan Carlos , de Mingo‐López Diego Víctor , Tortosa‐Ausina Emili
Published: December 2020

Sustainable investment responds to demands for carbon and climate‐neutral societies. To address the urgency around climate change and provide investors with more qualified information, Morningstar has developed the Low Carbon Designation (LCD) to indicate that the companies held in a portfolio are in general alignment with the transition to a low‐carbon economy. The designation is given to portfolios that have low carbon risk and fossil fuel exposure scores. The present study builds on the LCD by examining the relationship between these scores and financial performance. With this aim, we analyze 3920 socially responsible mutual funds from across the world. Results show differences in financial performance according to scores and investment areas. We find evidence that funds considered to have higher levels of sustainability achieved better performance than funds with higher exposure to companies involved in carbon and fossil fuel industries. We provide insights on the informativeness of these new scores with a focus on climate change and their relevance in helping investors to identify climate‐aware funds. This study highlights the importance of introducing strategies to develop green finance; the analysis confirms that sustainability improves performance. Finally, the LCD indicator is shown to be relevant for making fairer comparisons among socially responsible funds and, ultimately, for developing low‐carbon economies.
Consequences of canceling elective invasive cardiac procedures during Covid‐19 outbreak
Authors: Moreno Raúl , Díez José‐Luis , Diarte José‐Antonio , Macaya Fernando , de la Torrre Hernández José‐María , Rodríguez‐Leor Oriol , Trillo Ramiro , Alonso‐Briales Juan , Amat‐Santos Ignacio , Romaguera Rafael , Díaz José‐Francisco , Vaquerizo Beatriz , Ojeda Soledad , Cruz‐González Ignacio , Morena‐Salas Daniel , Pérez de Prado Armando , Sarnago Fernando , Portero Pilar , Gutierrez‐Barrios Alejandro , Alfonso Fernando , Bosch Eduard , Pinar Eduardo , Ruiz‐Arroyo José‐Ramón , Ruiz‐Quevedo Valeriano , Jiménez‐Mazuecos Jesús , Lozano Fernando , Rumoroso José‐Ramón , Novo Enrique , Irazusta Francisco J , García del Blanco Bruno , Moreu José , Ballesteros‐Pradas Sara M , Frutos Araceli , Villa Manuel , Alegría‐Barrero Eduardo , Lázaro Rosa , Paredes Emilio
Published: December 2020

Background

During COVID‐19 pandemic in Spain, elective procedures were canceled or postponed, mainly due to health care systems overwhelming.

Objective

The objective of this study was to evaluate the consequences of interrupting invasive procedures in patients with chronic cardiac diseases due to the COVID‐19 outbreak in Spain.

Methods

The study population is comprised of 2,158 patients that were pending on elective cardiac invasive procedures in 37 hospitals in Spain on the 14th of March 2020, when a state of alarm and subsequent lockdown was declared in Spain due to the COVID‐19 pandemic. These patients were followed‐up until April 31th.

Results

Out of the 2,158 patients, 36 (1.7%) died. Mortality was significantly higher in patients pending on structural procedures (4.5% vs. 0.8%, respectively; p < .001), in those >80 year‐old (5.1% vs. 0.7%, p < .001), and in presence of diabetes (2.7% vs. 0.9%, p = .001), hypertension (2.0% vs. 0.6%, p = .014), hypercholesterolemia (2.0% vs. 0.9%, p = .026) [Correction added on December 23, 2020, after first online publication: as per Dr. Moreno's request changes in p‐values were made after original publication in Abstract.], chronic renal failure (6.0% vs. 1.2%, p < .001), NYHA > II (3.8% vs. 1.2%, p = .001), and CCS > II (4.2% vs. 1.4%, p = .013), whereas was it was significantly lower in smokers (0.5% vs. 1.9%, p = .013). Multivariable analysis identified age > 80, diabetes, renal failure and CCS > II as independent predictors for mortality.

