bluuebunny/crossref_metadata_2025_split huggingface dataset:
2D VOPO4 Pseudocapacitive Ultrafast‐Charging Cathode with Multi‐Electron Chemistry for High‐Energy and High‐Power Solid‐State Lithium Metal Batteries
Authors: Xing Feifei , Su Feng , Qin Jieqiong , Wen Pengchao , Li Yuejiao , Zhang Liangzhu , Ma Jiaxin , Zheng Shuanghao , Guo Xin , Wu Zhong‐Shuai 
Published: April 2023

AbstractLithium metal batteries (LMBs) are acknowledged to be one major direction for next‐generation energy storage devices. However, the practical applications of LMBs are certainly limited by the low power density and safety issues owing to the lack of high‐capacity pseudocapacitive cathode materials and solid electrolytes. Herein, the rational synthesis of 2D VOPO4 nanosheets with enriched V4+ defects (VOPO4@G‐Air) enabling ultrafast multi‐electron reactions as a high‐capacity pseudocapacitive cathode is reported. Through V4+ defect engineering, the larger polarizationand inhomogeneous multi‐electron reactions are vastly improved, resulting in remarkably fast kinetics. Benefiting from the ultrathin 2D structure and controllably regulated V4+ defect concentration, a high discharge capacity of 313 mA h g−1at 0.1C is achieved, anda large capacity of 116 mA h g−1 is offered at 50C. Finally, utilizing the as‐synthesized VOPO4@G‐Air and a solid‐state electrolyte based on ethoxylated trimethylolpropane triacrylate (ETPTA‐LiClO4‐SSE) , the assembled solid‐state LMBs (Li||ETPTA‐LiClO4‐SSE||VOPO4) show high energy density of 85.4 Wh kg−1 at 114.5 W kg−1 and high power density of 2.3 kW kg−1 at 45.86 Wh kg−1. Further, the pouch cell unveils extraordinary safety and excellent flexibility. This work provides new insights in the construction of ultrafast and high‐capacity pseudocapacitive cathodes with multi‐electron reactions for solid‐state LMBs.
Accelerated Discovery of Advanced Thermoelectric Materials via Transfer Learning
Authors: Li Mengke , Yuan Hongmei , Luo Yufeng , Ma Xiaoyi , Liu Huijun , Jiang Wentao , Fang Ying 
Published: April 2023

AbstractThermoelectric (TE) technology can realize direct conversion of widely distributed heat into useful electricity, which provides a promising route to solve the global energy crisis that is increasingly severe. However, it is extremely complex and time‐consuming to discover advanced TE materials via conventional trial‐and‐error approaches. In this work, using a pre‐trained neural network architecture for the electronic bandgap, a transfer learning (TL) strategy that allows ready and accurate prediction on the ZT values of any TE materials at arbitrary temperature is proposed. Compared with direct machine learning algorithms, the TL‐driven model exhibits significantly enhanced predictive power beyond the initial dataset, as characterized by improved Pearson correlation coefficient (reduced mean absolute error) from 23% to 95% (0.35 to 0.07) for the p‐type systems, and 46% to 94% (0.23 to 0.06) for the n‐type systems. By screening 6353 possible candidates in the AFLOW repository that having relatively smaller gaps, 925 p‐type and 788 n‐type systems are quickly identified to exhibit ZT exceeding 2.0. Equally importantly, the established TL model is highly adaptable to ZT prediction in an even larger search space, where the constituent atoms and/or stoichiometric compositions of the screened systems may be variously tuned to further optimize their TE performance.
Engineering Peculiar Cathode Electrolyte Interphase toward Sustainable and High‐Rate Li–S Batteries
Authors: Qiu Chang‐Ding , Hu Youcheng , Cao Kewei , Wu Xiangjiang , Huang Bi‐Hong , Liu Jin , Wang Yun‐Xiao , Luo Laibing , Gu Dong , Ai Xinping , Cao Yuliang , Chen Shengli , Ke Fu‐Sheng 
Published: April 2023

