bluuebunny/crossref_metadata_2025_split huggingface dataset:
Review of Recent Development of In Situ/Operando Characterization Techniques for Lithium Battery Research
Authors: Liu Dongqing , Shadike Zulipiya , Lin Ruoqian , Qian Kun , Li Hai , Li Kaikai , Wang Shuwei , Yu Qipeng , Liu Ming , Ganapathy Swapna , Qin Xianying , Yang Quan‐Hong , Wagemaker Marnix , Kang Feiyu , Yang Xiao‐Qing , Li Baohua 
Published: May 2019

AbstractThe increasing demands of energy storage require the significant improvement of current Li‐ion battery electrode materials and the development of advanced electrode materials. Thus, it is necessary to gain an in‐depth understanding of the reaction processes, degradation mechanism, and thermal decomposition mechanisms under realistic operation conditions. This understanding can be obtained by in situ/operando characterization techniques, which provide information on the structure evolution, redox mechanism, solid‐electrolyte interphase (SEI) formation, side reactions, and Li‐ion transport properties under operating conditions. Here, the recent developments in the in situ/operando techniques employed for the investigation of the structural stability, dynamic properties, chemical environment changes, and morphological evolution are described and summarized. The experimental approaches reviewed here include X‐ray, electron, neutron, optical, and scanning probes. The experimental methods and operating principles, especially the in situ cell designs, are described in detail. Representative studies of the in situ/operando techniques are summarized, and finally the major current challenges and future opportunities are discussed. Several important battery challenges are likely to benefit from these in situ/operando techniques, including the inhomogeneous reactions of high‐energy‐density cathodes, the development of safe and reversible Li metal plating, and the development of stable SEI.
A Crystalline, 2D Polyarylimide Cathode for Ultrastable and Ultrafast Li Storage
Authors: Wang Gang , Chandrasekhar Naisa , Biswal Bishnu P. , Becker Daniel , Paasch Silvia , Brunner Eike , Addicoat Matthew , Yu Minghao , Berger Reinhard , Feng Xinliang 
Published: May 2019

AbstractOrganic electrode materials are of long‐standing interest for next‐generation sustainable lithium‐ion batteries (LIBs). As a promising cathode candidate, imide compounds have attracted extensive attention due to their low cost, high theoretical capacity, high working voltage, and fast redox reaction. However, the redox active site utilization of imide electrodes remains challenging for them to fulfill their potential applications. Herein, the synthesis of a highly stable, crystalline 2D polyarylimide (2D‐PAI) integrated with carbon nanotube (CNT) is demonstrated for the use as cathode material in LIBs. The synthesized polyarylimide hybrid (2D‐PAI@CNT) is featured with abundant π‐conjugated redox‐active naphthalene diimide units, a robust cyclic imide linkage, high surface area, and well‐defined accessible pores, which render the efficient utilization of redox active sites (82.9%), excellent structural stability, and fast ion diffusion. As a consequence, high rate capability and ultrastable cycle stability (100% capacity retention after 8000 cycles) are achieved in the 2D‐PAI@CNT cathode, which far exceeds the state‐of‐the‐art polyimide electrodes. This work may inspire the development of novel organic electrodes for sustainable and durable rechargeable batteries.
4D Printing of Shape‐Memory Hydrogels for Soft‐Robotic Functions
Authors: Shiblee MD Nahin Islam , Ahmed Kumkum , Kawakami Masaru , Furukawa Hidemitsu 
Published: May 2019

AbstractHydrogel actuators with soft‐robotic functions and biomimetic advanced materials with facile and programmable fabrication processes remain scarce. A novel approach to fabricating a shape‐memory‐hydrogel‐(SMG)‐based bilayer system using 3D printing to yield a soft actuator responsive to the methodical application of swelling and heat is introduced. Each layer of the bilayer is composed of poly(N,N‐dimethyl acrylamide‐co‐stearyl acrylate) (P(DMAAm‐co‐SA))‐based hydrogels with different concentrations of the crystalline monomer SA within the SMG network and which exhibit distinctive physicochemical properties that enable anisotropic swelling‐induced actuation of the bilayer with reversible shape‐memory properties. The deformation, reversibility, and response time of the bilayer actuator are extensively dependent on temperature. Utilizing the proposed SMG bilayer actuator model with its synergistic functions, a nature‐inspired flower architecture that changes its shape upon immersion in water and an underwater 3D macroscopic soft gripper that can grab, transport, and release a guest substance are developed to demonstrate the applicability of these hydrogels in biomimetic actuators, encapsulating systems, and soft robotics.
Recent Progress in 2D Layered III–VI Semiconductors and their Heterostructures for Optoelectronic Device Applications
Authors: Yang Zhibin , Hao Jianhua 
Published: May 2019