Conclusion

Mortality at 45 days during COVID‐19 outbreak in patients with chronic cardiovascular diseases included in a waiting list due to cancellation of invasive elective procedures was 1.7%. Some clinical characteristics may be of help in patient selection for being promptly treated when similar situations happen in the future.
Steric Effects in the Catalytic Tandem Isomerization‐Hydrosilylation Reaction
Authors: Prieto Unai , Azpeitia Susan , Sebastian Eider San , Freixa Zoraida , Garralda María A. , Huertos Miguel A.
Published: December 2020

The selective synthesis of linear silanes from remote alkenes is reported. Four new silane‐thioether bidentate proligands [SiMe2H(o‐C6H4SR)] (R=iBu, pentyl, benzyl, neopentyl) have been synthesized and used to form unsaturated and cationic 16‐electron hydrido‐silyl‐RhIII complexes. These compounds are efficient catalysts for the tandem catalytic alkene isomerization‐hydrosilylation reaction at room temperature under solvent‐free conditions. The different size of the substituent on the sulfur atom results on a difference in the activity of this tandem reaction. Experimental observations demonstrate that the isomerization process is the rate‐determining step of this catalytic transformation. This process would be of value to the chemical industry because mixtures of internal aliphatic olefins are substantially cheaper and more readily available than the pure terminal isomers.
Organocatalyzed C−N bond‐forming Reactions for the Synthesis of Amines and Amides
Authors: Upadhyay Rahul , Rana Rohit , Maurya Sushil K.
Published: December 2020

The synthesis of organonitrogen compounds via C−N bond formation emerges as a versatile route for drug discovery. Most of the pharmaceuticals and natural products, which are predominantly used generally contain amine functionalities and amide linkages in their structure. Traditionally, the synthesis is done by using several metal catalysts and hazardous chemicals. The organocatalyzed synthetic protocol provides a sustainable and eco‐compatible route for the synthesis of organonitrogen compounds and at the same time also avoids metal contamination. The main aim of this Review is to provide an overview of the organocatalyzed amine and amide synthesis via C−N bond formation reactions. We hope this Review provides valuable information about the organocatalyzed reaction to enable the development of more sustainable routes to form these linkages.
Mesoporous NiFe2O4 with Tunable Pore Morphology for Electrocatalytic Water Oxidation
Authors: Simon Christopher , Timm Jana , Tetzlaff David , Jungmann Jonas , Apfel Ulf‐Peter , Marschall Roland
Published: December 2020

Mesoporous NiFe2O4 for electrocatalytic water splitting was prepared via soft‐templating using citric‐acid‐complexed metal nitrates as precursors. The mesopore evolution during thermal treatment was examined systematically giving insights into the formation process of mesoporous NiFe2O4. Detailed nitrogen physisorption analysis including desorption scanning experiments reveal the presence of highly accessible mesopores generating surface areas of up to 200 m2/g. The ability of the NiFe2O4 powders to perform electrocatalytic oxygen evolution reaction under alkaline conditions was investigated, highlighting the advantages of mesopore insertion. The most active samples reach a current density of 10 mA cm−2 at an overpotential of 410 mV with a small Tafel slope of 50 mV dec−1, indicating an enhanced activity that originated from the increased catalyst surface.
Effect of Electrolyte Composition and Concentration on Pulsed Potential Electrochemical CO2 Reduction
Authors: Casebolt Rileigh , Kimura Kevin W. , Levine Kelsey , Cimada DaSilva Jessica Akemi , Kim Jiyoon , Dunbar Tyler A. , Suntivich Jin , Hanrath Tobias
Published: December 2020

