bluuebunny/crossref_metadata_2025_split huggingface dataset:
The impact of mild cognitive impairment on the neural dynamics serving verbal working memory
Authors: Proskovec Amy L. , Davenport Elizabeth M. , Bell Natalie , Rossetti Heidi , Cullum Munro , Longoria Anthony , Berry Jarett D. , Maldjian Joseph 
Published: February 2022

AbstractBackgroundIn healthy adults, neural oscillatory activity within a predominantly left‐lateralized network of brain regions underlies verbal working memory (VWM) performance, but how mild cognitive impairment (MCI) impacts these oscillatory dynamics is not well characterized. The present study utilized the spatiotemporal precision of magnetoencephalographic (MEG) brain imaging to investigate the effects of MCI on the neural oscillations serving specific phases (i.e., encoding, maintenance) of VWM. In congruence with the compensation‐related utilization of neural circuits hypothesis (CRUNCH), we hypothesized that MCI patients would recruit greater neural resources during VWM.MethodSixty‐one adults (13 clinically‐diagnosed MCI, 48 controls; 28 females; M age: 63.5) completed a Sternberg‐type VWM task during MEG. Only correct trials were analyzed, and the average number of trials included did not differ between groups. All MEG data underwent standard preprocessing, were transformed into the time‐frequency domain, and significant neural oscillatory responses relative to baseline were imaged using a beamformer. To determine the effect of group (MCI vs. controls), ANCOVAs were performed on the resulting encoding and maintenance whole‐brain maps with age as a covariate.ResultThroughout encoding and maintenance, decreases in alpha/beta (9‐16 Hz) oscillatory activity were seen in left fronto‐temporal regions, which were significantly larger in MCI patients during the encoding phase (p < .05, corrected). Additionally, significant group differences were detected in right inferior frontal and superior temporal cortices throughout both encoding and maintenance, such that MCI patients exhibited decreased alpha/beta activity within these regions, while these responses were largely absent in controls (p < .05, corrected). Interestingly, the strength of the alpha/beta response within the right inferior frontal cortex significantly predicted behavioral performance on the task, such that individuals who demonstrated stronger decreases in alpha/beta within this region during encoding and maintenance, tended to have faster reaction times (p < .01).ConclusionWhile both groups recruited a similar left‐hemispheric cortical network during VWM encoding and maintenance, individuals with MCI recruited some nodes more strongly and additionally recruited right fronto‐temporal regions. Additionally, stronger recruitment of the right inferior frontal cortex was beneficial for task performance. These results offer supporting evidence for CRUNCH.
B vitamin intakes modify the association between particulate air pollutants and incidence of all‐cause dementia: Findings from the Women's Health Initiative Memory Study
Authors: Chen Cheng , Whitsel Eric A. , Espeland Mark A. , Snetselaar Linda , Hayden Kathleen M. , Lamichhane Archana P. , Serre Marc L. , Vizuete William , Kaufman Joel D. , Wang Xinhui , Chui Helena C. , D'Alton Mary E. , Chen Jiu‐Chiuan , Kahe Ka 
Published: February 2022

AbstractIntroductionParticulate air pollutants may induce neurotoxicity by increasing homocysteine levels, which can be lowered by high B vitamin intakes. Therefore, we examined whether intakes of three B vitamins (folate, B12, and B6) modified the association between PM2.5 exposure and incidence of all‐cause dementia.MethodsThis study included 7183 women aged 65 to 80 years at baseline. B vitamin intakes from diet and supplements were estimated by food frequency questionnaires at baseline. The 3‐year average PM2.5 exposure was estimated using a spatiotemporal model.ResultsDuring a mean follow‐up of 9 years, 342 participants developed all‐cause dementia. We found that residing in locations with PM2.5 exposure above the regulatory standard (12 μg/m3) was associated with a higher risk of dementia only among participants with lower intakes of these B vitamins.DiscussionThis is the first study suggesting that the putative neurotoxicity of PM2.5 exposure may be attenuated by high B vitamin intakes.
Crosswalk between the Mini‐Mental State Examination and the Telephone Interview for Cognitive Status (TICS‐27/30/40)
Authors: Hlávka Jakub P. , Yu Jeffrey C. , Lakdawalla Darius N. 
Published: February 2022

