bluuebunny/crossref_metadata_2025_split huggingface dataset:
Pre‐Buried Additive for Cross‐Layer Modification in Flexible Perovskite Solar Cells with Efficiency Exceeding 22%
Authors: Zheng Zhonghao , Li Faming , Gong Jue , Ma Yinyi , Gu Jinwen , Liu Xiaochun , Chen Shuhan , Liu Mingzhen 
Published: April 2022

AbstractHalide perovskites have shown superior potentials in flexible photovoltaics due to their soft and high power‐to‐weight nature. However, interfacial residual stress and lattice mismatch due to the large deformation of flexible substrates have greatly limited the performance of flexible perovskite solar cells (F‐PSCs). Here, ammonium formate (HCOONH4) is used as a pre‐buried additive in electron transport layer (ETL) to realize a bottom‐up infiltration process for an in situ, integral modification of ETL, perovskite layer, and their interface. The HCOONH4 treatment leads to an enhanced electron extraction in ETL, relaxed residual strain and micro‐strain in perovskite film, along with reduced defect densities within these layers. As a result, a top power conversion efficiency of 22.37% and a certified 21.9% on F‐PSCs are achieved, representing the highest performance reported so far. This work links the critical connection between multilayer mechanics/defect profiles of ETL‐perovskite structure and device performance, thus providing meaningful scientific direction to further narrowing the efficiency gap between F‐PSCs and rigid‐substrate counterparts.
Electronic Structure Engineering of Single‐Atom Ru Sites via Co–N4 Sites for Bifunctional pH‐Universal Water Splitting
Authors: Rong Chengli , Shen Xiangjian , Wang Yuan , Thomsen Lars , Zhao Tingwen , Li Yibing , Lu Xunyu , Amal Rose , Zhao Chuan 
Published: April 2022

AbstractThe development of bifunctional water‐splitting electrocatalysts that are efficient and stable over a wide range of pH is of great significance but challenging. Here, an atomically dispersed Ru/Co dual‐sites catalyst is reported anchored on N‐doped carbon (Ru/Co–N–C) for outstanding oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) in both acidic and alkaline electrolytes. The Ru/Co–N–C catalyst requires the overpotential of only 13 and 23 mV for HER, 232 and 247 mV for OER to deliver a current density of 10 mA cmgeo−2 in 0.5 m H2SO4 and 1 m KOH, respectively, outperforming benchmark catalysts Pt/C and RuO2. Theoretical calculations reveal that the introduction of Co–N4 sites into Ru/Co–N–C efficiently modify the electronic structure of Ru by enlarging Ru–O covalency and increasing Ru electron density, which in turn optimize the bonding strength between oxygen/hydrogen intermediate species with Ru sites, thereby enhancing OER and HER performance. Furthermore, the incorporation of Co–N4 sites induces electron redistribution around Ru–N4, thus enhancing corrosion–resistance of Ru/Co–N–C during acid and alkaline electrolysis. The Ru/Co–N–C has been applied in a proton exchange membrane water electrolyzer and steady operation is demonstrated at a high current density of 450 mA cmgeo−2 for 330 h.
Liquid Crystal Elastomer with Integrated Soft Thermoelectrics for Shape Memory Actuation and Energy Harvesting
Authors: Zadan Mason , Patel Dinesh K. , Sabelhaus Andrew P. , Liao Jiahe , Wertz Anthony , Yao Lining , Majidi Carmel 
Published: April 2022