AbstractThe lithium–sulfur battery is considered to be one of the most promising rechargeable energy storage systems because of its high theoretical energy density. Unfortunately, the shuttle effect during cycling causes serious loss of sulfur species and corrosion of the lithium metal anode, resulting in severe capacity decay. This work proposes to completely suppress the shuttle effect of lithium polysulfides (LiPSs) without sacrificing the interfacial Li+ transport, through in situ construction of a compact cathode electrolyte interphase (CEI), which is formed of the reaction between vinylene carbonate (VC), bis(trifluoromethane)sulfonimide ions and LiPSs in a self‐limiting manner during the initial discharge process. Hence, the CEI‐confined sulfur cathode in the VC‐based electrolyte with a solid phase conversion mechanism delivers a long‐term cycling stability and high‐rate performance, as well as excellent performance under an extreme climate in a subzero temperature of −20 °C, limited lithium source with a low N/P ratio of 1.1, and even at mechanical mutilation. The present study reveals an appealing approach to tailor the composition and interfacial structure of sulfur cathodes by in situ construction of a robust, self‐healing, and high Li+ conductive CEI from the aspect of electrolyte, and thus completely solve the issue of the shuttle effect.
C−H Functionalized Molecules: Synthesis, Reaction Mechanism, and Biological Activity
Authors: Tandon Nitin , Thakur Rekha , Tandon Runjhun , Singh Iqubal , Paul Kamaldeep , Ahmad Bhat Aeyaz 
Published: April 2023

AbstractReplacement of traditionally unreactive C−H bond with C−C or C−X (X=Hetero atom) has emerged as one of the widely accepted methods over the last few decades for the synthesis of complex organic molecules which can act as important intermediates for the synthesis of biologically active compounds. Selective functionalization of the C−H bond especially in the presence of a more reactive C−H bond has remained one of the biggest challenges for synthetic organic chemists. The hybridization state of the C−H bond, substitution pattern, and presence of directive groups are some of the factors which have been exploited by researchers over the years for achieving fruitful results. A considerable amount of work has been reported in the literature on the use of metal catalysts for C−H bond functionalization leading to the formation of a C−M (carbon‐metal) bond which is also known as C−H bond activation. This review aims to summarize various synthetic strategies reported for the C−H functionalization, which has led to the development of targeted complex molecules with medicinal properties.
Impact of multivitamin‐mineral and cocoa extract on incidence of mild cognitive impairment and dementia: Results from the COcoa Supplement and Multivitamin Outcomes Study for the Mind (COSMOS‐Mind)
Authors: Sachs Bonnie C. , Williams Benjamin J. , Gaussoin Sarah A. , Baker Laura D. , Manson JoAnn E. , Espeland Mark A. , Sesso Howard D. , Shumaker Sally A. , Rapp Stephen R. ,   for the COSMOS‐Mind Research Group
Published: April 2023

AbstractINTRODUCTIONWe assessed the effects of multivitamin‐mineral and cocoa extract supplementation on incident mild cognitive impairment (MCI) and all‐cause probable dementia.METHODSCOSMOS‐Mind (N = 2262), a 2 × 2 factorial, randomized‐controlled clinical trial administered a telephone‐based cognitive battery at baseline and annually for 3 years. Incidence rates of MCI, and separately dementia, were compared among treatment arms with proportional hazards regression.RESULTSOver 3 years, 110 incident MCI and 14 incident dementia cases were adjudicated. Incidence rates did not vary by assignment to multivitamin‐mineral or cocoa extract (all p’s ≥ 0.05); however, statistical power was low. When participants assigned to multivitamin‐mineral versus placebo converted to MCI, their scores for global cognition (p = 0.03) and executive function (p < 0.001) were higher and had declined less relative to the previous year (p = 0.03 for global cognition; p = 0.004 for executive function).DISCUSSIONMultivitamin‐mineral therapy may provide cognitive resilience, countering conversion to MCI, but not significantly reduce its incidence over 3 years.Highlights
Multivitamin‐mineral supplementation did not reduce risks for cognitive impairment.
Cocoa extract supplementation did not reduce risks for cognitive impairment.
Multivitamin‐mineral supplementation slowed cognitive declines for incident mild cognitive impairment.
Hydrogen Isotope Exchange by Homogeneous Iridium Catalysis in Aqueous Buffers with Deuterium or Tritium Gas
Authors: Stork Carla Marie , Weck Remo , Valero Mégane , Kramp Henrik , Güssregen Stefan , Waldvogel Siegfried R. , Sib Anna , Derdau Volker 
Published: April 2023