With rising CO2 emissions and growing interests towards CO2 valorization, electrochemical CO2 reduction (eCO2R) has emerged as a promising prospect for carbon recycling and chemical energy storage. Yet, product selectivity and electrocatalyst longevity persist as obstacles to the broad implementation of eCO2R. A possible solution to ameliorate this challenge is to pulse the applied potential. However, it is currently unclear whether and how the trends and lessons obtained from the more conventional constant potential eCO2R translate to pulsed potential eCO2R. In this work, we report that the relationship between electrolyte concentration/composition and product distribution for pulsed potential eCO2R is different from constant potential eCO2R. In the case of constant potential eCO2R, increasing KHCO3 concentration favors the formation of H2 and CH4. In contrast, for pulsed potential eCO2R, H2 formation is suppressed due to the periodic desorption of surface protons, while CH4 is still favored. In the case of KCl, increasing the concentration during constant potential eCO2R does not affect product distribution, mainly producing H2 and CO. However, increasing KCl concentration during pulsed potential eCO2R persistently suppresses H2 formation and greatly favors C2 products, reaching 71 % Faradaic efficiency. Collectively, these results provide new mechanistic insights into the pulsed eCO2R mechanism within the context of proton‐donator ability and ionic conductivity.
NiFeMo Nanoparticles Encapsulated within Nitrogen‐Doped Reduced Graphene Oxide as Bifunctional Electrocatalysts for Zinc‐Air Batteries
Authors: Zeng Wenwen , Wei Chaohui , Zeng Kai , Cao Xuecheng , Rümmeli Mark H. , Yang Ruizhi
Published: December 2020

Rechargeable metal‐air batteries (MABs) have emerged as promising candidates for portable energy storage technologies because of their favorable energy/power density, safety, and cost‐effectiveness. However, the lack of advanced bifunctional electrocatalysts for the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) restricts the commercial realization of rechargeable MABs. Herein, we developed a facile fabrication route to prepare N‐doped graphene oxide encapsulating nanoparticles of a ternary NiFe metal oxide (NiFeMo@N‐rGO) serving as an efficient bifunctional catalyst. The obtained NiFeMo@N‐rGO bifunctional catalyst demonstrates a comparable catalytic reactivity when compared to precious metal catalysts in alkaline electrolytes regarding ORR/OER performance (ORR: half‐wave potential of 0.82 V; OER: overpotential of 330 mV; ▵E: 0.73 V at 10 mA cm−2). The assembled zinc‐air batteries (ZABs) catalyzed by NiFeMo@N‐rGO exhibit a high power density of 120 mW cm−2 and a capacity of 721 mAh gZn−1, coupled with long‐term durability of over 200 h. This contribution paves a practical avenue to prepare efficient bifunctional catalysts for superior ZABs.
Fluidization of fine lactose for dry powder inhalation: A comparison of assisting methods
Authors: Zhang Fuweng , La Zara Damiano , Sun Feilong , Quayle Michael J. , Petersson Gunilla , Folestad Staffan , van Ommen J. Ruud
Published: December 2020

Fluidization of cohesive pharmaceutical powders is difficult to achieve and typically requires the introduction of external forces. This study investigates the fluidization of the fine inhalation grade of lactose powders (size range from 0.1‐20 μm) that are specifically developed for dry powder inhalation (DPI) applications. The fluidization behaviour of fine lactose powders was evaluated under six conditions: without fluidization aids, with only vertical vibration (VFA), with only a downward‐pointing micro‐jet (MFA), with both vibration and pre‐mixing with coarse particles (VCFA), with both vibration and micro‐jet (VMFA), and with the combined assistance of vibration, micro‐jet, and addition of coarse particles (VMCFA). The enhancement of fluidization due to the use of different assistance methods is reflected by the increase of bed expansion and the decrease in both the minimum fluidization velocity and agglomerate formation. However, applying micro‐jet results in considerable powder losses due to the high fraction of fine particles stuck to the wall. Combining any two assisting methods leads to better fluidization than using a single approach. In particular, the combination of vibration and micro‐jet shows the best performance in improving fluidization. Further addition of coarse particles does not play a significant influence on promoting fluidization. Finally, the analysis of the forces acting on the lactose agglomerates shows the enhancement of separation forces by introducing the fluidization assistance, which leads to a decrease in agglomerate size.
Synthesis of σ Receptor Ligands with a Spirocyclic System Connected with a Tetrahydroisoquinoline Moiety via Different Linkers
Authors: Bergkemper Melanie , Schepmann Dirk , Wünsch Bernhard
Published: December 2020

