bluuebunny/crossref_metadata_2025_split huggingface dataset:
Controlling CO2 Hydrogenation Selectivity by Metal‐Supported Electron Transfer
Authors: Li Xiaoyu , Lin Jian , Li Lin , Huang Yike , Pan Xiaoli , Collins Sebastián E. , Ren Yujing , Su Yang , Kang Leilei , Liu Xiaoyan , Zhou Yanliang , Wang Hua , Wang Aiqin , Qiao Botao , Wang Xiaodong , Zhang Tao 
Published: July 2020

AbstractTuning CO2 hydrogenation selectivity to obtain targeted value‐added chemicals and fuels has attracted increasing attention. However, a fundamental understanding of the way to control the selectivity is still lacking, posing a challenge in catalyst design and development. Herein, we report our new discovery in ambient pressure CO2 hydrogenation reaction where selectivity can be completely reversed by simply changing the crystal phases of TiO2 support (anatase‐ or rutile‐TiO2) or changing metal loadings on anatase‐TiO2. Operando spectroscopy and NAP‐XPS studies reveal that the determining factor is a different electron transfer from metal to the support, most probably as a result of the different extents of hydrogen spillover, which changes the adsorption and activation of the intermediate of CO. Based on this new finding, we can not only regulate CO2 hydrogenation selectivity but also tune catalytic performance in other important reactions, thus opening up a door for efficient catalyst development by rational design.
A Non‐Conjugated Polymer Acceptor for Efficient and Thermally Stable All‐Polymer Solar Cells
Authors: Fan Qunping , Su Wenyan , Chen Shanshan , Liu Tao , Zhuang Wenliu , Ma Ruijie , Wen Xin , Yin Zhihong , Luo Zhenghui , Guo Xia , Hou Lintao , Moth‐Poulsen Kasper , Li Yu , Zhang Zhiguo , Yang Changduk , Yu Donghong , Yan He , Zhang Maojie , Wang Ergang 
Published: July 2020

AbstractA non‐conjugated polymer acceptor PF1‐TS4 was firstly synthesized by embedding a thioalkyl segment in the mainchain, which shows excellent photophysical properties on par with a fully conjugated polymer, with a low optical band gap of 1.58 eV and a high absorption coefficient >105 cm−1, a high LUMO level of −3.89 eV, and suitable crystallinity. Matched with the polymer donor PM6, the PF1‐TS4‐based all‐PSC achieved a power conversion efficiency (PCE) of 8.63 %, which is ≈45 % higher than that of a device based on the small molecule acceptor counterpart IDIC16. Moreover, the PF1‐TS4‐based all‐PSC has good thermal stability with ≈70 % of its initial PCE retained after being stored at 85 °C for 180 h, while the IDIC16‐based device only retained ≈50 % of its initial PCE when stored at 85 °C for only 18 h. Our work provides a new strategy to develop efficient polymer acceptor materials by linkage of conjugated units with non‐conjugated thioalkyl segments.
Thermochromic Meltable Materials with Reverse Spin Transition Controlled by Chemical Design
Authors: Valverde‐Muñoz Francisco‐Javier , Seredyuk Maksym , Muñoz M. Carmen , Molnár Gábor , Bibik Yurii S. , Real José Antonio 
Published: July 2020

AbstractWe report a series of meltable FeII complexes, which, depending on the length of aliphatic chains, display abrupt forward low‐spin to high‐spin transition or unprecedented melting‐triggered reverse high‐spin to low‐spin transition on temperature rise. The reverse spin transition is perfectly reproducible on thermal cycling and the obtained materials are easily processable in the form of thin film owing to their soft‐matter nature. We found that the discovered approach represents a potentially generalizable new avenue to control both the location in temperature and the direction of the spin transition in meltable compounds.
Nickel‐Catalyzed Mono‐Selective α‐Arylation of Acetone with Aryl Chlorides and Phenol Derivatives
Authors: Derhamine Sary Abou , Krachko Tetiana , Monteiro Nuno , Pilet Guillaume , Schranck Johannes , Tlili Anis , Amgoune Abderrahmane 
Published: July 2020