AbstractLiquid crystal elastomers (LCEs) have attracted tremendous interest as actuators for soft robotics due to their mechanical and shape memory properties. However, LCE actuators typically respond to thermal stimulation through active Joule heating and passive cooling, which make them difficult to control. In this work, LCEs are combined with soft, stretchable thermoelectrics to create transducers capable of electrically controlled actuation, active cooling, and thermal‐to‐electrical energy conversion. The thermoelectric layers are composed of semiconductors embedded within a 3D printed elastomer matrix and wired together with eutectic gallium–indium (EGaIn) liquid metal interconnects. This layer is covered on both sides with LCE, which alternately heats and cools to achieve cyclical bending actuation in response to voltage‐controlled Peltier activation. Moreover, the thermoelectric layer can harvest energy from thermal gradients between the two LCE layers through the Seebeck effect, allowing for regenerative energy harvesting. As demonstrations, first, closed‐loop control of the transducer is performed to rapidly track a changing actuator position. Second, a soft robotic walker that is capable of walking toward a heat source and harvesting energy is introduced. Lastly, phototropic‐inspired autonomous deflection of the limbs toward a heat source is shown, demonstrating an additional method to increase energy recuperation efficiency for soft systems.
Classical Complement Pathway Inhibition in a “Human‐On‐A‐Chip” Model of Autoimmune Demyelinating Neuropathies
Authors: Rumsey John W. , Lorance Case , Jackson Max , Sasserath Trevor , McAleer Christopher W. , Long Christopher J. , Goswami Arindom , Russo Melissa A. , Raja Shruti M. , Gable Karissa L. , Emmett Doug , Hobson‐Webb Lisa D. , Chopra Manisha , Howard James F. , Guptill Jeffrey T. , Storek Michael J. , Alonso‐Alonso Miguel , Atassi Nazem , Panicker Sandip , Parry Graham , Hammond Timothy , Hickman James J. 
Published: April 2022

AbstractChronic autoimmune demyelinating neuropathies are a group of rare neuromuscular disorders with complex, poorly characterized etiology. Here the authors describe a phenotypic, human‐on‐a‐chip (HoaC) electrical conduction model of two rare autoimmune demyelinating neuropathies, chronic inflammatory demyelinating polyneuropathy (CIDP) and multifocal motor neuropathy (MMN), and explore the efficacy of TNT005, a monoclonal antibody inhibitor of the classical complement pathway. Patient sera is shown to contain anti‐GM1 IgM and IgG antibodies capable of binding to human primary Schwann cells and induced pluripotent stem cell‐derived motoneurons (MNs). Patient autoantibody binding is sufficient to activate the classical complement pathway, resulting in detection of C3b and C5b‐9. A HoaC model, using a microelectrode array with directed axonal outgrowth over the electrodes treated with patient sera, exhibits reductions in MN action potential frequency and conduction velocity. TNT005 rescued the serum‐induced complement deposition and functional deficits while treatment with an isotype control antibody has no rescue effect. These data indicate that complement activation by CIDP and MMN patient serum is sufficient to mimic neurophysiological features of each disease and that complement inhibition with TNT005 is sufficient to rescue these pathological effects and provide efficacy data included in an investigational new drug application, demonstrating the model's translational potential.
Nonhuman primate abnormal behavior: Etiology, assessment, and treatment
Authors: Lutz Corrine K. , Coleman Kristine , Hopper Lydia M. , Novak Melinda A. , Perlman Jaine E. , Pomerantz Ori 
Published: April 2022

AbstractAcross captive settings, nonhuman primates may develop an array of abnormal behaviors including stereotypic and self‐injurious behavior. Abnormal behavior can indicate a state of poor welfare, since it is often associated with a suboptimal environment. However, this may not always be the case as some behaviors can develop independently of any psychological distress, be triggered in environments known to promote welfare, and be part of an animal's coping mechanism. Furthermore, not all animals develop abnormal behavior, which has led researchers to assess risk factors that differentiate individuals in the display of these behaviors. Intrinsic risk factors that have been identified include the animal's species and genetics, age, sex, temperament, and clinical condition, while environmental risk factors include variables such as the animal's rearing, housing condition, husbandry procedures, and research experiences. To identify specific triggers and at‐risk animals, the expression of abnormal behavior in captive nonhuman primates should be routinely addressed in a consistent manner by appropriately trained staff. Which behaviors to assess, what assessment methods to use, which primates to monitor, and the aims of data collection should all be identified before proceeding to an intervention and/or treatment. This article provides guidance for this process, by presenting an overview of known triggers and risk factors that should be considered, steps to design a comprehensive evaluation plan, and strategies that might be used for prevention or treatment. It also outlines the tools and processes for assessing and evaluating behavior in an appendix. This process will lead to a better understanding of abnormal behavior in captive primate colonies and ultimately to improved welfare.
Konzentriertes Wässriges Peroxodikarbonat: Effiziente Elektrosynthese und Anwendungen in Epoxidierungen, S‐, und N‐Oxidationen
Authors: Seitz Ann‐Katrin , Kohlpaintner Philipp J. , van Lingen Tim , Dyga Marco , Sprang Fiona , Zirbes Michael , Waldvogel Siegfried R. , Gooßen Lukas J. 
Published: April 2022

