bluuebunny/crossref_metadata_2025_split huggingface dataset:
Cobalt(II)‐Centered Fluorinated Phthalocyanine‐Sulfur SNAr Chemistry for Robust Lithium–Sulfur Batteries with Superior Conversion Kinetics
Authors: Kim Jiheon , Shin Hyuksoo , Yoo Dong‐Joo , Kang Sangho , Chung Sung‐Yoon , Char Kookheon , Choi Jang Wook 
Published: September 2021

AbstractDue to the exceptional theoretical energy density and low cost of elemental sulfur, lithium–sulfur (Li–S) batteries are spotlighted as promising post‐lithium‐ion batteries. Despite these advantages, the performance of Li–S batteries would need to be improved further for their wide dissemination in practical applications. Here, cobalt(II)‐centered fluorinated phthalocyanine, namely, F‐Co(II)Pc, is reported as a multi‐functional component for sulfur cathodes with the following benefits: 1) enhanced conversion kinetics as a result of the catalytic effect of the cobalt(II) center, 2) efficient sulfur linkage via the fluorine functionality, which undergoes a nucleophilic aromatic substitution (SNAr) reaction, 3) suppression of the shuttling issue by the nitrogen atoms because of their strong affinity with polysulfides, and 4) the necessary aromaticity to engage in π–π interaction with reduced graphene oxide for electrical conductivity. The resulting electrode has promising electrochemical properties, such as sustainable cycling for 700 cycles and robust operation with a sulfur loading of 12 mgsulfur cm−2, unveiling the promising nature of phthalocyanine and its related molecular families for advanced Li–S batteries.
Graphene Oxide Encapsulating Liquid Metal to Toughen Hydrogel
Authors: Hu Yijie , Zhuo Hao , Zhang Yu , Lai Haihong , Yi Jiwang , Chen Zehong , Peng Xinwen , Wang Xiaohui , Liu Chuanfu , Sun Runcang , Zhong Linxin 
Published: September 2021

AbstractStretchable and tough hydrogels are highly required for various flexible devices. Liquid metal (LM) emerges as an attractive applicant in preparing functional hydrogels due to its unique features. However, the high fluidity of LM and incompatibility between LM and polymer matrix make it hard to fabricate tough hydrogels. Herein, inspired by the function of ligaments in biological structure, graphene oxide (GO) nanosheets are introduced to encapsulate LM droplets. GO nanosheets form strong interaction with both LM and polymer matrix to create a stable shell that prevents LM droplet from fracture and exudation to polymer network. The flexible LM/GO core–shell microstructure avoids phase separation and produces a tough hydrogel with stress of high up to 303 kPa at 1240% elongation. It also shows notch insensitivity and strong adhesion to various surfaces. This study opens the possibility of using LM in stretchable and tough hydrogels.
Large‐Area Epitaxial Film Growth of van der Waals Ferromagnetic Ternary Chalcogenides
Authors: Giri Anupam , De Chandan , Kumar Manish , Pal Monalisa , Lee Hyun Hwi , Kim Jun Sung , Cheong Sang‐Wook , Jeong Unyong 
Published: September 2021

AbstractFollowing the first experimental realization of intrinsic ferromagnetism in 2D van der Waals (vdW) crystals, several ternary metal chalcogenides with unprecedented long‐range ferromagnetic order have been explored. However, the synthesis of large‐area 2D ternary metal chalcogenide thin films is a great challenge, and a generalized synthesis has not been demonstrated yet. Here, a quick and scalable synthesis of epitaxially aligned ferromagnetic ternary metal chalcogenide thin films (Cr2Ge2Te6, Cr2Si2Te6, Mn3Si2Te6) is reported. The synthesis is based on the flux‐controlled surface diffusion of Te on metal (Cr, Mn)‐deposited wafer (Ge, Si) substrates. Magnetic anisotropy study of the epitaxial ternary thin films reveals the intrinsic magnetic easy axis; out‐of‐plane direction for Cr2Ge2Te6 and Cr2Si2Te6, and in‐plane direction for Mn3Si2Te6. In addition to the synthesis, this work creates an opportunity for transfer‐free device fabrication for realizing magnetoelectronics based on the electrical control of both charge and spin degrees of freedom in 2D ferromagnetic semiconductors.
Flexible PDMS/Al2O3 Nanolaminates for the Encapsulation of Blue OLEDs
Authors: Li Yun , Xiong Yingfei , Cao Weiran , Zhu Qianqian , Lin Yuan , Zhang Yinghao , Liu Mengjia , Yang Fan , Cao Kun , Chen Rong 
Published: September 2021

