bluuebunny/crossref_metadata_2025_split huggingface dataset:
Crumpling Carbon‐Pillared Atomic‐Thin Dichalcogenides and CNTs into Elastic Balls as Superior Anodes for Sodium/Potassium‐Ion Batteries
Authors: Zhu Xinxin , Xia Fanjie , Liu Dan , Xiang Xinyuan , Wu Jinsong , Lei Jiaheng , Li Junsheng , Qu Deyu , Liu Jinping 
Published: November 2022

AbstractWith abundant electroactive sites and rapid ion diffusion paths, ultrathin dichalcogenides such as MoS2 demonstrate enormous potential as anodes for sodium/potassium‐ion batteries (SIBs/PIBs). However, ultrahigh‐aspect‐ratio nanosheets are very easy to aggregate and re‐stack, drastically weakening their intrinsic merits. Here a sustainable dichalcogenide anode is designed via crumpling carbon‐pillared atomic‐thin MoS2 nanosheets with CNTs into an elastic ball structure (C‐p‐MoS2/CNTs). In this architecture, the glucose‐derived carbon pillars atomic‐thin MoS2 nanosheets and broadens interlayer spacing, ensuring fast Na+/K+ diffusion; CNTs act as 3D scaffolds to impede re‐stacking of MoS2 while providing high‐speed pathways for electrons; the integration of flexible atomic‐thin sheets and high‐toughness CNTs further endows the balls with great elasticity to release the cycling stress. Consequently, the C‐p‐MoS2/CNTs material delivers high reversible capacities, outstanding cycling stability, and superior rate performance as anodes for both SIBs and PIBs. Pairing with Na3V2(PO4)2F3 cathode, the sodium‐ion coin‐cell could operate at a rate up to 50 C at high mass loading of 9.4 mg cm−2 and manifest ultrastable cycling stability at 40 C over 600 cycles. Impressively, the assembled pouch cell can be cycled stably with a high energy density of 188 Wh kg−1. This study is anticipated to provide inspiration for designing innovative metal dichalcogenides as battery anodes.
Surface Chemistry Determined Electrochemical Sensing Performance of Red Phosphorus and Single Walled Carbon Nanotube Composites
Authors: Liu Lingbo , Lei Ling , Zeng Keni , Wu Kangbing , Yang Nianjun 
Published: November 2022

AbstractRed phosphorus (RP) is a promising electrochemical sensing material owing to its abundant surface groups and reactive sites. In this study, a sodium dodecyl sulfate‐assisted phosphorus‐amine approach is employed to tune surface chemistry of RP nanoparticles. During the transition of the polyphosphorus‐amine anion to RP, the cleavage of POP bond and the formation of POC bond are monitored by in situ attenuated total reflection surface‐enhanced infrared absorption spectroscopy. The formed POC bonds that are originated from the PO reactive sites are theoretically revealed with the density functional theory calculations, charge density difference, and X‐ray photoelectron spectroscopy. The energies of optimized aromatic and aliphatic POC bonds are −2.51 and −2.65 eV, respectively. To explore electrochemical sensing applications, RP nanoparticles are in situ grown on single‐walled carbon nanotube (SWCNT). Such a stable RP/SWCNT suspension is applied to fabricate the RP/SWCNT integrated arrays via a template‐filtration method. Such an array is efficient for sensitive and selective monitoring of p‐phenylenediamine on hair dyes. This study provides insights into surface chemistry of RP, its roles in electrochemical sensing applications, and an approach to produce high‐performance RP sensors at large scales.
Avalanche Coalescence of Liquid Metal Particles for Uniform Flexible and Stretchable Electrodes
Authors: Park Kwangseok , Pyeon Jeongsu , Jeong Seung Hee , Yoon Yong‐Jin , Kim Hyoungsoo 
Published: November 2022