AbstractPeroxodikarbonate sind potenziell leistungsstarke, nachhaltige Oxidationsmittel und deshalb von großem Interesse. Diese konnten aber bisher nur in unzureichend hohen Konzentrationen und mit unbefriedigender Energieeffizienz erhalten werden. Konzentrierte (>0.9 mol L−1) Peroxodikarbonat‐Lösungen konnten nun erstmals durch Elektrolyse von wässrigen K2CO3/Na2CO3/KHCO3‐Lösungen bei hohen Stromdichten von 3.33 A cm−2 in einem effizient gekühlten Flusselektrolyseur mittels einer Bor‐dotierten Diamant (BDD)‐Anode und Edelstahlkathode erzeugt werden. Die potenzielle Anwendung als Oxidationsmittel konnte klar anhand verschiedener Reaktionen wie Sulfoxidation, N‐Oxidation und Epoxidierung gezeigt werden.
Hybrid Pyridine–Pyridone Foldamer Channels as M2‐Like Artificial Proton Channels
Authors: Shen Jie , Ye Ruijuan , Liu Zhiwei , Zeng Huaqiang 
Published: April 2022

AbstractCurrently, completely abiotic channel systems that concurrently reproduce the high selectivity and high permeation rate of natural protein channels are rare. Here, we provide one such biomimetic channel system, i.e., a novel family of helically folded hybrid amide foldamers that can serve as powerful artificial proton channels to mimic key transport features of the exceptionally selective Matrix‐2 (M2) proton channels. Possessing an angstrom‐scale tubular pore 3 Å in diameter, these low water permeability artificial channels transport protons at a rate 1.22 and 11 times as fast as gramicidin A and M2 channels, respectively, with exceptionally high selectivity factors of 167.6, 122.7, and 81.5 over Cl−, Na+, and K+ ions. Based on the experimental and computational findings, we propose a novel proton transport mechanism where a proton may create a channel‐spanning water chain from two or more short water chains to facilitate its own transmembrane flux via the Grotthuss mechanism.
Molecular Iron Oxide Clusters Boost the Oxygen Reduction Reaction of Platinum Electrocatalysts at Near‐Neutral pH
Authors: Lv Jia‐Qi , Lang Zhong‐Ling , Fu Jia‐Qi , Lan Qiao , Liu Rongji , Zang Hong‐Ying , Li Yang‐Guang , Ye Ding‐Ding , Streb Carsten 
Published: April 2022

AbstractThe oxygen reduction reaction (ORR) is a key energy conversion process, which is critical for the efficient operation of fuel cells and metal–air batteries. Here, we report the significant enhancement of the ORR‐performance of commercial platinum‐on‐carbon electrocatalysts when operated in aqueous electrolyte solutions (pH 5.6), containing the polyoxoanion [Fe28(μ3‐O)8(L‐(−)‐tart)16(CH3COO)24]20−. Mechanistic studies provide initial insights into the performance‐improving role of the iron oxide cluster during ORR. Technological deployment of the system is demonstrated by incorporation into a direct formate microfluidic fuel cell (DFMFC), where major performance increases are observed when compared with reference electrolytes. The study provides the first examples of iron oxide clusters in electrochemical energy conversion and storage.
Discrete, Cationic Palladium(II)‐Oxo Clusters via f‐Metal Ion Incorporation and their Macrocyclic Host‐Guest Interactions with Sulfonatocalixarenes
Authors: Bhattacharya Saurav , Barba‐Bon Andrea , Zewdie Tsedenia A. , Müller Anja B. , Nisar Talha , Chmielnicka Anna , Rutkowska Iwona A. , Schürmann Christian J. , Wagner Veit , Kuhnert Nikolai , Kulesza Pawel J. , Nau Werner M. , Kortz Ulrich 
Published: April 2022