AbstractDuring the past decade, great effort has been devoted to research on 2D layered materials due to their reduced thickness and extraordinary physical properties, which open new opportunities for developing next‐generation applications in various fields. Ultrathin III–VI semiconductors (e.g., GaSe, InSe, In2Se3, etc.) have emerged as potential candidates for nano‐optoelectronic applications thanks to their sizable layer‐dependent bandgaps and high carrier mobility, which could enable broadband photodetection and efficient conversion of solar energy. A systematic review is provided on 2D III–VI semiconductor‐based state‐of‐the‐art optoelectronic devices, such as phototransistors, photoconductors, and solar cells, reported in recent years. To better understand the mechanism and performance of the devices, an introduction to the electronic structures and optical properties of several representative III–VI members is first given. A comprehensive overview is then given on device geometry design, operating principles, and performance in optoelectronic applications based on III–VI semiconductors and their heterostructures. The techniques to enhance the performances of devices are also discussed. Finally, a brief discussion on the challenges and future opportunities in this field is provided.
Light‐Responsive (Supra)Molecular Architectures: Recent Advances
Authors: Baroncini Massimo , Groppi Jessica , Corra Stefano , Silvi Serena , Credi Alberto 
Published: May 2019

AbstractThe development and investigation of (supra)molecular‐based architectures characterized by light‐activated functionalities is a highly relevant topic of chemical research. The interest on photo‐controlled systems arises not only from their potential applications in different fields of technology but also from their scientific significance related to the understanding of light–matter interactions at the nanoscale. Indeed, light is a peculiar and unique tool as it can be conveniently applied to supply the energy required to affect and operate a system and, at the same time, to probe its state and investigate its transformations. Some basic aspects of light‐induced processes in (supra)molecular architectures are discussed here in the frame of their use to implement novel functionalities in nanostructured systems and materials. In this perspective, a few recent examples from our own work will be illustrated which are meant to provide an overview of the current directions in this highly cross‐disciplinary field of research.
A High Voltage Aqueous Zinc–Organic Hybrid Flow Battery
Authors: Park Minjoon , Beh Eugene S. , Fell Eric M. , Jing Yan , Kerr Emily F. , De Porcellinis Diana , Goulet Marc‐Antoni , Ryu Jaechan , Wong Andrew A. , Gordon Roy G. , Cho Jaephil , Aziz Michael J. 
Published: May 2019

AbstractWater‐soluble redox‐active organic molecules have attracted extensive attention as electrical energy storage alternatives to redox‐active metals that are low in abundance and high in cost. Here an aqueous zinc–organic hybrid redox flow battery (RFB) is reported with a positive electrolyte comprising a functionalized 1,4‐hydroquinone bearing four (dimethylamino)methyl groups dissolved in sulfuric acid. By utilizing a three‐electrolyte, two‐membrane configuration this acidic positive electrolyte is effectively paired with an alkaline negative electrolyte comprising a Zn/[Zn(OH)4]2− redox couple and a hybrid RFB is operated at a high operating voltage of 2.0 V. It is shown that the electrochemical reversibility and kinetics of the organic redox species can be enhanced by an electrocatalyst, leading to a cyclic voltammetry peak separation as low as 35 mV and enabling an enhanced rate capability.
KCNJ6 variants modulate reward‐related brain processes and impact executive functions in attention‐deficit/hyperactivity disorder
Authors: Ziegler Georg C. , Röser Christoph , Renner Tobias , Hahn Tim , Ehlis Ann‐Christine , Weber Heike , Dempfle Astrid , Walitza Susanne , Jacob Christian , Romanos Marcel , Fallgatter Andreas J. , Reif Andreas , Lesch Klaus‐Peter 
Published: May 2019