AbstractIn this work, the polydimethylsiloxane (PDMS)/Al2O3 nanolaminates with optimized sublayer thickness and interfaces have been developed to protect the organic light‐emitting didoes (OLEDs) from the erosion of the moisture in the ambient. The O2 plasma pretreatment is used to tune the wettability of the ultrathin PDMS sublayers with nanoscale thickness, and the distinct interfaces between the Al2O3 and PDMS sublayers are obtained. The electrical calcium test is exploited to evaluate the barrier properties of the encapsulation nanolayers, and the water vapor transmission rate (WVTR) value of the 2.5 PDMS/Al2O3 dyads can reach the range of ≈10−5 g m−2 day−1. The mechanical stability of the nanolaminates is further improved by introducing the top epoxy layer, which helps move the neutral axis (NA) to the center of the barrier, and the applied external strain decreases significantly. Compared with the sample without the epoxy layer, a slighter increase of the WVTR value of the multilayered encapsulation films with optimized NA position is obtained. Furthermore, the operational lifetime of blue OLEDs encapsulated with the multilayered encapsulation films improves from 6 to more than 370 h, which shows significantly improved stability and reliability.
2D Optical Waveguides Based on Hierarchical Organic Semiconductor Single Crystals
Authors: Ma Yingxin , Zong Yi , Yin Huiling , Lin Hongtao , Chen Shuhai , Wang Xue‐Dong 
Published: September 2021

AbstractToward the evolution of integrated optoelectronic circuits, it is vital matter to realize 2D optical waveguide at micro/nanoscale. However, due to the waveguiding principle of the traditional dielectric waveguide, the transverse and longitudinal dimensions cannot be greatly reduced, thus the size of photonic apparatus is far from reaching the size level for the microelectronic device. Therefore, it is difficult to achieve a high‐level hybrid integration of integrated optical path and microelectronic circuit. However, the organic crystals with polygonal structure and hierarchical structure as the medium also can form optical waveguide by confining photons/electrons at the micro/nanoscale along different directions, and these organic microcrystals can be well applied into the ultracompact optoelectronic devices. Herein, the fabrication of organic crystals as the medium of 2D optical waveguide is briefly introduced, as well as the 2D optical waveguide phenomenon existing in these polygonal and hierarchical microcrystals. Moreover, a conclusion is drawn and expectations are expressed for the 2D optical waveguide based on organic microstructure in the near future.
Cover crops and residual herbicides reduce selection pressure for Palmer amaranth resistance to dicamba‐applied postemergence in cotton
Authors: Hand Lavesta C. , Randell Taylor M. , Nichols Robert L. , Steckel Lawrence E. , Basinger Nicholas T. , Culpepper A. Stanley 
Published: September 2021

AbstractThe most widely planted cotton (Gossypium hirsutumL.) and soybean [Glycine max(L.) Merr.] varieties in the United States are resistant to the herbicide dicamba. Measures to reduce selection pressure for dicamba‐resistant weeds is paramount. Four studies evaluated strategies to reduce selection pressure for Palmer amaranth (Amaranthus palmeriS. Watson) resistance to dicamba applied postemergence (POST) in cotton. A split‐plot arrangement consisted of conventional tillage or cereal rye (Secale cerealeL.) cover crop as the whole plot. The subplot included four herbicide systems: no herbicide, 3 POSTs, fomesafen plus diuron applied pre‐emergence (PRE) followed by (fb) 3 POSTs, and PRE fb 2 POSTs fb diuron plus monosodium methyl arsenate applied lay‐by post‐directed (LPD). The POST herbicide applications were glyphosate plus dicamba. The cover crop reduced Palmer amaranth density 75, 70, and 54% at the time of POST 1, POST 2, and POST 3 application, respectively. Pre‐emergence herbicides fb POST applications reduced Palmer amaranth densities 99, 99, and 96% at the aforementioned application timings, respectively. Cover crop plus PRE herbicides provided similar reductions. Cumulative for the season, Palmer amaranth exposure to dicamba was reduced 65% by the cover crop, 98% by both PRE herbicides and cover crop plus PRE herbicides compared to 3 POST applications. An LPD application reduced Palmer amaranth exposure to dicamba by 38,319 plants ha–1compared to a third POST. Cotton stand was higher in conventional systems when soil temperatures were 30–37 °C during emergence; however, stand in the cover crop was greater when soil temperatures were 40–43 °C. Yields were reduced 14% in a total POST herbicide program, and were improved 14% in a cover crop. A cereal rye cover crop and residual PRE herbicides had the biggest impact on reducing selection pressure for Palmer amaranth resistance to dicamba while also improving yield.
Soil hydrologic grouping guide which soil and weather properties best estimate corn nitrogen need
Authors: Bean Gregory Mac , Ransom Curtis J. , Kitchen Newell R. , Scharf Peter C. , Veum Kristen S. , Camberato James J. , Ferguson Richard B. , Fernández Fabián G. , Franzen David W. , Laboski Carrie A. M. , Nafziger Emerson D. , Sawyer John E. , Nielsen Robert L. 
Published: September 2021