AbstractSelf‐sinterable gallium‐based liquid metal (LM) ink for a handy drop‐casting coating method is developed. The fabricated LM electrode is coffee‐ring‐free and bilayer‐free, which guarantees high electrical conductivity, wettability, flexibility, and stretchability. The ink consists of Galinstan, ethanol‐water mixture, hydrochloric acid, and polyvinylpyrrolidone. The binary mixture provides excellent wetting conditions and suppresses a coffee‐ring stain from Marangoni mixing. The acid removes an oxide layer on the LM interface. The colloidal interaction forces by self‐assembled polyvinylpyrrolidone induce avalanche coalescences of the particles at the end of evaporation, which produces a thin and uniform dried conductive layer. The acid and polymer provide a bilayer‐free structure and electrification without any post sintering. The drop‐casted self‐transformed LM electrode showed excellent electrical resistance of O (0.1–1 Ω) on folding and stretching conditions. It is believed that this method can serve as flexible and stretchable electrodes, on various substances for soft robots and wearable devices, without any complicated post‐process.
Triphenylcarbenium Tetrafluoroborate‐Catalyzed 1,6‐Addition of 1‐Aminobenzotriazole to p‐Quinone Methides: Synthesis of Diarylmethylamines
Authors: Song Ran , Zhuo Caiqi , Si Wen , Wu Xiaoying , Guan Tianyi , Yang Daoshan , Lv Jian 
Published: November 2022

AbstractA metal‐free synthesis of diarylmethylamines via triphenylcarbenium tetrafluoroborate‐catalyzed 1,6‐addition of 1‐aminobenzotriazole to p‐quinone methides (p‐QMs) was developped. Under mild condition, diarylmethylamines could be obtained in moderate to good yields (up to 84%) by simple filtration, showing essentially unchanged activity after 6 reuses.magnified image
Birth defects associated with paternal firefighting in the National Birth Defects Prevention Study
Authors: Siegel Miriam R. , Rocheleau Carissa M. , Hollerbach Brittany S. , Omari Amel , Jahnke Sara A. , Almli Lynn M. , Olshan Andrew F. ,   National Birth Defects Prevention Study
Published: November 2022

AbstractBackgroundFew studies have evaluated birth defects among children of firefighters. We investigated associations between birth defects and paternal work as a firefighter compared to work in non‐firefighting and police officer occupations.MethodsWe analyzed 1997–2011 data from the multi‐site case‐control National Birth Defects Prevention Study. Cases included fetuses or infants with major structural birth defects and controls included a random sample of live‐born infants without major birth defects. Mothers of infants self‐reported information about parents' occupations held during pregnancy. We investigated associations between paternal firefighting and birth defect groups using logistic regression to estimate odds ratios (ORs) and 95% confidence intervals (CIs). Referent groups included families reporting fathers working non‐firefighting and police officer jobs.ResultsOccupational groups included 227 firefighters, 36,285 non‐firefighters, and 433 police officers. Twenty‐nine birth defects were analyzed. In adjusted analyses, fathers of children with total anomalous pulmonary venous return (TAPVR; OR = 3.1; 95% CI = 1.1–8.7), cleft palate (OR = 1.8; 95% CI = 1.0–3.3), cleft lip (OR = 2.2; 95% CI = 1.2–4.2), and transverse limb deficiency (OR = 2.2; 95% CI = 1.1–4.7) were more likely than fathers of controls to be firefighters, versus non‐firefighters. In police‐referent analyses, fathers of children with cleft palate were 2.4 times more likely to be firefighters than fathers of controls (95% CI = 1.1–5.4).ConclusionsPaternal firefighting may be associated with an elevated risk of birth defects in offspring. Additional studies are warranted to replicate these findings. Further research may contribute to a greater understanding of the reproductive health of firefighters and their families for guiding workplace practices.
Bioinspired Gradient Stretchable Aerogels for Ultrabroad‐Range‐Response Pressure‐Sensitive Wearable Electronics and High‐Efficient Separators
Authors: Zhang Xiaoyu , Hu Zhenyu , Sun Qi , Liang Xing , Gu Puzhong , Huang Jia , Zu Guoqing 
Published: November 2022

AbstractBroad‐range‐response pressure‐sensitive wearable electronics are urgently needed but their preparation remains a challenge. Herein, we report unprecedented bioinspired wearable electronics based on stretchable and superelastic reduced graphene oxide/polyurethane nanocomposite aerogels with gradient porous structures by a sol‐gel/hot pressing/freeze casting/ambient pressure drying strategy. The gradient structure with a hot‐pressed layer promotes strain transfer and resistance variation under high pressures, leading to an ultrabroad detection range of 1 Pa–12.6 MPa, one of the broadest ranges ever reported. They can withstand 10 000 compression cycles under 1 MPa, which can't be achieved by traditional flexible pressure sensors. They can be applied for broad‐range‐response electronic skins and monitoring various physical signals/motions and ultrahigh pressures of automobile tires. Moreover, the gradient aerogels can be used as high‐efficient gradient separators for water purification.
Bayesian Self‐Optimization for Telescoped Continuous Flow Synthesis
Authors: Clayton Adam D. , Pyzer‐Knapp Edward O. , Purdie Mark , Jones Martin F. , Barthelme Alexandre , Pavey John , Kapur Nikil , Chamberlain Thomas W. , Blacker A. John , Bourne Richard A. 
Published: November 2022