AbstractWe report on the discovery of the first two examples of cationic palladium(II)‐oxo clusters (POCs) containing f‐metal ions, [PdII6O12M8{(CH3)2AsO2}16(H2O)8]4+ (M=CeIV, ThIV), and their physicochemical characterization in the solid state, in solution and in the gas phase. The molecular structure of the two novel POCs comprises an octahedral {Pd6O12}12− core that is capped by eight MIV ions, resulting in a cationic, cubic assembly {Pd6O12MIV8}20+, which is coordinated by a total of 16 terminal dimethylarsinate and eight water ligands, resulting in the mixed PdII‐CeIV/ThIV oxo‐clusters [PdII6O12M8{(CH3)2AsO2}16(H2O)8]4+ (M=Ce, Pd6Ce8; Th, Pd6Th8). We have also studied the formation of host‐guest inclusion complexes of Pd6Ce8 and Pd6Th8 with anionic 4‐sulfocalix[n]arenes (n=4, 6, 8), resulting in the first examples of discrete, enthalpically‐driven supramolecular assemblies between large metal‐oxo clusters and calixarene‐based macrocycles. The POCs were also found to be useful as pre‐catalysts for electrocatalytic CO2‐reduction and HCOOH‐oxidation.
Long‐Lived Charge‐Transfer State in Spiro Compact Electron Donor–Acceptor Dyads Based on Pyromellitimide‐Derived Rhodamine: Charge Transfer Dynamics and Electron Spin Polarization
Authors: Chen Xi , Sukhanov Andrey A. , Yan Yuxin , Bese Damla , Bese Cagri , Zhao Jianzhang , Voronkova Violeta K. , Barbon Antonio , Yaglioglu Halime Gul 
Published: April 2022

AbstractWe observed a long‐lived charge transfer (CT) state in a novel orthogonal compact electron donor–acceptor dyads, with closed form of rhodamine (Rho) as electron donor and pyromellitimide (PI),or thionated PI, as electron acceptor. The two parts in the dyads are connected via a spiro quaternary carbon atom, thus the torsion between the donor and acceptor is completely inhibited, which is beneficial to reduce the reorganization energy and to exploit the Marcus inverted region effect to prolong the CT state lifetime. Femtosecond transient absorption spectra show that the charge separation is rather fast, while nanosecond transient absorption spectra confirmed the formation of long‐lived CT state (2.6 μs). Time‐resolved electron paramagnetic resonance (TREPR) spectra determined the spin multiplicity of the long living state and assigned it to a 3CT state. Replacement of an oxygen atom in the PI part with a sulfur atom favoring classical intersystem crossing processes, causes a consistently shortening of the lifetime of the 3CT state (0.29 μs).
A Hybrid Supramolecular Polymeric Nanomedicine for Cascade‐Amplified Synergetic Cancer Therapy
Authors: Yang Kai , Qi Shaolong , Yu Xinyang , Bai Bing , Zhang Xueyan , Mao Zhengwei , Huang Feihe , Yu Guocan 
Published: April 2022