AbstractNitrogen fertilizer recommendations in corn (Zea mays L.) that match the economically optimal nitrogen fertilizer rate (EONR) are imperative for profitability and minimizing environmental degradation. However, the amount of soil N available for the crop depends on soil and weather factors, making it difficult to know the EONR from year‐to‐year and from field‐to‐field. Our objective was to explore, within the framework of hydrologic soil groups and drainage classifications (HGDC), which site‐specific soil and weather properties best estimated corn N needs (i.e., EONR) for two application timings (at‐planting and side‐dress). Included in this investigation was a validation step using an independent dataset. Forty‐nine N response trials conducted across the U.S. Midwest Corn Belt over three growing seasons (2014–2016) were used for recommendation model development, and 181 independent site‐years were used for validation. For HGDC models, soil organic matter (SOM), clay content, and evenness of rainfall distribution before side‐dress N application were the properties generally most helpful in predicting EONR. Using the validation data, model recommendations were within 34 kg N ha–1 of EONR for 37 and 42% of the sites with a root mean square error (RMSE) of 70 and 68 kg N ha–1 for at‐planting and side‐dress applications, respectively. Compared to state‐specific recommendations, sites needing <100 kg N ha–1 or no N were better estimated with HGDC models. In contrast, for sites where EONR was >150 kg N ha–1, HGDC models underestimated N needs compared to state specific. These results show HGDC groupings could aid in developing tools for N fertilizer recommendations.
Monte Carlo simulations for water adsorption in porous materials: Best practices and new insights
Authors: Datar Archit , Witman Matthew , Lin Li‐Chiang 
Published: September 2021

AbstractTechnologies based on water adsorption such as water harvesting from air have tremendous potential in mitigating important global crises such as water scarcity. An important challenge to the deployment of such technologies is finding optimal adsorbent materials. Given the large materials space of available adsorbents, large‐scale computational screening can be extremely helpful for this task. This work explores the methods and details associated with such screening procedures and recommends best practices. We also shed light on the limitations of traditionally used and inexpensive to compute prescreening approaches involving geometric and energetic features to predict water adsorption behavior of porous materials. Such approaches can provide general trends to predict adsorption behavior but may lead to the overlook of potentially important structures due to the complex nature of water adsorption. This study offers insights for future water adsorption simulations to facilitate the development of optimal water adsorbents.
Nicotinamide nucleotide transhydrogenase mutation analysis in Chinese patients with thyroid dysgenesis
Authors: Li Miaomiao , Tian Weibing , Wang Fengqi , Yang Chengyu , Zhang Lu , Tang Qian , Liu Shiguo , Wang Fang 
Published: September 2021

AbstractThyroid dysgenesis (TD) accounts for 80% cases of congenital hypothyroidism, which is the most common neonatal disorder. Until now, the gene mutations have been reported associated with TD can only account for 5% cases, suggesting the genetic heterogeneity of the pathology. Nicotinamide nucleotide transhydrogenase (NNT) plays a crucial role in regulating redox homeostasis, patients carrying NNT mutations have been described with a clinical phenotype of hypothyroidism. As TD risk is increased in the context of several syndromes and redox homeostasis is vital for thyroid development and function, NNT might be a candidate gene involved in syndromic TD. Therefore, we performed target sequencing (TS) in 289 TD patients for causative mutations in NNT and conducted functional analysis of the gene mutations. TS and Sanger sequence were used to screen the novel mutations. For functional analysis, we performed western blot, measurement of NADPH/NADPtotal and H2O2 generation, cell proliferation, and wounding healing assay. As a result, three presumably pathogenic mutations (c.811G > A, p.Ala271Ser; c.2078G > A, p.Arg693His; and c.2581G > A, p.Val861Met) in NNT had been identified. Our results showed the damaging effect of NNT mutations on stability and catalytic activity of proteins and redox balance of cells. In conclusion, our findings provided novel insights into the role of the NNT isotype in thyroid physiopathology and broaden the spectrum of pathogenic genes associated with TD. However, the pathogenic mechanism of NNT in TD is still need to be investigated in further study.
New Hybrid Organic‐inorganic Multifunctional Materials Based on Polydopamine‐like Chemistry
Authors: Calabrese Carla , Liotta Leonarda Francesca , Soumoy Loraine , Aprile Carmela , Giacalone Francesco , Gruttadauria Michelangelo 
Published: September 2021