AbstractThe challenging nickel‐catalyzed mono‐α‐arylation of acetone with aryl chlorides, pivalates, and carbamates has been achieved for the first time. A nickel/Josiphos‐based catalytic system is shown to feature unique catalytic behavior, allowing the highly selective formation of the desired mono‐α‐arylated acetone. The developed methodology was applied to a variety of (hetero)aryl chlorides including biologically relevant derivatives. The methodology has been extended to the unprecedented coupling of acetone with phenol derivatives. Mechanistic studies allowed the isolation and characterization of key Ni0 and NiII catalytic intermediates. The Josiphos ligand is shown to play a key role in the stabilization of NiII intermediates to allow a Ni0/NiII catalytic pathway. Mechanistic understanding was then leveraged to improve the protocol using an air‐stable NiII pre‐catalyst.
Controlling Residual Lithium in High‐Nickel (>90 %) Lithium Layered Oxides for Cathodes in Lithium‐Ion Batteries
Authors: Seong Won Mo , Cho Kwang‐Hwan , Park Ji‐Won , Park Hyeokjun , Eum Donggun , Lee Myeong Hwan , Kim Il‐seok Stephen , Lim Jongwoo , Kang Kisuk 
Published: July 2020

AbstractThe rampant generation of lithium hydroxide and carbonate impurities, commonly known as residual lithium, is a practical obstacle to the mass‐scale synthesis and handling of high‐nickel (>90 %) layered oxides and their use as high‐energy‐density cathodes for lithium‐ion batteries. Herein, we suggest a simple in situ method to control the residual lithium chemistry of a high‐nickel lithium layered oxide, Li(Ni0.91Co0.06Mn0.03)O2 (NCM9163), with minimal side effects. Based on thermodynamic considerations of the preferred reactions, we systematically designed a synthesis process that preemptively converts residual Li2O (the origin of LiOH and Li2CO3) into a more stable compound by injecting reactive SO2 gas. The preformed lithium sulfate thin film significantly suppresses the generation of LiOH and Li2CO3 during both synthesis and storage, thereby mitigating slurry gelation and gas evolution and improving the cycle stability.
Synthesis and properties of syndiotactic 1,2‐polybutadiene catalyzed by iron catalyst with phosphate as additive
Authors: Hu Zhonghan , Xu Yuechao , Hu Wenhong , Luo Wanwei , Zhao Yu , Huang Weizhong , Gong Dirong 
Published: July 2020

Abstract1,2 Syndiotactic polymerization of butadiene is accessible by iron catalysts prepared from commercially available iron sources, trialkylaluminum with additional phosphate as additive. The catalyst formation is quite robust in terms of handling and stability under polymerization conditions. Activity equal to 115 kg (polymer)/mol(Fe)·h is achieved at 10,000 equiv. of monomer relative to the catalyst loading in 2 h at 50°C. The resultant polymer possesses 1,2 incorporation up to 80.2–93.1% with syndiotactic configuration (rrrr) of 40.2–85.2%. Crystallinity of polymers can be also tuned over a wide range degree from weak (2.1%) to high crystallinity (68.2%) by varying catalyst component feeding, enabling potential application as both rubber and resin. The higher activity of iron catalyst is preferred at hydrocarbon solvent n‐hexane, n‐heptane or toluene, higher temperature as well as trialkylalumium, such as tri‐iso‐butylaluminum, tri‐ethylaluminum, and tri‐methylaluminum as cocatalyst. Significant stereospecificity stability to variation for monomer concentration, type of alkylaluminum and temperature is also found. The high activity and 1,2‐stereoselectivity featured with these thermal robust iron catalysts sheds light on the significance of additive on regulating stereo‐polymerization promoted by conventional Ziegler–Natta catalysts. These features collectively could offer advantages for application in industry production of 1,2‐syndiotactic polybutadiene.
Indole/isatin‐containing hybrids as potential antibacterial agents
Authors: Song Feng , Li Zhenghua , Bian Yunqiang , Huo Xiankai , Fang Junman , Shao Linlin , Zhou Meng 
Published: July 2020

AbstractThe emergence and worldwide spread of drug‐resistant bacteria have already posed a serious threat to human life, creating the urgent need to develop potent and novel antibacterial drug candidates with high efficacy. Indole and isatin (indole‐2,3‐dione) present a wide structural and mechanistic diversity, so their derivatives possess various pharmacological properties and occupy a salient place in the development of new drugs. Indole/isatin‐containing hybrids, which demonstrate a promising activity against a panel of clinically important Gram‐positive and Gram‐negative bacteria, are privileged scaffolds for the discovery of novel antibacterial candidates. This review, covering articles published between January 2015 and May 2020, focuses on the development and structure–activity relationship (SAR) of indole/isatin‐containing hybrids with potential application for fighting bacterial infections, to facilitate further rational design of novel drug candidates.
Rossby number and chromospheric activity of solar mass stars
Authors: Gondoin Philippe 
Published: July 2020