AbstractThe optimization of multistep chemical syntheses is critical for the rapid development of new pharmaceuticals. However, concatenating individually optimized reactions can lead to inefficient multistep syntheses, owing to chemical interdependencies between the steps. Herein, we develop an automated continuous flow platform for the simultaneous optimization of telescoped reactions. Our approach is applied to a Heck cyclization‐deprotection reaction sequence, used in the synthesis of a precursor for 1‐methyltetrahydroisoquinoline C5 functionalization. A simple method for multipoint sampling with a single online HPLC instrument was designed, enabling accurate quantification of each reaction, and an in‐depth understanding of the reaction pathways. Notably, integration of Bayesian optimization techniques identified an 81 % overall yield in just 14 h, and revealed a favorable competing pathway for formation of the desired product.
Superchaotropic Nano‐ion Binding as a Gelation Motif in Cellulose Ether Solutions
Authors: Hohenschutz Max , Bauduin Pierre , Lopez Carlos G. , Förster Beate , Richtering Walter 
Published: November 2022

AbstractNanometer‐sized anions (nano‐ions) like polyoxometalates and boron clusters exhibit so‐called superchaotropic behavior, which describes their strong binding to hydrated non‐ionic matter in water. We show here that nano‐ions, at millimolar concentrations, dramatically enhance the viscosity and induce gelation of aqueous solutions of non‐ionic cellulose ethers (CEs), a class of widely utilized polymers known for their thickening and gel‐forming ability. These phenomena arise from an interplay of attractive forces and repulsive electrostatic forces between CE‐chains upon nano‐ion binding. The attractive forces manifest themselves as aggregation of CE‐chains into a physically crosslinked polymer network (gel). In turn, the electrostatic repulsions hamper the viscosity increase and gelation. Superchaotropic nano‐ion binding emerges as a novel and general physical crosslinking motif for CE‐solutions and exceeds by far the conventional thickening effects of classical salts and ionic surfactants.
Circularly Polarized Light Probes Excited‐State Delocalization in Rectangular Ladder‐type Pentaphenyl Helices
Authors: Ammenhäuser Robin , Klein Patrick , Schmid Eva , Streicher Sabrina , Vogelsang Jan , Lehmann Christian W. , Lupton John M. , Meskers Stefan C. J. , Scherf Ullrich 
Published: November 2022

AbstractLadder‐type pentaphenyl chromophores have a rigid, planar π‐system and show bright fluorescence featuring pronounced vibrational structure. Such moieties are ideal for studying interchromophoric interactions and delocalization of electronic excitations. We report the synthesis of helical polymers with a rigid square structure based on spiro‐linked ladder‐type pentaphenyl units. The variation of circular dichroism with increasing chain length provides direct evidence for delocalization of electronic excitations over at least 10 monomeric units. The change in the degree of circular polarization of the fluorescence across the vibronic side bands shows that vibrational motion can localize the excitation dynamically to almost one single unit through breakdown of the Born‐Oppenheimer approximation. The dynamic conversion between delocalized and localized excited states provides a new paradigm for interpreting circular dichroism in helical polymers such as proteins and polynucleic acids.
An Amorphous n‐Type Conjugated Polymer with an Ultra‐Rigid Planar Backbone
Authors: Cao Xu , Li Hongxiang , Hu Junli , Tian Hongkun , Han Yanchun , Meng Bin , Liu Jun , Wang Lixiang 
Published: November 2022

AbstractHigh charge carrier mobility polymer semiconductors are always semi‐crystalline. Amorphous conjugated polymers represent another kind of polymer semiconductors with different charge transporting mechanism. Here we report the first near‐amorphous n‐type conjugated polymer with decent electron mobility, which features a remarkably rigid, straight and planar polymer backbone. The molecular design strategy is to copolymerize two fused‐ring building blocks which are both electron‐accepting, centrosymmetrical and planar. The polymer is the alternating copolymer of double B←N bridged bipyridine (BNBP) unit and benzobisthiazole (BBTz) unit. It shows a decent electron mobility of 0.34 cm2 V−1 s−1 in organic field‐effect transistors. The excellent electron transporting property of the polymer is possibly due to the ultrahigh backbone stiffness, small π‐π stacking distance, and high molecular weight.
Diboron(4)‐Catalyzed Remote [3+2] Cycloaddition of Cyclopropanes via Dearomative/Rearomative Radical Transmission through Pyridine
Authors: Xu Ming , Wang Zhijun , Sun Zhaohui , Ouyang Yizhao , Ding Zhengwei , Yu Tao , Xu Liang , Li Pengfei 
Published: November 2022