AbstractWe have studied the highly selective homogeneous iridium‐catalyzed hydrogen isotope exchange (HIE) with deuterium or tritium gas as an isotope source in water and buffers. With an improved water‐soluble Kerr‐type catalyst, we have achieved the first insight into applying HIE reactions in aqueous media with varying pH. Density functional theory (DFT) calculations gave consistent insights in the calculated energies of transition states and coordination complexes, further explaining the observed reactivity and guidance on the scope and limitations for HIE reactions in water. Finally, we successfully adapted these findings to tritium chemistry.
Characterization and mechanism of natural rubber composites reinforced by modified calcium sulfate whisker
Authors: Qi Yuanhao , Wu Jinxiu , Qin Sicheng , Liu Zhaogang , Hu Yanhong , Zhang Xiaowei , Li Jianfei , Feng Fushan 
Published: April 2023

AbstractThis study concentrated on the mechanical properties of natural rubber (NR) composites [modified calcium sulfate whisker (MCSW)] and the reinforcement mechanism of MCSW on NR. First, anhydrous CSW with an orthogonal crystal system bottom center structure was prepared by hydrothermal method. Subsequently, MCSW was obtained by treating whiskers with inorganic, organic compounds, which effectively coated the surface of the whiskers with an average thickness of 40.85 nm, making the surface change from hydrophilic to hydrophobic. The CSW/MCSW filler was added to the NR under the optimum experimental conditions of 70°C, 12 min, 5 times of rolling, 140°C, and 1 h of curing time. The results showed that the tensile strength, elongation at break, and crosslink density of the NR composites with 15 phr of MCSW added were increased by 80.8%, 9.0%, and 80.2%, respectively, compared with the NR without the filler. The mechanism of MCSW improving the performance of composites was revealed from vulcanization kinetics and interfacial thermodynamics. In this work, a new type of high‐efficiency environmental protection NR filler reinforcing agent was developed.
Efficacy of very early interventions on neurodevelopmental outcomes for infants and toddlers at increased likelihood of or diagnosed with autism: A systematic review and meta‐analysis
Authors: McGlade Andrea , Whittingham Koa , Barfoot Jacqui , Taylor Leisa , Boyd Roslyn N. 
Published: April 2023

AbstractThe aim of this systematic review was to determine the efficacy of very early interventions for infants and toddlers at increased likelihood of or diagnosed with autism for autism symptomatology, developmental outcomes and/or neurocognitive markers. Eight databases were searched (14 April 2022) with inclusion criteria: (i) RCTs with care as usual (CAU) comparison group, (ii) participants at increased likelihood of or diagnosed with autism and aged <24 months corrected age (CA), (iii) parent‐mediated and/or clinician directed interventions, and (iv) outcome measures were autism symptomatology, cognition, language, adaptive skills, or neurocognitive assessments (EEG and eye tracking). Quality was assessed using Risk of Bias 2 and GRADE. Nineteen publications from 12 studies reported on 715 infants and toddlers. There was low to moderate certainty evidence that clinician‐assessed outcomes did not show significant treatment effects for: autism symptomatology (ADOS CSS: MD −0.08, 95% CI −0.61, 0.44, p = 0.75), cognitive outcome (Mullen Scales of Early Learning‐Early Learning Composite (MSEL‐ELC): SMD 0.05, 95% CI −0.19, 0.29, p = 0.67), receptive language (MSEL—Receptive Language: SMD 0.04, 95% CI −0.21, 0.3, p = 0.74) or expressive language (MSEL‐Expressive Language: SMD 0.06, 95% CI −0.1, 0.23, p = 0.45). Neurocognitive outcomes (EEG and eye tracking) were heterogeneous, with inconsistent findings. There is low to moderate certainty evidence that very early interventions have limited impact on neurodevelopmental outcomes by age 3 years.
A Long Cycle Life Zinc‐Iodide Flow Battery Enabled by a Multifunctional Low Cost Supporting Electrolyte
Authors: Chakraborty Monalisa , Andreu Teresa , Guc Maxim , Amazian Mohamed , Murcia‐López Sebastián 
Published: April 2023