AbstractKCNJ6, encoding a potassium channel subunit, regulates the excitability of dopaminergic neurons and is expressed in attention‐deficit/hyperactivity disorder (ADHD)‐relevant brain regions. As a potential ADHD risk gene, KCNJ6, therefore, may contribute to the endophenotypic variation of the disorder. The impact of two SNPs, rs7275707 and rs6517442, both located in the transcriptional control region of KCNJ6, on reporter gene expression was explored in cultured cells. The KCNJ6 variants were then tested for association with ADHD and personality traits in a family‐based sample (165 affected children) and an adult case–control sample (450 patients, 426 controls). Furthermore, the genotypic influence on performance in an n‐back task and a cued continuous performance test (cCPT) was investigated by electroencephalography recordings. Finally, rs6517442 function was assessed by a reward anticipation paradigm using functional magnetic resonance imaging. Different haplotypes of rs7275707 and rs6517442 significantly influenced KCNJ6 gene expression proving their functional relevance on the molecular level. In the family‐based children sample rs7275707 was associated with ADHD (p = .038). Moreover, rs7275707 showed association with the personality trait of Reward Dependence (p = .031). In the ADHD group, both rs7275707 and rs6517442 influenced the Go‐centroid location in the cCPT and the N200 amplitude in the n‐back task. Furthermore, ventral striatal activation was impacted by rs6517442 during reward anticipation. Our data indicate that functional variants of KCNJ6 influence brain activity during reward‐related and executive processes supporting the view of a differential, age‐dependent modulatory impact of dopamine‐related brain processes in ADHD risk.
Physical Manipulation of Lanthanide‐Activated Photoluminescence
Authors: Wang Yangbo , Zhou Jie , Gao Jiaxin , Zhang Kun , Gao Chao , Xie Xiaoji , Huang Ling 
Published: May 2019

AbstractVersatile manipulation of lanthanide photoluminescence not only enables a more thorough understanding of the luminescent mechanism, but also promotes their widespread applications including advanced display and security, bioimaging and biotherapy, and sensors. The traditional chemical methods, engineering of composition, concentration, size, morphology, and surface defects, can easily tune the excitation, energy transfer and emission processes and have been frequently used. Despite the powerful ability to control luminescence intensity and selectivity, these chemical approaches suffer from cumbersome synthesis processes and are usually time consuming and irreversible. Recently, there have been numerous examples of physical approaches realizing in situ, real time, and reversible luminescence manipulation for certain materials under a given excitation. Herein, the existing physical strategies comprising temperature, magnetic field, electric field, and mechanical stress are summarized. For each approach, the action mechanism, material design, applications, as well as current challenges are discussed, and possible development directions and broadening of the potential application areas are considered.
Silica‐Supported Molybdenum Oxo Alkylidenes: Bridging the Gap between Internal and Terminal Olefin Metathesis
Authors: Pucino Margherita , Zhai Feng , Gordon Christopher P. , Mance Deni , Hoveyda Amir H. , Schrock Richard R. , Copéret Christophe 
Published: May 2019

AbstractGrafting a molybdenum oxo alkylidene on silica (partially dehydroxylated at 700 °C) affords the first example of a well‐defined silica‐supported Mo oxo alkylidene, which is an analogue of the putative active sites in heterogeneous Mo‐based metathesis catalysts. In contrast to its tungsten analogue, which shows poor activity towards terminal olefins because of the formation of a stable off‐cycle metallacyclobutane intermediate, the Mo catalyst shows high metathesis activity for both terminal and internal olefins that is consistent with the lower stability of Mo metallacyclobutane intermediates. This Mo oxo metathesis catalyst also outperforms its corresponding neutral silica‐supported Mo and W imido analogues.
Darstellung von hochmolekularen Polyethern durch die zwitterionische Lewis‐Paar‐Polymerisation von Epoxiden
Authors: Walther Patrick , Krauß Annabelle , Naumann Stefan 
Published: May 2019

AbstractEin dualkatalytisches System bestehend aus N‐heterocyclischen Olefinen (NHOs) und Magnesium Bis(hexamethyldisilazid) (Mg(HMDS)2) ermöglicht die Herstellung von Poly(propylenoxid) (PPO) mit einem Molekulargewicht (Mn) von >500 000 g mol−1, in manchen Fällen sogar >106 g mol−1, wie mittels GPC/Lichtstreuung verifiziert wurde. Dies wird durch die Kombination der schnellen Polymerisationskinetik eines zwitterionischen Lewis‐Paares mit der effizienten Epoxidaktivierung durch die MgII‐Spezies erreicht. Hierbei werden Übertragungsreaktionen auf Monomere (“transfer‐to‐monomer”), die üblicherweise die Synthese von Polyethern mit hohen Polymerisationsgraden behindern, quantitativ unterdrückt. Mittels NMR‐ und MALDI‐ToF‐MS‐Experimenten konnten Schlüsselaspekte des vorgeschlagenen Mechanismus identifiziert werden, wobei die Polymerisation über einen nukleophilen Angriff des NHOs am aktivierten Monomer initiiert wird, was eine zwitterionische Spezies generiert. Weiterhin wird demonstriert, dass dieser Ansatz auch auf andere Epoxide übertragbar ist, einschließlich funktionalisierter Monomere.
Core–Shell‐Structured LaTaON2 Transformed from LaKNaTaO5 Plates for Enhanced Photocatalytic H2 Evolution
Authors: Wang Xin , Hisatomi Takashi , Wang Zheng , Song Jun , Qu Junle , Takata Tsuyoshi , Domen Kazunari 
Published: May 2019