AbstractBackgroundWe develop a crosswalk between the Mini‐Mental State Examination (MMSE) and Telephone Interview for Cognitive Status (TICS)‐27, TICS‐30, and TICS‐40 for adults 65 years and older.MethodsWe examined the scores of 1809 participants, with and without cognitive impairment, who completed the MMSE and the TICS assessment in the 2016 Health and Retirement Study and the 2016 Harmonized Cognitive Assessment Protocol study. Crosswalks between MMSE and TICS‐27/30/40 were developed via equipercentile equating.ResultsWe present crosswalks for MMSE and TICS‐27/30/40 for the 65+ population representative of the US elderly. While monotonic, the pattern of the TICS‐30 to MMSE crosswalk differs from the other two crosswalks (MMSE to TICS‐27/40).ConclusionOur analysis offers an empirical crosswalk between two commonly used cognitive measures—the MMSE and TICS. Our findings suggest the need for validated and robust measures that allow for the comparison of scores on different cognitive scales.
Traumatic brain injury and dementia risk in male veteran older twins—Controlling for genetic and early life non‐genetic factors
Authors: Plassman Brenda L. , Chanti‐Ketterl Marianne , Pieper Carl F. , Yaffe Kristine 
Published: February 2022

AbstractIntroductionThis study leveraged the twin study design, which controls for shared genetic and early life exposures, to investigate the association between traumatic brain injury (TBI) and dementia.MethodsMembers of the National Academy of Sciences–National Research Council's Twins Registry of World War II male veterans were assigned a cognitive outcome based on a multi‐step assessment protocol. History of TBI was obtained via interviews.ResultsAmong 8302 individuals, risk of non‐Alzheimer's disease (non‐AD) dementia was higher in those with TBI (hazard ratio [HR] = 2.00, 95% confidence interval [CI], 0.97–4.12), than for AD (HR = 1.23, 95% CI, 0.76–2.00). To add more control of genetic and shared environmental factors, we analyzed 100 twin pairs discordant for both TBI and dementia onset, and found TBI‐associated risk for non‐AD dementia increased further (McNemar odds ratio = 2.70; 95% CI, 1.27–6.25).DiscussionThese findings suggest that non‐AD mechanisms may underlie the association between TBI and dementia, potentially providing insight into inconsistent results from prior studies.
Genetic Encoding of Cyanopyridylalanine for In‐Cell Protein Macrocyclization by the Nitrile–Aminothiol Click Reaction
Authors: Abdelkader Elwy H. , Qianzhu Haocheng , George Josemon , Frkic Rebecca L. , Jackson Colin J. , Nitsche Christoph , Otting Gottfried , Huber Thomas 
Published: February 2022

AbstractCyanopyridylalanines are non‐canonical amino acids that react with aminothiol compounds under physiological conditions in a biocompatible manner without requiring added catalyst. Here we present newly developed aminoacyl‐tRNA synthetases for genetic encoding of meta‐ and para‐cyanopyridylalanine to enable the site‐specific attachment of a wide range of different functionalities. The outstanding utility of the cyanopyridine moiety is demonstrated by examples of i) post‐translational functionalization of proteins, ii) in‐cell macrocyclization of peptides and proteins, and iii) protein stapling. The biocompatible nature of the protein ligation chemistry enabled by the cyanopyridylalanine amino acid opens a new path to specific in vivo protein modifications in complex biological environments.
Nutzung von elektronenarmen Iminiumintermediaten zur Synthese von wertvollen Aminen
Authors: Hsu Che‐Sheng , Gonçalves Carlos R. , Tona Veronica , Pons Amandine , Kaiser Marcel , Maulide Nuno 
Published: February 2022

AbstractDie Entwicklung von Reaktionen zur Umwandlung von Alkenen und Alkinen in wertvolle Bausteine ist nach wie vor eines der Hauptziele in der synthetischen Chemie. In dieser Arbeit berichten wir von der Nutzbarmachung von stark elektronenarmen, seltenen und kurzlebigen Iminiumionen zur Synthese von Aminen. Dies ermöglicht die milde Herstellung von Aminen mit z. B. trifluormethylierten Einheiten. Dieses umfassende Konzept wird durch die Aminierung von Chinin zu einem biologisch interessanten neuen Analogon verdeutlicht.
Double Lock Label Based on Thermosensitive Polymer Hydrogels for Information Camouflage and Multilevel Encryption
Authors: Lou Dongyang , Sun Yujing , Li Jian , Zheng Yuanyuan , Zhou Zhipeng , Yang Jing , Pan Chuxuan , Zheng Zhikun , Chen Xudong , Liu Wei 
Published: February 2022