AbstractHigh energy density and cost‐effective zinc‐iodide flow battery (ZIFB) offers great promise for future grid‐scale energy storage. However, its practical performance is hindered by poor cyclability, because of irreversible zinc plating/stripping, slow kinetics of redox reactions, and solid I2 precipitation. Herein, we report NaCl‐supported electrolyte chemistry to address these issues simultaneously. The formation of soluble chloride anions by coordination interactions between Zn2+ and Cl−, are key factor for the improvement of Zn/Zn2+ redox reversibility. While formation of soluble I2Cl− complex stabilizes ZIFB from I2 precipitation, participation of Na+ and K+ as dominant migrating carriers passing through Nafion, restricts Zn2+ migration, thus, blocking electrolyte crossover. A ZIFB with this improved electrolyte stably cycled 100 times with excellent capacity retention and energy efficiency at 20 mA cm−2, while conventional ZIFB shows the trend of capacity fade from 10th cycle onwards. These encouraging results of NaCl‐added electrolyte chemistry enlighten great prospects for high‐performance ZIFB applications.
Economic evaluation of Optilume, a drug‐coated balloon for recurrent anterior male urethral stricture
Authors: Kelly Laura , Shore Judith , Wright James , Patrick Craig , Holmes Hayden 
Published: April 2023

AbstractObjectivesWe aim to conduct an economic evaluation of the Optilume urethral drug‐coated balloon (DCB) compared with endoscopic management for the treatment of recurrent anterior male urethral stricture in England.Patients and MethodsA cohort Markov model was developed to estimate the costs and savings to the NHS over a 5‐year time horizon of adopting Optilume for the treatment of anterior urethral male stricture versus current endoscopic standard of care. A scenario analysis was conducted which compared Optilume to urethroplasty. Probabilistic and deterministic sensitivity analyses were performed to estimate the impact of uncertainties in model parameters.ResultsWhen compared with current endoscopic standard of care Optilume resulted in an estimated cost saving of £2502 per patient if introduced in the NHS for the treatment of recurrent anterior male urethral stricture. In the scenario analysis, the use of Optilume compared with urethroplasty resulted in an estimated cost saving of £243. Results were robust to changes in individual input parameters as demonstrated in the deterministic sensitivity analyses, with the monthly probability of symptom recurrence associated with endoscopic management the only exception. Probabilistic sensitivity analysis results demonstrated that Optilume was cost saving in 93.4% of model iterations, when running 1000 iterations.ConclusionOur analysis suggests that the Optilume urethral DCB treatment can be a cost‐saving alternative management option for the treatment of recurrent anterior male urethral stricture within the NHS in England.
A hidden Markov model for continuous longitudinal data with missing responses and dropout
Authors: Pandolfi Silvia , Bartolucci Francesco , Pennoni Fulvia 
Published: April 2023