AbstractPhotometric surveys of open clusters have produced extensive measurements of rotation periods on Sun‐like stars of different ages. In particular, observations of intermediate age clusters, such as the Pleiades and M34, indicate a brief episode of rapid deceleration of stellar rotation at Rossby numbers between 0.1 and 0.3. I used those results to obtain new insights into the long‐term evolution of chromospheric activity on solar mass stars.
A Psychometrically Robust Screening Tool To Rapidly Identify Socially Impaired Monkeys In The General Population
Authors: Talbot Catherine F. , Garner Joseph P. , Maness Alyssa C. , McCowan Brenda , Capitanio John P. , Parker Karen J. 
Published: July 2020

Naturally low‐social rhesus macaques exhibit social impairments with direct relevance to autism spectrum disorder (ASD). To more efficiently identify low‐social individuals in a large colony, we exploited, refined, and psychometrically assessed the macaque Social Responsiveness Scale (mSRS), an instrument previously derived from the human ASD screening tool. We performed quantitative social behavior assessments and mSRS ratings on a total of N = 349 rhesus macaques (Macaca mulatta) housed in large, outdoor corrals. In one cohort (N = 116), we conducted inter‐rater and test‐retest reliabilities, and in a second cohort (N = 233), we evaluated the convergent construct and predictive validity of the mSRS‐Revised (mSRS‐R). Only 17 of the original 36 items demonstrated inter‐rater and test–retest reliability, resulting in the 17‐item mSRS‐R. The mSRS‐R showed strong validity: mSRS‐R scores robustly predicted monkeys' social behavior frequencies in home corrals. Monkeys that scored 1.5 standard deviations from the mean on nonsocial behavior likewise exhibited significantly more autistic‐like traits, and mSRS‐R scores predicted individuals' social classification (low‐social vs. high‐social) with 96% accuracy (likelihood ratio chi‐square = 25.07; P < 0.0001). These findings indicate that the mSRS‐R is a reliable, valid, and sensitive measure of social functioning, and like the human SRS, can be used as a high‐throughput screening tool to identify socially impaired individuals in the general population.Lay SummaryVariation in autistic traits can be measured in humans using the Social Responsiveness Scale (SRS). Here, we revised this scale for rhesus macaques (i.e., the mSRS‐R), and showed that macaques exhibit individual differences in mSRS‐R scores, and at the behavioral extremes, low‐social vs. high‐social monkeys exhibit more autistic‐like traits. These results suggest that the mSRS‐R can be used as a screening tool to rapidly and accurately identify low‐social monkeys in the general population. Autism Res 2020, 13: 1465–1475. © 2020 International Society for Autism Research, Wiley Periodicals, Inc.
Survival outcomes in an older US population with advanced melanoma and central nervous system metastases: SEER‐Medicare analysis
Authors: Sadetsky Natalia , Hernandez Alexandra , Wallick Chris J. , McKenna Edward F. , Surinach Andy , Colburn Dawn E. 
Published: July 2020

AbstractBackgroundCentral nervous system (CNS) metastasis is common in advanced melanoma patients. New treatment options have improved overall prognosis, but information is lacking for patients with CNS metastases. We investigated treatment patterns and survival outcomes in older melanoma patients with and without CNS metastases.MethodsA retrospective analysis of SEER‐Medicare, a population‐based linked database, was undertaken in patients aged > 65 years with advanced melanoma diagnosed from 2004 to 2011 and followed until 2013.ResultsA total of 2522 patients were included. CNS metastases were present in 24.8% of patients at initial metastatic diagnosis; 16.5% developed CNS metastases during follow‐up. Chemotherapy was the most common treatment regardless of CNS metastases. Overall survival (OS) was better for patients without CNS metastases (median, 9.5 months; 95% confidence interval [CI], 8.8‐10.2) vs patients with CNS metastases (3.63 months; 95% CI, 3.4‐3.9). Among patients with CNS metastases, median OS for targeted therapy, immunotherapy, and chemotherapy was 6 (95% CI, 2.5‐9.6), 5.5 (95% CI, 3.8‐7.5), and 4.5 (95% CI, 3.8‐5.4) months, respectively, vs 2.4 (95% CI, 2.1‐2.7) and 2.1 (95% CI, 1.8‐2.7) months for local radiotherapy and no treatment, respectively. Stereotactic radiosurgery demonstrated higher OS vs whole‐brain radiation therapy (median, 4.98 [95% CI, 3.5‐7.5] vs 2.4 [95% CI, 2.1‐2.7] months).ConclusionPatients with CNS metastases from melanoma remain a population with high unmet medical need despite recent advances in treatment. Systemic treatments (eg, BRAF‐targeted therapy and immunotherapy) and stereotactic radiosurgery demonstrated meaningful but modest improvements in OS. Further explorations of combinations of radiotherapy, BRAF‐targeted therapies, and immunotherapies are needed.
Functionalization of Heterocycles through 1,2‐Metallate Rearrangement of Boronate Complexes
Authors: Das Kanak Kanti , Panda Santanu 
Published: July 2020