With the aim to develop new σ2 receptor ligands, spirocyclic piperidines or cyclohexanamines with 2‐benzopyran and 2‐benzofuran scaffolds were connected to the 6,7‐dimethoxy‐1,2,3,4‐tetrahydroisoquinoline moiety by variable linkers. In addition to flexible alkyl chains, linkers containing an amide as functional group were synthesized. The 2‐benzopyran and 2‐benzofuran scaffold of the spirocyclic compounds were synthesized from 2‐bromobenzaldehyde. The amide linkers were constructed by acylation of amines with chloroacetyl chloride and subsequent nucleophilic substitution, the alkyl linkers were obtained by LiAlH4 reduction of the corresponding amides. For the development of σ2 receptor ligands, the spirocyclic 2‐benzopyran scaffold is more favorable than the ring‐contracted 2‐benzofuran system. Compounds bearing an alkyl chain as linker generally show higher σ affinity than acyl linkers containing an amide as functional group. A higher σ1 affinity for the cis‐configured cyclohexanamines than for the trans‐configured derivatives was found. The highest σ2 affinity was observed for cis‐configured spiro[[2]benzopyran‐1,1′‐cyclohexan]‐4′‐amine connected to the tetrahydroisoquinoline system by an ethylene spacer (cis‐31, Ki (σ2)=200 nM; the highest σ1 affinity was recorded for the corresponding 2‐benzofuran derivative with a CH2C=O linker (cis‐29, Ki (σ1)=129 nM).
The inheritance and creative design of traditional color scheme based on modern consumer's psychological perception: Taking Chinese traditional decorative pattern's color collocation as an example
Authors: Xu Bing
Published: December 2020

Color in traditional decorative patterns is one of the most important characteristics that can not only be easily identified, but also be taken as a specific symbol of one country or nation. As most of the traditional color schemes are based on ancient aesthetics and wisdom, in order to make them more in line with the aesthetic cognition of modern consumers, an innovation of traditional color schemes is very necessary. This article conducted an experiment to test modern consumers' psychological perception towards different traditional color combinations based on PAD three‐dimensional model and SAM measurement scale. Then the computer image recognition technology and mathematical modeling were applied to establish the relationship between different psychological perceptions and traditional color schemes to guide further design. It was found that some colors have a positive effect on consumers' preference, while some others can reduce consumers' preference; certain color combinations convey feelings of joy or warmth; the appropriate use of high saturation and moderate value colors have more attractions for consumers. Based on the results, new combination schemes for traditional colors were presented, so as to realize the creative design of traditional colors based on the psychological perception of modern consumers.
Hydrogen Production from Methanol‐Water Mixture over Immobilized Iridium Complex Catalysts in Vapor‐Phase Flow Reaction
Authors: Yamaguchi Sho , Maegawa Yoshifumi , Fujita Ken‐ichi , Inagaki Shinji
Published: December 2020

CO‐free hydrogen production from methanol and water by using transition metal complex catalysts has attracted increasing attention. However, liquid‐phase batch reactions using homogeneous catalysts are impractical for large‐scale operations, owing to the consumption of bases and the use of organic solvents or additives. This study concerns a novel method for continuous hydrogen production from a simple methanol‐water solution under vapor‐phase flow. The reaction is catalyzed by an anionic iridium bipyridonate (Ir‐bpyd) complex immobilized on a periodic mesoporous organosilica. The liquid‐phase batch reaction using homogeneous anionic Ir‐bpyd complex is immediately deactivated, owing to CO2 generation, whereas no catalyst deactivation is observed in the vapor‐phase flow reaction because CO2 is smoothly removed from the catalyst bed, enabling continuous hydrogen production without the addition of a base. Thus, the critical problems pertaining to homogeneous catalysts are overcome.
Numerical study of penetration and distribution of charged particles in the magnetosphere during southward IMF case
Authors: Esmaeili Amin , Kalaee Mohammad Javad , Ikram M.
Published: December 2020