AbstractSupramolecular nanomedicines have shown great merits in cancer therapy, but their clinical translation is hampered by monotonous therapeutic modality and unsatisfactory antitumor performance. Herein, a hybrid supramolecular polymeric nanomedicine (SNPs) is developed based on β‐cyclodextrin/camptothecin (CPT) host−guest molecular recognition and iron‐carboxylate coordination. Iron ions stabilizingSNPscatalyze the conversion of intracellular hydrogen peroxide into highly toxic hydroxyl radical through a Fenton reaction, which further cleaves the thioketal linker of the supramolecular monomer to release potent CPT, thus amplifying the therapeutic efficacy by combining chemodynamic therapy and chemotherapy. The combination therapy stimulates antitumor immunity and promotes intratumoral infiltration of cytotoxic T lymphocytes by triggering immunogenic cell death. In synergy with PD‐L1 checkpoint blockade,SNPsenables enhanced immune therapy and a long‐term tumor remission.
Spotlight on mass spectrometric non‐target screening analysis: Advanced data processing methods recently communicated for extracting, prioritizing and quantifying features
Authors: Minkus Susanne , Bieber Stefan , Letzel Thomas 
Published: April 2022

AbstractNon‐target screening of trace organic compounds complements routine monitoring of water bodies. So‐called features need to be extracted from the raw data that preferably represent a chemical compound. Relevant features need to be prioritized and further be interpreted, for instance by identifying them. Finally, quantitative data is required to assess the risks of a detected compound. This review presents recent and noteworthy contributions to the processing of non‐target screening (NTS) data, prioritization of features as well as (semi‐) quantitative methods that do not require analytical standards. The focus lies on environmental water samples measured by liquid chromatography, electrospray ionization and high‐resolution mass spectrometry. Examples for fully‐integrated data processing workflows are given with options for parameter optimization and choosing between different feature extraction algorithms to increase feature coverage. The regions of interest‐multivariate curve resolution method is reviewed which combines a data compression alternative with chemometric feature extraction. Furthermore, prioritization strategies based on a confined chemical space for annotation, guidance by targeted analysis and signal intensity are presented. Exploiting the retention time (RT) as diagnostic evidence for NTS investigations is highlighted by discussing RT indexing and prediction using quantitative structure‐retention relationship models. Finally, a seminal technology for quantitative NTS is discussed without the need for analytical standards based on predicting ionization efficiencies.
Stability, structure, and antioxidant activity of astaxanthin crystal from Haematococcus pluvialis
Authors: Zhang Xiaowei , Ren Xiangrui , Zhao Xiaoyan , Liu Hongkai , Wang Meng , Zhu Yunping 
Published: April 2022

AbstractCrystallized anthaxanthin was prepared through the cleaning crystallization method and the stabilities during thermal, lighting, and pH treatment, and antioxidant activities in vitro were evaluated. The structural characterizations of astaxanthin crystal were verified by 1H, 13C NMR, and XRD analysis. The stability data showed that the astaxanthin crystal was more sensitive to heat, light, and pH compared to oleoresin. The sucrose had no outstanding influence on the astaxanthin crystal, while the stability of astaxanthin oleoresin slightly increased with the increase of sugar concentration. The XRD and nuclear magnetic resonance spectra elucidated that the astaxanthin crystal was all trans structure. The astaxanthin crystal showed the dominant 1,1′‐diphenyl‐2‐picrylhydrazyl (IC50 18.65 μmol L−1), 2,2′‐azino‐bis(3‐ethylbenzothiazoline‐6‐sulfonic acid) diammonium salt˙+(21.1 μmol L−1), •OH (IC50 49.46 μmol L−1) and ferric reducing antioxidant power (IC50 81.60 μmol L−1) activities. The investigated results would be helpful for improving the development of astaxanthin crystal in food products.
Bis(2‐, 3‐, 4‐carboxyethylpyridinium) hexafluorosilicates as potential caries prophylactic agents
Authors: Gelmboldt Vladimir O. , Lytvynchuk Irina V. , Shyshkin Ivan O. , Khromagina Larysa N. , Fonari Marina S. , Kravtsov Victor Ch. 
Published: April 2022