AbstractDeveloping extra safety encryption technologies to prevent information leakage and combat fakes is in high demand but is challenging. Herein, we propose a “double lock” strategy based on both lower critical solution temperature (LCST) and upper critical solution temperature (UCST) polymer hydrogels for information camouflage and multilevel encryption. Two types of hydrogels were synthesized by the method of random copolymerization. The number of −CO−NH2 groups in the network structure of the hydrogels changed the enthalpic or entropic thermo‐responsive hydrogels, and ultimately precisely controlled their phase transition temperature. The crosslink density of the polymer hydrogels governs the diffusion kinetics, resulting in a difference in the time for their color change. The combination of multiple LCST and UCST hydrogels in one label realized information encryption and dynamic information identification in the dimensions of both time and temperature. This work is highly interesting for the fields of information encryption, anti‐counterfeiting, and smart responsive materials.
Reversible Three‐Color Fluorescence Switching of an Organic Molecule in the Solid State via “Pump–Trigger” Optical Manipulation
Authors: Yang Runqing , Ren Xue , Mei Lijun , Pan Guocui , Li Xiao‐Ze , Wu Zhiyuan , Zhang Song , Ma Wenyue , Yu Weili , Fang Hong‐Hua , Li Chong , Zhu Ming‐Qiang , Hu Zheng , Sun Tianmeng , Xu Bin , Tian Wenjing 
Published: February 2022

AbstractIn photoswitches that undergo fluorescence switching upon ultraviolet irradiation, photoluminescence and photoisomerization often occur simultaneously, leading to unstable fluorescence properties. Here, we successfully demonstrated reversible solid‐state triple fluorescence switching through “Pump–Trigger” multiphoton manipulation. A novel fluorescence photoswitch, BOSA‐SP, achieved green, yellow, and red fluorescence under excitation by pump light and isomerization induced by trigger light. The energy ranges of photoexcitation and photoisomerization did not overlap, enabling appropriate selection of the multiphoton light for “pump” and “trigger” photoswitching, respectively. Additionally, the large free volume of the spiropyran (SP) moiety in the solid state promoted reversible photoisomerization. Switching between “pump” and “trigger” light is useful for three‐color tunable switching cell imaging, which can be exploited in programmable fluorescence switching. Furthermore, we exploited reversible dual‐fluorescence switching in a single molecular system to successfully achieve two‐color super‐resolution imaging.
Real‐Time NMR Recording of Fermentation and Lipid Metabolism Processes in Live Microalgae Cells
Authors: Nami Faezeh , Ferraz Maria Joao , Bakkum Thomas , Aerts Johannes M. F. G. , Pandit Anjali 
Published: February 2022

AbstractNon‐invasive and real‐time recording of processes in living cells has been limited to detection of small cellular components such as soluble proteins and metabolites. Here we report a multiphase NMR approach using magic‐angle spinning NMR to synchronously follow microbial processes of fermentation, lipid metabolism and structural dynamic changes in live microalgae cells. Chlamydomonas reinhardtii green algae were highly concentrated, introducing dark fermentation and anoxia conditions. Single‐pulse NMR experiments were applied to obtain temperature‐dependent kinetic profiles of the formed fermentation products. Through dynamics‐based spectral editing NMR, simultaneous conversion of galactolipids into TAG and free fatty acids was observed and rapid loss of rigid lipid structures. This suggests that lipolysis under dark and anoxia conditions finally results in the breakdown of cell and organelle membranes, which could be beneficial for recovery of intracellular microbial useful products.
NHC Catalysis for Umpolung Pyridinium Alkylation via Deoxy‐Breslow Intermediates
Authors: Wu Terence , Tatton Matthew R. , Greaney Michael F. 
Published: February 2022

AbstractUmpolung N‐heterocyclic carbene (NHC) catalysis of non‐aldehyde substrates offers new pathways for C−C bond formation, but has proven challenging to develop in terms of viable substrate classes. Here, we demonstrate that pyridinium ions can undergo NHC addition and subsequent intramolecular C−C bond formation through a deoxy‐Breslow intermediate. The alkylation demonstrates, for the first time, that deoxy‐Breslow intermediates are viable for catalytic umpolung of areniums.
Enantioselective Recognition of Helicenes by a Tailored Chiral Benzo[ghi]perylene Trisimide π‐Scaffold
Authors: Teichmann Ben , Krause Ana‐Maria , Lin Mei‐Jin , Würthner Frank 
Published: February 2022