AbstractWe propose a hidden Markov model for multivariate continuous longitudinal responses with covariates that accounts for three different types of missing pattern: (I) partially missing outcomes at a given time occasion, (II) completely missing outcomes at a given time occasion (intermittent pattern), and (III) dropout before the end of the period of observation (monotone pattern). The missing‐at‐random (MAR) assumption is formulated to deal with the first two types of missingness, while to account for the informative dropout, we rely on an extra absorbing state. Estimation of the model parameters is based on the maximum likelihood method that is implemented by an expectation‐maximization (EM) algorithm relying on suitable recursions. The proposal is illustrated by a Monte Carlo simulation study and an application based on historical data on primary biliary cholangitis.
Impact of coronary artery disease on clinical outcomes after TAVR: Insights from the BRAVO‐3 randomized trial
Authors: Feldman Daniel , Cao Davide , Sartori Samantha , Zhang Zhongjie , Hengstenberg Christian , Tron Christophe , Anthopoulos Prodromos , Widder Julian D. , Meneveau Nicolas , Stella Pieter R. , Ferrari Markus , Jeger Raban , Violini Roberto , Dumonteil Nicolas , Chen Shiwei , Yan Ruiqi , Nicolas Johny , Razuk Victor , Spirito Alessandro , Vogel Birgit , Mehran Roxana , Dangas George 
Published: April 2023

AbstractObjectiveTo determine the prognostic impact of coronary artery disease (CAD) in patients randomized to bivalirudin or unfractionated heparin (UFH) during transcatheter aortic valve replacement (TAVR).BackgroundCAD is a common comorbidity among patients undergoing TAVR and studies provide conflicting data on its prognostic impact.MethodsThe Bivalirudin on Aortic Valve Intervention Outcomes‐3 (BRAVO‐3) randomized trial compared the use of bivalirudin versus UFH in 802 high‐surgical risk patients undergoing transfemoral TAVR for severe symptomatic aortic stenosis. Patients were stratified according to the presence or absence of history of CAD as well as periprocedural anticoagulation. The coprimary endpoints were net adverse cardiac events (NACE; a composite of all‐cause mortality, myocardial infarction, stroke, or major bleeding) and major Bleeding Academic Research Consortium (BARC) bleeding ≥3b at 30 days postprocedure.ResultsAmong 801 patients, 437 (54.6%) had history of CAD of whom 223 (51.0%) received bivalirudin. There were no significant differences in NACE (adjusted odds ratio [OR]: 1.04; 95% confidence interval [CI]: 0.69–1.58) or BARC ≥ 3b bleeding (adjusted OR: 0.84; 95% CI: 0.51–1.39) in patients with vs without CAD at 30 days. Among CAD patients, periprocedural use of bivalirudin was associated with similar NACE (OR: 0.80; 95% CI: 0.47–1.35) and BARC ≥ 3b bleeding (OR: 0.64; 95% CI: 0.33–1.25) compared with UFH, irrespective of history of CAD (p‐interaction = 0.959 for NACE; p‐interaction = 0.479 for major bleeding).ConclusionCAD was not associated with a higher short‐term risk of NACE or major bleeding after TAVR. Periprocedural anticoagulation with bivalirudin did not show any advantage over UFH in patients with and without CAD.
The Synergistic Promotion Effect of In‐situ Formed Metal Cationic Vacancies and Interstitial Metals on Photocatalytic Performance of WO3 in CO2 Reduction
Authors: Chen Mingfeng , Mao Yunhang , Zhang Haotian , Ren Manman , Wu Daiqun , Zhao Xin , Tu Weixia 
Published: April 2023