AbstractRing structures such as pyridine, cyclopentane or their combinations are important motifs in bioactive molecules. In contrast to previous cycloaddition reactions that necessitated a directly bonded initiating functional group, this work demonstrated a novel through‐(hetero)arene radical transmission concept for selective activation of a remote bond. An efficient, metal‐free and atom‐economical [3+2] cycloaddition between 4‐pyridinyl cyclopropanes and alkenes or alkynes has been developed for modular synthesis of pyridine‐substituted cyclopentanes, cyclopentenes and bicyclo[2.1.1]hexanes that are difficult to access using known methods. This complexity‐building reaction was catalyzed by a very simple and inexpensive diboron(4) compound and took place via dearomative/rearomative processes. The substrate scope was broad and more than 100 new compounds were prepared in generally high yields. Mechanistic experiments and density function theory (DFT) investigation supported a radical relay catalytic cycle involving alkylidene dihydropyridine radical intermediates and boronyl radical transfer.
Enantioselective Hydrosilylation of β,β‐Disubstituted Enamides to Construct α‐Aminosilanes with Vicinal Stereocenters
Authors: Zhang Wen‐Wen , Li Bi‐Jie 
Published: November 2022

AbstractDespite the advances in the area of catalytic alkene hydrosilylation, the enantioselective hydrosilylation of alkenes bearing a heteroatom substituent is scarce. Here we report a rhodium‐catalyzed hydrosilylation of β,β‐disubstituted enamides to directly afford valuable α‐aminosilanes in a highly regio‐, diastereo‐, and enantioselective manner. Stereodivergent synthesis could be achieved by regulating substrate geometry and ligand configuration to generate all the possible stereoisomers in high enantio‐purity.
Conformational Control of Organocatalyst in Strongly Brønsted‐Acidic Metal‐Organic Frameworks for Enantioselective Catalysis
Authors: Jiang Hong , Zhao Xiangxiang , Zhang Wenqiang , Liu Yan , Li Haiyang , Cui Yong 
Published: November 2022

AbstractChiral imidodiphosphates (IDPs) have emerged as strong Brønsted acid catalysts for many enantioselective processes. However, the dynamic transformation between O,O‐syn and O,O‐anti conformers typically results in low enantioselectivity. Here we demonstrate that topologies of metal‐organic frameworks (MOFs) can be exploited to control IDP conformations and local chiral microenvironments for enantioselective catalysis. Two porous Dy‐MOFs with different topologies are obtained from an enantiopure 1,1′‐biphenol IDP‐based tetracarboxylate ligand. While the ligand adopts a 4‐ or 3‐connected (c) binding mode, all IDPs are rigidified to get only a single O,O‐syn conformation and display greatly enhanced Brønsted acidity relative to the free IDP. The MOF with the 4‐c IDP that has a relatively less compact shape than the 3‐c IDP can be an efficient and recyclable heterogeneous Brønsted acid catalysing the challenging asymmetric O,O‐acetalization reaction with up to 96 % enantiomeric excess.
Catalytic, Regioselective 1,4‐Fluorodifunctionalization of Dienes
Authors: Yu You‐Jie , Schäfer Michael , Daniliuc Constantin G. , Gilmour Ryan 
Published: November 2022

AbstractA catalysis‐based regioselective 1,4‐fluorofunctionalization of trifluoromethyl substituted 1,3‐dienes has been developed to access compact, highly functionalized products. The process allows E,Z‐mixed dienes to be processed to a single E‐alkene isomer, and leverages an inexpensive and operationally convenient I(I)/I(III) catalysis platform. The first example of catalytic 1,4‐difluorination is disclosed and subsequently evolved to enable 1,4‐hetero‐difunctionalization, which allows δ‐fluoro‐alcohol and amine derivatives to be forged in a single operation. The protocol is compatible with a variety of nucleophiles including fluoride, nitriles, carboxylic acids, alcohols and even water thereby allowing highly functionalized products, with a stereocenter bearing both C(sp3)−F and C(sp3)−CF3 groups, to be generated rapidly. Scalability (up to 3 mmol), and facile post‐reaction modifications are demonstrated to underscore the utility of the method in expanding organofluorine chemical space.
The structure and priorities of researchers' scholarly profile maintenance activities: A case of institutional research information management system
Authors: Lee Dong Joon , Stvilia Besiki , Ha Seungyeon , Hahn Douglas 
Published: November 2022