AbstractOver the last decade, 1,2‐metallate rearrangement of boronate complex has been dominating the literature of organoboron chemistry for the construction of very important C−C and C−boron bonds. Owing to the coordinative unsaturated nature of the boron atom, a nucleophile can attack on boron center for the formation of a boronate complex, which triggers 1,2‐migration under electrophilic activation at the α‐carbon. Apart from using stochiometric electrophilic activating reagents, several catalytic methods using transition metals in the presence or absence of light have been reported. The 1,2‐migration of boronate complexes allows synthesis of many different classes of racemic and chiral compounds including a wide range of substituted heterocycles. Synthesis of chiral and achiral substituted heterocycles by using 1,2‐metallate rearrangement of boronate complexes has been extensively reported by several groups owing to its prevalence in medicinal chemistry. This minireview highlights the methods known to date for the synthesis of heteroaryls by using 1,2‐migration of boronate complexes, organized in a chronological manner.
A Full Li–S Battery with Ultralow Excessive Li Enabled via Lithiophilic and Sulfilic W2C Modulation
Authors: Wei Benben , Shang Chaoqun , Akinoglu Eser Metin , Wang Xin , Zhou Guofu 
Published: July 2020

AbstractThe practical application of Li–S batteries demands low cell balance (Licapacity/Scapacity), which involves uniform Li growth, restrained shuttle effect, and fast redox reaction kinetics of S species simultaneously. Herein, with the aid of W2C nanocrystals, a freestanding 3D current collector is applied as both Li and S hosts owing to its lithiophilic and sulfilic property. On the one hand, the highly conductive W2C can reduce Li nucleation overpotentials, thus guiding uniform Li nucleation and deposition to suppress Li dendrite growth. On the other hand, the polar W2C with catalytic effect can enhance the chemisorption affinity to lithium polysulfides (LiPSs) and guarantee fast redox kinetics to restrain S species in cathode region and promote the utilization of S. Surprisingly, a full Li–S battery with ultralow cell balance of 1.5:1 and high sulfur loading of 6.06 mg cm−2 shows obvious redox plateaus of S and maintains high reversible specific capacity of 1020 mAh g−1 (6.2 mAh cm−2) after 200 cycles. This work may shed new sights on the facile design of full Li–S battery with low excessive Li supply.
Influence of Contaminants in Steel Mill Exhaust Gases on Cu/ZnO/Al2O3 Catalysts Applied in Methanol Synthesis
Authors: He Jiayue , Laudenschleger Daniel , Schittkowski Julian , Machoke Albert , Song Huiqing , Muhler Martin , Schlögl Robert , Ruland Holger 
Published: July 2020

AbstractThe influence of impurities in steel mill exhaust gases on ternary Cu/ZnO/Al2O3 catalysts was studied for conventional methanol synthesis, which is one of the central reactions within the cross‐industrial approach of Carbon2Chem®. A series of hydrocarbons was identified as inert spectators for methanol synthesis. Several catalyst poisons like N‐containing compounds or O2 show reversible characteristics at low pressure. However, by increasing the partial pressure of O2, poisoning becomes irreversible, indicating different poisoning mechanisms concerning the reversibility of deactivation.
Subcategorization of atypical glandular cells is useful to identify lesion site
Authors: Kawano Kouichiro , Yamaguchi Tomohiko , Nasu Hiroki , Nishio Shin , Ushijima Kimio 
Published: July 2020