AbstractMicrostructure modulation of photocatalysts is an effective way to improve photocatalytic performances. The synergistic effect of metal cationic vacancies and interstitial metals on photocatalysts is rarely studied. In‐situ formations of metal cationic vacancies and interstitial metals are achieved in WO3 via acid treatments, resulting from the migration of metal impurities in WO3. Characterizations of structures, components, photo‐responsive and photoelectric properties identify the differences of WO3 photocatalysts via different treatments. The presence of both metal cationic vacancies and interstitial metal impurities exhibits the positive synergistic effect in photocatalytic reaction. Photocatalytic activities in CO2 reduction are enhanced with the high production rates of CO and CH4. Experimental characterizations of WO3 photocatalysts indicate the increased photoinduced electrons and photocurrent intensities, and the decreased electrochemical impedances. Theoretical simulations confirm the changes of electronic structures of WO3. The calculated band gaps of WO3 after acid treatment decrease and the defect energy levels form, which favor the separation and the transfer of photoinduced carriers for the promotion of photocatalytic activities. To utilize the dissolution difference of metals is feasible to fabricate metal cationic vacancies and interstitial metals simultaneously, an option for other metal‐containing photocatalysts with the in‐situ introduced impurities.
Spontaneous Chiral Resolution of a MnIIISpin‐Crossover Complex with High Temperature 80 K Hysteresis
Authors: Kelly Conor T. , Jordan Ross , Felton Solveig , Müller‐Bunz Helge , Morgan Grace G. 
Published: April 2023

AbstractNon‐centrosymmetric spin‐switchable systems are of interest for their prospective applications as magnetically active non‐linear optical materials and in multiferroic devices. Chiral resolution of simple spin‐crossover chelate complexes into the Δ and Λ forms offers a facile route to homochiral magnetic switches, which could be easily enantiomerically enriched. Here, we report the spontaneous resolution of a new hysteretic spin‐crossover complex, [MnIII(sal2323)]SCN ⋅ EtOH (1), into Δ and Λ forms, without the use of chiral reagents, where sal2323 is a Schiff base resulting from condensation of 1,2‐bis(3‐aminopropylamino)ethane with 2‐hydroxybenzaldehyde. The enantiopurity of the Δ and Λ isomers was confirmed by single crystal X‐ray diffraction and circular dichroism. Quantum chemistry calculations were used to investigate the electronic structure. The opening of a wide 80 K thermal hysteresis window at high temperature highlights the potential for good magneto‐optical function at ambient temperature for materials of this type.
Capillary‐Bridge Controlled Patterning of BTR:PC71BM Bulk Heterojunction Micro Arrays towards High‐Performance Photodetector
Authors: Yue Yuchen , Su Zhaoqing , Zheng Bing , Huo Lijun , Wang Jingxia , Jiang Lei 
Published: April 2023

AbstractThe patterning strategy of organic semiconductors is a crucial issue for integrated circuit. However, due to the uncontrollable liquid dewetting, most of the research is mainly focused on the patterning of single component, few works have been done on the patterning of multi‐component or heterojunction, which play an important role in optoelectronic devices. Therefore, a capillary‐bridge strategy was introduced for patterning of bulk heterojunction (BHJ) micro‐arrays, with liquid crystalline BTR and PC71BM utilized as donor and acceptor, respectively. The BTR:PC71BM arrays presented hierarchical morphology with suitable phase separation, which contributes to the efficient charge generation and transport. Moreover, the photodetector exhibited excellent performance with the light on/off ratio greater than 2000, the responsivity of 40.57 A W−1, and specific detectivity of 2.15×1012 Jones. Such progress demonstrates that the capillary‐bridge strategy is a promising approach for the fabrication of high‐quality BHJ micropatterns arrays.
Fe(III)‐Catalyzed Aerobic Oxidation of 1,4‐Diols†
Authors: Li Junlin , Liu Jinxian , Fu Chunling , Ma Shengming 
Published: April 2023

Comprehensive SummaryAerobic oxidation has been catching more and more attention because of its atom economy and environmental friendliness. Oxidation of diols is a challenge due to various oxidative products. Thus, highly selective aerobic oxidation affording specific products is of current interest. In this work, a combination of Fe(NO3)3·9H2O/TEMPO/KCl catalysis has been identified as an efficient recipe for the aerobic oxidation of 1,4‐diols affording γ‐butyrolactones under mild conditions. The reaction exhibits decent chemo‐ and regioselectivity of symmetrical and unsymmetrical 1,4‐diols. The optically active γ‐lactones may also be prepared from optically active 1,4‐diols without erosion of the ee via this method. Furthermore, this approach was successfully applied to synthesize NBP, a commercial drug.