AbstractEnantioselective molecular recognition of chiral molecules that lack specific interaction sites for hydrogen bonding or Lewis acid–base interactions remains challenging. Here we introduce the concept of tailored chiral π‐surfaces toward the maximization of shape complementarity. As we demonstrate for helicenes it is indeed possible by pure van‐der‐Waals interactions (π–π interactions and CH–π interactions) to accomplish enantioselective binding. This is shown for a novel benzo[ghi]perylene trisimide (BPTI) receptor whose π‐scaffold is contorted into a chiral plane by functionalization with 1,1′‐bi‐2‐naphthol (BINOL). Complexation experiments of enantiopure (P)‐BPTI with (P)‐ and (M)‐[6]helicene afforded binding constants of 10 700 M−1 and 550 M−1, respectively, thereby demonstrating the pronounced enantiodifferentiation by the homochiral π‐scaffold of the BPTI host. The enantioselective recognition is even observable by the naked eye due to a specific exciplex‐type emission originating from the interacting homochiral π‐scaffolds of electron‐rich [6]helicene and electron‐poor BPTI.
Vorhersage der MOF‐Synthese durch automatisches Data‐Mining und maschinelles Lernen**
Authors: Luo Yi , Bag Saientan , Zaremba Orysia , Cierpka Adrian , Andreo Jacopo , Wuttke Stefan , Friederich Pascal , Tsotsalas Manuel 
Published: February 2022

AbstractTrotz großer Fortschritte auf dem Gebiet der metallorganischen Gerüststrukturen (MOF) ist das volle Potential des Maschinellen Lernens (ML) für die Vorhersage von MOF‐Syntheseparametern bisher noch nicht erschlossen. In diesem Beitrag wird dargestellt, wie Methoden des ML für die Rationalisierung und Beschleunigung von MOF‐Entwicklungsverfahren eingesetzt werden können, indem die Synthesebedingungen der MOFs direkt anhand ihrer Kristallstruktur vorhergesagt werden. Unser Ansatz stützt sich auf: i) die Erstellung der ersten MOF‐Synthese‐Datenbank durch automatische Extraktion der Syntheseparameter aus der Fachliteratur, ii) das Trainieren und die Optimierung von ML‐Modellen mit Daten der MOF‐Datenbank und iii) die ML basierte Vorhersage der Synthesebedingungen neuer MOF‐Strukturen. Schon jetzt übertreffen die Ergebnisse der Vorhersagemodelle die Vorhersagen menschlicher ExpertInnen, welche in einer Befragung ermittelt wurden. Die automatisierte Synthesevorhersage ist über ein Web‐Tool unter https://mof‐synthesis.aimat.science verfügbar.
Asymmetric Total Synthesis of Shizukaol J, Trichloranoid C and Trishizukaol A
Authors: Wang Xiao , Wang Zhuang , Ma Xianjian , Huang Zhengsong , Sun Ke , Gao Xiang , Fu Shaomin , Liu Bo 
Published: February 2022

AbstractThe asymmetric total synthesis of three lindenane sesquiterpenoid oligomers, shizukaol J, trichloranoid C and trishizukaol A, has been accomplished concisely in 15, 16 and 18 longest linear steps, respectively. The expeditious construction of molecular architectures was facilitated by Nelson's catalytic asymmetric ketene–aldehyde cycloaddition, a sequence of allylic alkylation/reduction/acidic cyclization to forge a lactone, and a double aldol condensation cascade to construct the 5/6 bicyclic system. Diastereoselective nucleophilic substitution promoted by a phase transfer catalyst constructed the C11 quaternary stereogenic center, thus prompting synthetic efficacy toward shizukaol J. The synthesis of trichloranoid C and trishizukaol A was achieved after a cascade involving furanyl diene formation and a Diels–Alder reaction, as well as a one‐pot sequence involving furan oxidation and global deprotection. Furthermore, our biological evaluation revealed that two compounds exhibited unexpected toxicity against tumor cell lines.
A Universal Single‐Atom Coating Strategy Based on Tannic Acid Chemistry for Multifunctional Heterogeneous Catalysis
Authors: Wang Haifeng , Li Xiaopeng , Jiang Ying , Li Minhan , Xiao Qi , Zhao Tao , Yang Shuai , Qi Chunhong , Qiu Pengpeng , Yang Jianping , Jiang Zheng , Luo Wei 
Published: February 2022