AbstractA simple one‐pot procedure under mild conditions has been developed with the aim of preparing a set of hybrid organic‐inorganic multifunctional materials. This procedure is based on the use of catechol and KIO4 as oxidizing agent in conjunction with 3‐aminopropyl‐, substituted 3‐aminopropyl‐ and 3‐methylimidazolium‐1‐trimethoxypropylsilane mimicking polydopamine‐like chemistry. Reactions were carried out in water at room temperature and 70 °C to give fifteen materials that were characterised by using several techniques (nitrogen physisorption, TGA, XPS, 13C and 29Si CP‐MAS NMR, IR, pHPZC). Knoevenagel reaction was chosen as a good probe to investigate the availability of functional groups on the surface of the materials. The most active catalytic materials were tested in recycling procedures. Such simple procedure is of broad interest for the scientific community and it open the doors to the development of new hybrid organic‐inorganic multifunctional materials for several purposes.
Oxidative Ritter‐type Chloroamidation of Alkenes Using NaCl and Oxone
Authors: Kato Takehiro , Okada Yuya , Fujii Yuto , Uyanik Muhammet , Ishihara Kazuaki 
Published: September 2021

AbstractWe report a practical and environmentally benign method for the oxidative Ritter‐type chloroamidation of alkenes using sodium chloride and oxone as a chlorinating source and an oxidant, respectively, in acetonitrile under mild conditions. The reaction proceeded smoothly under non‐aqueous conditions without the use of any catalyst. Excellent chemoselectivity (i. e., chloroamidation versus dichlorination) could be achieved for electron‐deficient styrenes. In addition, this protocol could be easily applied to 7‐gram‐scale synthesis.
Putting DNA to Work as Generic Polymeric Materials
Authors: Wang Dong , Liu Peifeng , Luo Dan 
Published: September 2021

AbstractDNA is a true polymer that stores the genetic information of an organism. With its amazing biological and polymeric characteristics, DNA has been regarded as a universal building block for the construction of diverse materials for real‐world applications. Through various approaches including ligation, polymerization, chemical crosslinking, and physical crosslinking, both pure and hybrid DNA gels have been developed as generic materials. This Review discusses recent advances in the construction of DNA‐based networks without considering any of DNA′s genetic properties. In addition, we highlight the biomedical and non‐biomedical applications of DNA as generic materials. Owing to the superb molecular recognition, self‐assembly, and responsiveness of DNA, a mushrooming number of DNA materials with various properties have been developed for general utilization.
Revealing the Side‐Chain‐Dependent Ordering Transition of Highly Crystalline Double‐Cable Conjugated Polymers
Authors: Feng Guitao , Tan Wenliang , Karuthedath Safakath , Li Cheng , Jiao Xuechen , Liu Amelia C. Y. , Venugopal Hariprasad , Tang Zheng , Ye Long , Laquai Frédéric , McNeill Christopher R. , Li Weiwei 
Published: September 2021

AbstractWe developed a series of highly crystalline double‐cable conjugated polymers for application in single‐component organic solar cells (SCOSCs). These polymers contain conjugated backbones as electron donor and pendant perylene bisimide units (PBIs) as electron acceptor. PBIs are connected to the backbone via alkyl units varying from hexyl (C6H12) to eicosyl (C20H40) as flexible linkers. For double‐cable polymers with short linkers, the PBIs tend to stack in a head‐to‐head fashion, resulting in large d‐spacings (e.g. 64 Å for the polymer P12 with C12H24 linker) along the lamellar stacking direction. When the length of the linker groups is longer than a certain length, the PBIs instead adopt a more ordered packing likely via H‐aggregation, resulting in short d‐spacings (e.g. 50 Å for the polymer P16 with C16H32 linker). This work highlights the importance of linker length on the molecular packing of the acceptor units and the influences on the photovoltaic performance of SCOSCs.
Mechanistic Insights Into Iron(II) Bis(pyridyl)amine‐Bipyridine Skeleton for Selective CO2 Photoreduction
Authors: Wang Xu‐Zhe , Meng Shu‐Lin , Chen Jia‐Yi , Wang Hai‐Xu , Wang Yang , Zhou Shuai , Li Xu‐Bing , Liao Rong‐Zhen , Tung Chen‐Ho , Wu Li‐Zhu 
Published: September 2021