AbstractLaTaON2 is a photocatalyst with intense visible light absorption up to 650 nm, but exhibits low H2 evolution activity owing to uncontrolled facets and high defect densities. In this work, core–shell‐structured plate‐like LaKNaTaO5/LaTaON2 was synthesized by nitriding a layered perovskite‐type LaKNaTaO5. The volatilization of K and Na species during the nitridation promoted the rapid transformation of LaKNaTaO5 into LaTaON2 along [010] direction with the plate‐like shape retained. This yielded high‐quality LaTaON2 shells exposing (010) facets on the lattice‐matched LaKNaTaO5 cores. After loading with a Rh co‐catalyst, LaKNaTaO5/LaTaON2 showed photocatalytic H2 evolution activity four times greater than that obtained from conventional irregular‐shaped LaTaON2 powders and utilized visible light up to 620 nm. This work provides a novel strategy yielding oxynitrides with well‐defined facets and low defect densities by selecting lattice‐matched oxide precursors containing volatile components.
Lewis Pair Polymerization of Epoxides via Zwitterionic Species as a Route to High‐Molar‐Mass Polyethers
Authors: Walther Patrick , Krauß Annabelle , Naumann Stefan 
Published: May 2019

AbstractA dual catalytic setup based on N‐heterocyclic olefins (NHOs) and magnesium bis(hexamethyldisilazide) (Mg(HMDS)2) was used to prepare poly(propylene oxide) with a molar mass (Mn) >500 000 g mol−1, in some cases even >106 g mol−1, as determined by GPC/light scattering. This is achieved by combining the rapid polymerization characteristics of a zwitterionic, Lewis pair type mechanism with the efficient epoxide activation by the MgII species. Transfer‐to‐monomer, traditionally frustrating attempts at synthesizing polyethers with a high degree of polymerization, is practically removed as a limiting factor by this approach. NMR and MALDI‐ToF MS experiments reveal key aspects of the proposed mechanism, whereby the polymerization is initiated via nucleophilic attack by the NHO on the activated monomer, generating a zwitterionic species. This strategy can also be extended to other epoxides, including functionalized monomers.
Reactivity and Catalytic Activity of Homobimetallic Vanadium(V) Complex Derived from Bis(5‐chlorosalicylaldehyde)oxaloyldihydrazone Ligand
Authors: Syiemlieh Ibanphylla , Asthana Mrityunjaya , Lal Ram A. 
Published: May 2019

Homobimetallic vanadium(V) complex of the composition [(CH3)2NH2+]2[(VO2)2(sloxCl)].4H2O was synthesized from the reaction of V2O5 with bis(5‐chlorosalicylaldehyde)oxaloyldihydrazone ligand in a 1:1 molar ratio in methanol. The structure of the complex was established by X‐ray crystallography. Reactivity of the complex with H2O2 leads to bis (monooxidoperoxidovanadate(V)) [{VO(O2)}2(sloxCl)]2− formation and with HCl, oxidohydroxido complex of composition [(VO (OH)(sloxCl)]2− was formed. Binding interaction of the complex was also investigated toward protein (BSA) and it was found to be 2.21 x 108 M−1. The catalytic activity of the complex in the oxidation of alcohols and oxidative bromination of some organic substrates was also studied, and it showed a great potent as a catalyst.
Causal Factors for Knee, Hip, and Hand Osteoarthritis: A Mendelian Randomization Study in the UK Biobank
Authors: Funck‐Brentano Thomas , Nethander Maria , Movérare‐Skrtic Sofia , Richette Pascal , Ohlsson Claes 
Published: May 2019