The energetic charged particles penetration in the plasmasphere are carried out using the updated version of 3D Stanford PIC code. We considered slow and fast wind streams to know the penetration of the energetic charged particles (electrons and ions) having different velocities into four regions i.e. cusp, plasmasphere, sunward, and tailward sides. It is observed that the ion penetrations are higher than electrons for solar slow wind streams in the plasmasphere, while it is reverse for the solar fast streams. Also, the results show that the percentage of penetration of the energetic charged particles (both electrons and ions) are the same into the cusp and subsolar point reconnection region. It is different for the higher speed of fast streams; so that the penetrated electrons reached about 10–20 times than penetrated ions. The results show that for the tailward reconnection region, the penetration of ions is 2–3 times higher than the penetration of electrons, but it is the same for the case of higher solar fast speed.
Clustering of loci controlling species differences in male chemical bouquets of sympatric Heliconius butterflies
Authors: Byers Kelsey J. R. P. , Darragh Kathy , Fernanda Garza Sylvia , Abondano Almeida Diana , Warren Ian A. , Rastas Pasi M. A. , Merrill Richard M. , Schulz Stefan , McMillan W. Owen , Jiggins Chris D.
Published: December 2020

The degree to which loci promoting reproductive isolation cluster in the genome—that is, the genetic architecture of reproductive isolation—can influence the tempo and mode of speciation. Tight linkage between these loci can facilitate speciation in the face of gene flow. Pheromones play a role in reproductive isolation in many Lepidoptera species, and the role of endogenously produced compounds as secondary metabolites decreases the likelihood of pleiotropy associated with many barrier loci. Heliconius butterflies use male sex pheromones to both court females (aphrodisiac wing pheromones) and ward off male courtship (male‐transferred antiaphrodisiac genital pheromones), and it is likely that these compounds play a role in reproductive isolation between Heliconius species. Using a set of backcross hybrids between H. melpomene and H. cydno, we investigated the genetic architecture of putative male pheromone compound production. We found a set of 40 significant quantitative trait loci (QTL) representing 33 potential pheromone compounds. QTL clustered significantly on two chromosomes, chromosome 8 for genital compounds and chromosome 20 for wing compounds, and chromosome 20 was enriched for potential pheromone biosynthesis genes. There was minimal overlap between pheromone QTL and known QTL for mate choice and color pattern. Nonetheless, we did detect linkage between a QTL for wing androconial area and optix, a color pattern locus known to play a role in reproductive isolation in these species. This tight clustering of putative pheromone loci might contribute to coincident reproductive isolating barriers, facilitating speciation despite ongoing gene flow.
Design parameters and material‐scale damage evolution of seismic upgraded RC frames by viscoelastic haunch bracing‐dampers
Authors: Dong Yao‐Rong , Xu Zhao‐Dong , Li Qiang‐Qiang , Zhu Chen , He Zhen‐Hua
Published: December 2020

To improve the seismic design of reinforced concrete (RC) frame structures and upgrade existing RC frame structures that have insufficient seismic design, a new suitable seismic upgraded solution, the installation of viscoelastic haunch bracing‐dampers (VHBD) to increase the seismic performance of RC frames, is proposed in this paper. For a comprehensive and systematical research about this new upgraded frames system, a comparative study on the seismic performance between 15 RC frame structure specimens by adding the VHBD with different design parameters and one common RC frame structure specimen is performed under sinusoidal dynamic loading. The specific items of seismic performance mainly include hysteresis performance, load‐bearing capacity, stiffness degradation, energy dissipation capacity, and additional damping ratio, and so on. First, on the basic of this, the material‐scale damage evolution of structure specimens at each stage is qualitatively analyzed. Then, six reasonable material‐scale damage indexes that can describe the damage evolution of the structures precisely are proposed. Finally, a quantitative comparative analysis on the material‐scale damage evolution of structure specimens in the whole process is carried out under different design parameters. The research results indicate that the upgraded scheme (reasonable design parameters of and ) proposed in this study can improve the seismic performance of RC frame structures to the appropriate level required for the design, in terms of load‐bearing capacity, stiffness, energy dissipation capacity, and damping ratio. At the same time, the failure mode of the structures can be well controlled. The occurred damage at beam‐column joints is reasonably transferred to the beam area, which can guarantee the seismic design requirements of “strong joints and weak components.”
Genetic algorithm‐based ground motion selection method matching target distribution of generalized conditional intensity measures
Authors: Ji Kun , Wen Ruizhi , Zong Chengcai , Ren Yefei
Published: December 2020