AbstractInteraction of 2‐, 3‐, 4‐carboxyethylpyridines (L1, L2, L3) with fluorosilicic acid results in the corresponding bis(pyridinium) hexafluorosilicates I–III, characterized by elemental analysis, IR, 1H, 19F nuclear magnetic resonance (NMR), and mass spectrometry, solubility data, and X‐ray crystallography. Crystallographic data: Fdd2, Z = 8, a = 28.610(2) Å, b = 18.8378(14) Å, c = 7.3236(5) Å (I); P‐1, Z = 1, a = 6.2712(4) Å, b = 7.1706(5) Å, c = 10.9721(7) Å, α = 102.514(6)°, β = 97.037(5)°, γ = 93.640(6)° (II); P21/c, Z = 2, a = 10.0345(6) Å, b = 9.8734(5) Å, c = 9.4704(6) Å, β = 94.347(6)° (III). The dominant intermolecular contacts from the Hirshfeld surface analysis are H…F/F…H, H…H, and H…O/O…H with percentages of 33.3%–34.5%, 26.4%–30.0%, and 16.0%–21.8%. The infrared spectra for I–III exhibit stretching vibrations ν(N+H) at 3300–3050 cm–1; stretching and deformation vibrations ν(SiF) and δ(SiF2) for [SiF6]2– anions are registered near 740 cm–1 and in the range of 480–440 cm–1. In the 19F NMR spectra of aqueous solutions of I–III, strong singlet signals of the [SiF6]2– anion were registered at δ(F) = −133.35 ppm (I), –131.43 ppm (II), –129.02 ppm (III) with two satellites due to the spin‐spin interaction 29Si–19F (J(29Si–19F) = 107.5 Hz (II), 107.6 Hz (III)). I–III reveal high solubility in water and dimethyl sulfoxide and very poor solubility in methanol and ethanol. All compounds demonstrate noticeable anticaries activity and absence of hepatotoxic effects, and bis(3‐carboxyethylpyridinium) hexafluorosilicate II displays the highest caries‐preventive efficacy, which significantly exceeds values for the reference preparations, NaF and (NH4)2[SiF6].
Bauhaus und Bauphysik – Eine bauphysikalische Untersuchung und Bewertung am Beispiel Haus Oud
Authors: Röseler Holger , Krause Pia , Eitle Adrian , Veres Eva , Leistner Philip 
Published: April 2022

AbstractWährend aktuell das Neue Europäische Bauhaus mit einer interdisziplinären Ausrichtung die zukünftige Gestaltung unserer Lebens‐ und Bauweisen in den Blickpunkt rückt, fielen vor wenigen Jahren zwei Jubiläen zusammen. 100 Jahre waren seit der Bauhaus‐Gründung vergangen und 90 Jahre seit der Gründung eines der ersten Forschungsinstitute mit dem Schwerpunkt Bauphysik. Natürlich trennt beide Institutionen nicht nur ein 10‐jähriger „Altersunterschied”. Mit dem historisch einzigartigen Bauhaus ist die anfangs sehr kleine Stuttgarter Gruppe bauphysikalischer Enthusiasten nicht zu vergleichen. Rückblickend lassen sich aber Ähnlichkeiten der Motive beider Initiativen konstatieren und es ist anzunehmen, dass beim „Neuen Bauen” von Anfang an auch Überlegungen in den Entwurfsprozess einflossen, die der Bauphysik zentrale Fragestellungen und wichtige Impulse mit auf den Weg gaben. Diese Beziehung zwischen Bauhaus und Bauphysik wird am Beispiel des Reihenhauses Oud in der Weißenhofsiedlung in Stuttgart untersucht.Die Ergebnisse zeigen, dass die Bausubstanz im Reihenhaus Oud eine deutlich schlankere Konstruktion als Vergleichsbauten seiner Zeit aufwies. Die daraus resultierenden bauphysikalischen Auswirkungen, mit Fokus auf den Wärme‐, Feuchte‐ und Schallschutz, werden analysiert. In Summe stellte das Haus Oud einen wertvollen Beitrag zur Erforschung und Weiterentwicklung von kostengünstigen, innovativen Wohnformen dar und war prägend für zukünftige Bauprozesse bis in die Gegenwart.