ObjectiveThere is no curative treatment for osteoarthritis (OA), which is the most common form of arthritis. This study was undertaken to identify causal risk factors of knee, hip, and hand OA.MethodsIndividual‐level data from 384,838 unrelated participants in the UK Biobank study were analyzed. Mendelian randomization (MR) analyses were performed to test for causality for body mass index (BMI), bone mineral density (BMD), serum high‐density lipoprotein cholesterol, low‐density lipoprotein cholesterol, and triglyceride levels, type 2 diabetes, systolic blood pressure (BP), and C‐reactive protein (CRP) levels. The primary outcome measure was OA determined using hospital diagnoses (all sites, n = 48,431; knee, n = 19,727; hip, n = 11,875; hand, n = 2,330). Odds ratios (ORs) with 95% confidence intervals (95% CIs) were calculated.ResultsMR analyses demonstrated a robust causal association of genetically determined BMI with all OA (OR per SD increase 1.57 [95% CI 1.44–1.71]), and with knee OA and hip OA, but not with hand OA. Increased genetically determined femoral neck BMD was causally associated with all OA (OR per SD increase 1.14 [95% CI 1.06–1.22]), knee OA, and hip OA. Low systolic BP was causally associated with all OA (OR per SD decrease 1.55 [95% CI 1.29–1.87]), knee OA, and hip OA. There was no evidence of causality for the other tested metabolic factors or CRP level.ConclusionOur findings indicate that BMI exerts a major causal effect on the risk of OA at weight‐bearing joints, but not at the hand. Evidence of causality of all OA, knee OA, and hip OA was also observed for high femoral neck BMD and low systolic BP. However, we found no evidence of causality for other metabolic factors or CRP level.
One‐Dimensional Nanostructured Pseudocapacitive Materials: Design, Synthesis and Applications in Supercapacitors
Authors: Sun Jinfeng , Guo Lingzhi , Sun Xuan , Zhang Jinyang , Hou Linrui , Li Li , Yang Shuhua , Yuan Changzhou 
Published: May 2019

AbstractIn the past decades, pseudocapacitive materials (PCMs) for electrochemical energy storage have drawn enthusiastic attention from researchers, owing to their virtue of larger Faradaic capacitance facilitating enhanced energy densities compared to electric double‐layer capacitive materials. To maximize capacitive properties without sacrificing power densities, novel design and fine fabrication of innovative PCMs with rational micro‐structures become of significant importance. Typically, enormous efforts have been devoted to fabricating 1D nanostructured PCMs for advanced supercapacitors, thanks to their geometrical merits facilitating the ionic/electronic transport. This review mainly focuses on the latest development and progress of 1D nanostructured PCMs for advanced supercapacitors. Firstly, typical pseudocapacitive mechanisms are discussed in detail. Secondly, physicochemical properties and intrinsic merits of 1D nanoscaled electrodes are comprehensively described. Thirdly, representative synthetic methodologies, optimization strategies and involved formation mechanisms for 1D nanodimensional PCMs are surveyed. Besides, the applications of 1D versatile PCMs including 1D conventional nanostructures, nano‐arrays, core‐shell nano‐architectures and secondary superstructures are systematically summarized as competitive electrodes for supercapacitors. Finally, future challenges, prospects and opportunities of 1D nanostructured PCMs for next‐generation supercapacitors are further proposed.
Life‐cycle assessment of green biorefinery process options
Authors: Prieler Manuela , Lindorfer Johannes , Steinmüller Horst 
Published: May 2019

AbstractIn this study, the biorefinery process for generating amino acids (AA) from grass silage is analyzed ecologically. Life‐cycle assessment is conducted in accordance with ISO 14040 and ISO 14044. A kilogram of amino acid is selected as a functional unit. The system boundary is drawn around silage production and includes both agricultural and conversion processes. The technology setup is modeled based on data from a demonstration amino acid production plant that uses the silages of permanent grassland in Austria (GBR 1), and data from the experimental work conducted within the European‐funded GRASSFinery project (GBR 2) located in the Czech Republic and Germany, using life‐cycle assessment software (GaBi®).Different scenarios are developed with different system boundaries. The baseline scenario for GBR 1 and the primary and central processing units of GBR 2 includes the green biorefinery processes without the disposal of waste flows to the biogas plant. By enlarging the system boundaries, the waste flows to the biogas plant and the energy yield from anaerobic digestion are considered as well as the transportation of intermediate products.The global warming potential (GWP) of the whole AA production process ranges from 11.4 to 16.8 kg CO2eq/kg AA, depending on the scenario. The GWP excludes biogenic carbon so the bound carbon in the grass silage is not included. High quality grass silage is crucial to achieve high yields of amino acids. Closed loops are a sensible step to reduce the environmental impact. © 2019 Society of Chemical Industry and John Wiley & Sons, Ltd