This study developed an approach for selecting sets of ground motion recordings that match a target conditional multivariate distribution of ground motion intensity measures (IMs). This was achieved by applying a genetic algorithm (GA) that treats IMs of interest of each recording as a “chromosome” and the set of the desired number of recordings as a single “individual.” The fitness function was constructed by measuring the mismatch between the target and the individual's means and variances for all IMs. Then, through Roulette wheel natural parent selection, one‐point chromosome crossover, and individual mutation, new generations of ground motion sets were produced and the process was continued until the optimum combination of recordings was obtained. Example application illustrated that the proposed GA method could efficiently search and find a desired number of recordings to represent the target conditional IMs’ distribution, including the mean and variance. The IMs considered included response spectrum (range: 0.05‐10.0 s), amplitude/intensity‐based IMs, cumulative‐based IMs, and duration. Comparison with existing GCIM selection method indicated that the standard deviation of the recordings selected using the proposed GA method was closer to the target and more stable among replications. The results demonstrated that the proposed GA method represents a promising approach for searching pairs of recordings that could simultaneously match the target conditional distribution of various IMs.
Case Study in 21st Century Ecotoxicology: Using In Vitro Aromatase Inhibition Data to Predict Short-Term In Vivo Responses in Adult Female Fish
Authors: Villeneuve Daniel L. , Blackwell Brett R. , Cavallin Jenna E. , Cheng Wan-Yun , Feifarek David J. , Jensen Kathleen M. , Kahl Michael W. , Milsk Rebecca Y. , Poole Shane T. , Randolph Eric C. , Saari Travis W. , Ankley Gerald T.
Published: December 2020

The present study evaluated whether in vitro measures of aromatase inhibition as inputs into a quantitative adverse outcome pathway (qAOP) construct could effectively predict in vivo effects on 17β-estradiol (E2) and vitellogenin (VTG) concentrations in female fathead minnows. Five chemicals identified as aromatase inhibitors in mammalian-based ToxCast assays were screened for their ability to inhibit fathead minnow aromatase in vitro. Female fathead minnows were then exposed to 3 of those chemicals: letrozole, epoxiconazole, and imazalil in concentration–response (5 concentrations plus control) for 24 h. Consistent with AOP-based expectations, all 3 chemicals caused significant reductions in plasma E2 and hepatic VTG transcription. Characteristic compensatory upregulation of aromatase and follicle-stimulating hormone receptor (fshr) transcripts in the ovary were observed for letrozole but not for the other 2 compounds. Considering the overall patterns of concentration–response and temporal concordance among endpoints, data from the in vivo experiments strengthen confidence in the qualitative relationships outlined by the AOP. Quantitatively, the qAOP model provided predictions that fell within the standard error of measured data for letrozole but not for imazalil and epoxiconazole. However, the inclusion of measured plasma concentrations of the test chemicals as inputs improved model predictions, with all predictions falling within the range of measured values. Results highlight both the utility and limitations of the qAOP and its potential use in 21st century ecotoxicology. Environ Toxicol Chem 2021;40:1155–1170. © 2020 SETAC. This article has been contributed to by US Government employees and their work is in the public domain in the USA.

Abstract
Non‐linear mixed‐effects models for time series forecasting of smart meter demand
Authors: Roach Cameron , Hyndman Rob , Ben Taieb Souhaib
Published: December 2020

Buildings are typically equipped with smart meters to measure electricity demand at regular intervals. Smart meter data for a single building have many uses, such as forecasting and assessing overall building performance. However, when data are available from multiple buildings, there are additional applications that are rarely explored. For instance, we can explore how different building characteristics influence energy demand. If each building is treated as a random effect and building characteristics are handled as fixed effects, a mixed‐effects model can be used to estimate how characteristics affect energy usage. In this paper, we demonstrate that producing 1‐day‐ahead demand predictions for 123 commercial office buildings using mixed models can improve forecasting accuracy. We experiment with random intercept, random intercept and slope and non‐linear mixed models. The predictive performance of the mixed‐effects models are tested against naive, linear and non‐linear benchmark models fitted to each building separately. This research justifies using mixed models to improve forecasting accuracy and to quantify changes in energy consumption under different building configuration scenarios.