AbstractHere, we report a universal single‐atom coating (SAC) strategy by taking advantage of the rich chemistry of tannic acid (TA). TA units not only self‐assemble into a cross‐linked porous polyphenolic framework, but also can grip on different substates via multiple binding modes. Benefiting from the diverse chelating ability of TA, a series of mono‐, and bi‐metallic SACs can be formed on substrates of different materials (e. g., carbon, SiO2, TiO2, MoS2), dimensions (0D–3D) and sizes (50 nm–5 cm). By contrast, uniform SAC cannot be achieved using common approaches such as pyrolysis of metal–dopamine complexes or metal–organic frameworks. As a proof‐of‐concept demonstration, two Co SACs immobilized on graphene and TiO2 were prepared. The former one shows six‐fold higher mass activity than Pt/C toward oxygen reduction. The latter one displays outstanding photocatalytic activity owing to the high activity of the single atoms and the formation of the single‐atom coating–TiO2 heterojunction.
Supported Lanthanum Borohydride Catalyzes CH Borylation Inside Zeolite Micropores
Authors: Li Yuting , Kanbur Uddhav , Cui Jinlei , Wang Guocang , Kobayashi Takeshi , Sadow Aaron D. , Qi Long 
Published: February 2022

AbstractThe zeolite‐supported lanthanide La(BH4)x‐HY30 catalyzes C−H borylation of benzene with pinacolborane (HBpin), providing a complementary approach to precious, late transition metal‐catalyzed borylations. The reactive catalytic species are generated from La grafted at the Brønsted acid sites (BAS) in micropores of the zeolite, whereas silanoate‐ and aluminoate‐grafted sites are inactive under the reaction conditions. During typical catalytic borylations, conversion to phenyl pinacolborane (PhBpin) is zero‐order in HBpin concentration. A turnover number (TON) of 167 is accessed by capping external silanols, selectively grafting at BAS sites, and adding HBpin slowly to the reaction.
Advancing the Development of Recyclable Aromatic Polyesters by Functionalization and Stereocomplexation
Authors: Fan Hua‐Zhong , Yang Xing , Chen Jia‐Hao , Tu Yi‐Min , Cai Zhongzheng , Zhu Jian‐Bo 
Published: February 2022

AbstractThe development of innovative synthetic polymer systems to overcome the trade‐offs between the polymer's depolymerizability and performance properties is in high demand for advanced material applications and sustainable development. In this contribution, we prepared a class of aromatic cyclic esters (M1–M5) from thiosalicylic acid and epoxides by facile one‐pot synthesis. Ring‐opening polymerization of Ms afforded aromatic polyesters P(M)s with high molecular weights and narrow dispersities. The physical and mechanical properties of P(M)s can be modulated by stereocomplexation and regulation of the side‐chain flexibility of the polymers, ultimately achieving high‐performance properties such as high thermal stability and crystallinity (Tm up to 209 °C), as well as polyolefin‐like high mechanical strength, ductility, and toughness. Furthermore, the functionalizable moieties of P(M)s have driven a wide array of post‐polymerization modifications toward access to value‐added materials. More importantly, the P(M)s were able to selectively depolymerize into monomers in excellent yields, thus establishing its circular life cycle.
Facile preparation of transparent poly (γ‐glutamic acid) modified poly (vinyl alcohol) hydrogels with high tensile strength and toughness
Authors: Wu Hailin , Chen Jing , Kim Jiyoung , Zhu Peizhi , Zhu Jiadeng , Gao Qiang , Gao Chunxia 
Published: February 2022

AbstractIn the present work, a transparent poly (γ‐glutamic acid) modified polyvinyl alcohol (γ‐PGA/PVA) hydrogel with excellent tensile strength and toughness was prepared by a simple and effective immersion method. Results revealed that γ‐PGA concentration and immersion time have great influence on the mechanical properties of prepared γ‐PGA/PVA hydrogels. The mechanical tensile strength of γ‐PGA/PVA hydrogel reached to 16.68 ± 0.43 MPa with the strain of 511.64% ± 23.38% when prepared PVA hydrogel was immersed in 20% γ‐PGA solution for 24 h (denoted as 20% γ‐PGA/PVA). Meanwhile, 20% γ‐PGA/PVA hydrogel exhibited excellent mechanical properties, such as high‐level torsion, knotting and puncture resistant, and can lift a 5 kg weight without obvious rupture. The morphology, structure, compositions and mechanism of enhanced mechanical properties were investigated. Besides the excellent mechanical properties, 20% γ‐PGA/PVA hydrogel possessed good conductivity as well as high sensitivity to external strain. Furthermore, in vitro good cytocompatibility of 20% γ‐PGA/PVA hydrogels was demonstrated by using MC3T3‐E1 cells. Therefore, the prepared 20% γ‐PGA/PVA hydrogel may provide the possibility for the applications in the field of cartilage repair/regeneration, artificial skin and human motion sensor.