AbstractResearch information management systems (RIMS) have become critical components of information technology infrastructure on university campuses. They are used not just for sharing and promoting faculty research, but also for conducting faculty evaluation and development, facilitating research collaborations, identifying mentors for student projects, and expert consultants for local businesses. This study is one of the first empirical investigations of the structure of researchers' scholarly profile maintenance activities in a nonmandatory institutional RIMS. By analyzing the RIMS's log data, we identified 11 tasks researchers performed when updating their profiles. These tasks were further grouped into three activities: (a) adding publication, (b) enhancing researcher identity, and (c) improving research discoverability. In addition, we found that junior researchers and female researchers were more engaged in maintaining their RIMS profiles than senior researchers and male researchers. The results provide insights for designing profile maintenance action templates for institutional RIMS that are tailored to researchers' characteristics and help enhance researchers' engagement in the curation of their research information. This also suggests that female and junior researchers can serve as early adopters of institutional RIMS.
Recent Advances of ZnCo2O4‐based Anode Materials for Li‐ion Batteries
Authors: Han Meng‐Cheng , Zou Ming‐ci , Yi Ting‐Feng , Wei Feng 
Published: November 2022

AbstractZnCo2O4 has been attracted wide research attention as a promising anode material for lithium‐ion batteries (LIBs) in recent years based on its high theoretical specific capacity, low toxicity as well as stable chemical properties. However, the further large‐scale application of pristine ZnCo2O4 anode have been impeded because of its undesirable Li+ ion conductivity, low electronic conductivity, and finite stability of electrolytes at high potentials. Recently, optimizing the micro/nano structure, modification with carbonaceous materials, incorporation with metal oxides and constructing a binder‐free structure on conductive substrate for ZnCo2O4‐based materials have been verified as promising effective routes for solving the above problems. In this review, the recent advances in underlying reaction mechanisms, synthetic methods and strategies for improving the performance of ZnCo2O4 anodes are comprehensively summarized. The factors affecting the electrochemical properties of ZnCo2O4‐based materials are mainly discussed, and paths to promote the specific capacity and cyclic stability are proposed. Finally, several insights into the future developments, challenges, and prospects of ZnCo2O4‐based anode materials of LIBs are proposed.
Survival of infants and children born with severe microcephaly, Texas, 1999–2015
Authors: Marengo Lisa K. , Archer Natalie , Shumate Charlie , Canfield Mark A. , Drummond‐Borg Margaret 
Published: November 2022

AbstractBackgroundSevere microcephaly is a brain reduction defect where the delivery head circumference is <3rd percentile for gestational age and sex with subsequent lifelong morbidities. Our objective was to evaluate survival among 2,704 Texas infants with severe microcephaly delivered 1999–2015.MethodsInfants with severe microcephaly from the Texas Birth Defects Registry were linked to death certificates and the national death index. Survival estimates, hazard ratios (HR) and confidence intervals (CI) were calculated using the Kaplan–Meier method and Cox proportional hazards models stratified by presence versus absence of co‐occurring defects.ResultsWe identified 496 deaths by age 4 years; most (42.9%) occurred in the neonatal period, and another 39.9% died by 1 year of age. Overall infant survival was 84.8%. Lowest infant survival subgroups included those with chromosomal/syndromic conditions (66.1%), very preterm deliveries (63.9%), or co‐occurring critical congenital heart defects (44.0%). Among infants with severe microcephaly and a chromosomal/syndromic co‐occurring defect, the risk of death was nearly three‐fold higher among those with: proportionate microcephaly (i.e., small baby overall), relative to non‐proportionate (HR = 2.84, 95% CI = 2.17–3.71); low‐birthweight relative to normal (HR = 2.72, 95% CI = 1.92–3.85); critical congenital heart defects (CCHD) relative to no CCHD (HR = 2.90, 95% CI = 2.20–3.80). Trisomies were a leading underlying cause of death (27.5%).ConclusionsOverall, infants with severe microcephaly had high 4‐year survival rates which varied by the presence of co‐occurring defects. Infants with co‐occurring chromosomal/syndromic anomalies have a higher risk of death by age one than those without any co‐occurring birth defects.