AbstractBackgroundIn the subcategorization of atypical glandular cells (AGCs), origin of cells should be mentioned to estimate lesion sites for diagnosis. However, cases without subcategorization are often encountered due to limited reproducibility. We evaluated whether the subcategorization of AGC based on the Bethesda terminology can estimate lesion sites.MethodsWe retrospectively investigated cases whose cervical smears were interpreted as AGC and underwent pathological assessment at our institution between June 2009 and September 2017. AGC was subcategorized based on the Bethesda System. Not‐otherwise‐specified (NOS) was subcategorized into endocervical cells (NOS‐EC), endometrial cells (NOS‐EM), or glandular cells (NOS‐G). Favor neoplastic (FN) was subcategorized into endocervical cells (FN‐EC) or glandular cells (FN‐G). FN‐G was further subcategorized into endometrial cells (FN‐EM) or unknown origin (FN‐UO). Clinicopathological data were retrieved from the medical records.ResultsOf 88 AGC cases, there were 30 NOS‐EC (34.1%), 2 NOS‐EM (2.3%), 25 FN‐EC (28.4%), 22 FN‐EM (25.0%), and 9 FN‐UO (10.2%). A significantly higher proportion of neoplastic lesions occurred in FN than in NOS (P <.001). The concordance of AGC subclass and lesion site was 88.0%, 70.7%, and 77.3% in FN‐EC, FN‐G, and FN‐EM, respectively. The concordance of FN‐EM and lesion site increased to 88.9% in patients aged >50 years. Of nine cases of FN‐UO, six experienced nonendometrioid endometrial cancer and extrauterine malignancy.ConclusionSubcategorization of NOS and FN would be useful in estimating neoplastic lesions. Further subcategorization into FN‐EC, FN‐EM, and FN‐UO would similarly be beneficial in estimating the lesion site, especially for small endometrial and extrauterine lesions.
Leaf nonstructural carbohydrate concentrations of understory woody species regulated by soil phosphorus availability in a tropical forest
Authors: Mo Qifeng , Chen Yiqun , Yu Shiqin , Fan Yingxu , Peng Zhongtong , Wang Wenjuan , Li Zhi’an , Wang Faming 
Published: July 2020

AbstractLeaf soluble sugars and starch are important components of nonstructural carbohydrates (NSCs), which are crucial for plant growth, development, and reproduction. Although there is a large body of research focusing on the regulation of plant NSC (soluble sugars and starch) concentrations, the response of foliar NSC concentrations to continuous nitrogen (N) and phosphorus (P) addition is still unclear, especially in tropical forests. Here, we used a long‐term manipulative field experiment to investigate the response of leaf NSC concentrations to continuous N and P addition (3‐, 5‐, and 8‐year fertilization) in a tropical forest in southern China. We found significant species‐specific variation in leaf NSC concentrations in this tropical forest. Phosphorus addition dramatically decreased both leaf soluble sugar and starch concentrations, while N addition had no significant effects on leaf soluble sugar and starch concentrations. These results suggest that, in plants growing in P‐limiting tropical soil, leaf NSC concentrations are regulated by soil P availability rather than N availability. Moreover, the negative relationships between NSC concentrations and leaf mass per area (LMA) revealed that NSCs could supply excess carbon (C) for leaf expansion under P addition. This was further supported by the increased structural P fraction after P fertilization in our previous study at the same site. We conclude that soil P availability strongly regulates leaf starch and soluble sugar concentrations in the tropical tree species included in this study. The response of leaf NSC concentrations to long‐term N and P addition can reflect the close relationships between plant C dynamics and soil nutrient availability in tropical forests. Maintaining relatively higher leaf NSC concentrations in tropical plants can be a potential mechanism for adapting to P‐deficient conditions.
The transplantation technology of communication intensive applications on heterogeneous clusters
Authors: Cui Xiang , Li Xiaowen , Chen Yifeng 
Published: July 2020

AbstractCompared with traditional clusters, heterogeneous clusters cherish the high performance to price ratio. However, compared with the rapid development of hardware technology, the current software technology is still lagging behind. This article introduces a parallel programming model to describe the multidimensional structure, arrangement, and communication modes of the data, threads, and fast Fourier transform. This model provides a new mechanism for transplantation between different types of heterogeneous systems. Using direct methods of turbulence simulation as an example, this article discusses the new software technologies of the parallel software theory, methods of program design, algorithm design, and system software support and provides experience for application transplantation on these heterogeneous systems.