AbstractA bis(pyridyl)amine‐bipyridine‐iron(II) framework (Fe(BPAbipy)) of complexes 1–3 is reported to shed light on the multistep nature of CO2 reduction. Herein, photocatalytic conversion of CO2 to CO even at low CO2 concentration (1 %), together with detailed mechanistic study and DFT calculations, reveal that 1 first undergoes two sequential one‐electron transfer affording an intermediate with electron density on both Fe and ligand for CO2 binding over proton. The following 2 H+‐assisted Fe‐CO formation is rate‐determining for selective CO2‐to‐CO reduction. A pendant, proton‐shuttling α‐OH group (2) initiates PCET for predominant H2 evolution, while an α‐OMe group (3) cancels the selectivity control for either CO or H2. The near‐unity selectivity of 1 and 2 enables self‐sorting syngas production at flexible CO/H2 ratios. The unprecedented results from one kind of molecular catalyst skeleton encourage insight into the beauty of advanced multi‐electron and multi‐proton transfer processes for robust CO2RR by photocatalysis.
Enantioselective Construction of Modular and Asymmetric Baskets
Authors: Gunther Michael J. , Pavlović Radoslav Z. , Finnegan Tyler J. , Wang Xiuze , Badjić Jovica D. 
Published: September 2021

AbstractThe precise positioning of functional groups about the inner space of abiotic hosts is a challenging task and of interest for developing more effective receptors and catalysts akin to those found in nature. To address it, we herein report a synthetic methodology for preparing basket‐like cavitands comprised of three different aromatics as side arms with orthogonal esters at the rim for further functionalization. First, enantioenriched A (borochloronorbornene), B (iodobromonorbornene), and C (boronorbornene) building blocks were obtained by stereoselective syntheses. Second, consecutive A‐to‐B and then AB‐to‐C Suzuki–Miyaura (SM) couplings were optimized to give enantioenriched ABC cavitand as the principal product. The robust synthetic protocol allowed us to prepare (a) an enantioenriched basket with three benzene sides and each holding either tBu, Et, or Me esters, (b) both enantiomers of a so‐called “spiral staircase” basket with benzene, naphthalene, and anthracene groups surrounding the inner space, and (c) a photo‐responsive basket bearing one anthracene and two benzene arms.
An overview of iron‐catalyzed N‐alkylation reactions
Authors: Stiniya Sebastian , Saranya Padinjare Veetil , Anilkumar Gopinathan 
Published: September 2021

AbstractN‐containing compounds are very important molecules in nature and in the field of synthetic organic chemistry. N‐alkylation reactions play crucial role in the area of pharmaceuticals and various other industrial chemical syntheses. Iron‐catalyzed N‐alkylation reactions have attained greater acceptance among the scientific community. Environmentally benign, abundant, nontoxic, biocompatible, reusable, and inexpensive iron catalysts are gaining more attention in various research fields. Green protocols, milder reaction conditions, wide substrate scope, and so forth, signify the prominent nature of iron‐catalyzed N‐alkylation reactions. Most of the protocols are eco‐friendly and atom economic since water is the only by‐product. This review gives an overview of the advances in the Fe‐catalyzed N‐alkylation reactions covering literature up to 2021.
High energy conversion composites based on graphene material with excellent healing performances
Authors: Xiao Peishuang , Li Guanghao , Ma Suping , Cai Zhihao , Huang Lu , Huang Yi 
Published: September 2021

AbstractEnergy conversion efficiency is an important characteristic of photothermal self‐healing materials. Herein, reduced graphene oxide‐thermoplastic polyurethane composites (RGO‐TPU) were fabricated via a simple and practical method. The RGO‐TPU composites have a high tensile strength of ~37.4 MPa, and exhibit excellent self‐healing performances under the IR light irradiation, the healing efficiency >99%, the healing time <160 s (IR light power density of 0.2 W/cm2). It is worth mentioning that the photothermal conversion efficiency of the composites was investigated detailedly for the first time with a maximum efficiency of ~32%. Also, theoretical modeling was performed, and the results were in accordance with the experimental results for the influence of the weight fractions of the RGO on their healing performance. That excellent photothermal conversion efficiency indicates that the RGO‐TPU self‐healing composites have promising potential applications in surface protective coatings, medical protective equipment, building materials, military, and so forth.