bluuebunny/crossref_metadata_2025_split huggingface dataset:
Mechanochemische Cyclotrimerisierung: Ein Synthesekonzept für kovalent‐organische Gerüstverbindungen mit regulierbarer Schichtfolge
Authors: Hutsch Stefanie , Leonard Allison , Grätz Sven , Höfler Mark Valentin , Gutmann Torsten , Borchardt Lars 
Published: April 2024

AbstractDie mechanochemische Cyclotrimerisierung von Nitrilen ist ein einfaches Synthesekonzept für Triazin‐haltige Moleküle und Materialien und adressiert Probleme in Zusammenhang mit ungewollter Karbonisierung und mangelnder Löslichkeit verwendeter Edukte. In einer Festkörperreaktion in der Kugelmühle wird 4‐Methylbenzonitril quantitativ in nur 90 Minuten zu Tris(4‐methylphenyl)‐1,3,5‐triazin umgesetzt. Ebenso schnell wird das kovalent‐organische Triazin‐Netzwerk CTF‐1 unter Verwendung von 1,4 Dicyanobenzol aufgebaut. Das erhaltene Material ist porös (650 m2 g−1) und kristallin. Über den mechanischen Energieeintrag kann die erhaltenen Konformation kontrolliert werden – von einer gestaffelten AB‐Anordnung zu einer überlappenden AA‐Stapelung. Weiterhin wird über die Variation der Monomere die Vielseitigkeit dieser Methode belegt.
Typ‐I‐Photoinitiator auf der Basis nachhaltiger Kohlenstoffpunkte
Authors: Li Ruiping , Guo Hongda , Luo Xiongfei , Wang Qunying , Pang Yulian , Li Shujun , Liu Shouxin , Li Jian , Strehmel Bernd , Chen Zhijun 
Published: April 2024

AbstractNachhaltige Kohlenstoffpunkte, die an der Oberfläche Oximestergruppen enthalten, welche einer homolytischen Bindungsspaltung folgen, zeigen ein Potential als Photoinitiatoren für die traditionelle freie radikalische Photopolymerisation. Die Kohlenstoffpunkte wurden nach einem solvothermalen Verfahren aus nachhaltigem Furfural, welches über Lignocellulose erhältlich ist, hergestellt. Aldehydgruppen der Oberfläche reagierten mit Hydroxylamin zu dem entsprechendem Oxim, während die Reaktion mit Benzoylchlorid zu einem bio‐basierten Typ I Photoinitiator (CD‐PI) führte, welcher nachhaltige Kohlenstoffpunkte enthält. Die Fähigkeit zur Photoinitiierung wurde unter UV‐Bestrahlung bei 365 nm mit dem traditionellen Photoinitiator (PI) Ethyl (2,4,6‐trimethyl benzoyl) phenyl phosphinat (TPO‐L) mittels Echtteit FTIR Spektroskopie verglichen. Die auf einem Gemisch von Urethandimethacrylat (UDMA) und Tripropylenglykoldiacrylat (TPGDA) basierte Photopolymerzusammensetzung führte unter Verwendung von CD‐PI oder TPO‐L zu einem ähnlichen Endumsatz von etwa 70 %. Dennoch erschien das vernetzte Material im Fall der Zusammensetzungen, die mit CD‐PI verarbeitet wurden, homogen, während jene, die mit TPO‐L hergestellt wurden, heterogen waren, was durch die beiden Glasübergangstemperaturen gezeigt wurde. Außerdem war die Migrationsgeschwindigkeit von CD‐PI in den gehärteten Proben geringer im Vergleich zu jenen Proben für die TPO‐L als PI eingesetzt wurde.
Constructing Metal(II)‐Sulfate Site Catalysts toward Low Overpotential Carbon Dioxide Electroreduction to Fuel Chemicals
Authors: Yuan Chen‐Yue , Feng Li , Qin Xuetao , Liu Jin‐Xun , Li Xin , Sun Xiao‐Chen , Chang Xiao‐Xia , Xu Bing‐Jun , Li Wei‐Xue , Ma Ding , Dong Hao , Zhang Ya‐Wen 
Published: April 2024

AbstractPrecise regulation of the active site structure is an important means to enhance the activity and selectivity of catalysts in CO2 electroreduction. Here, we creatively introduce anionic groups, which can not only stabilize metal sites with strong coordination ability but also have rich interactions with protons at active sites to modify the electronic structure and proton transfer process of catalysts. This strategy helps to convert CO2 into fuel chemicals at low overpotentials. As a typical example, a composite catalyst, CuO/Cu−NSO4/CN, with highly dispersed Cu(II)−SO4 sites has been reported, in which CO2 electroreduction to formate occurs at a low overpotential with a high Faradaic efficiency (−0.5 V vs. RHE, FEformate=87.4 %). Pure HCOOH is produced with an energy conversion efficiency of 44.3 % at a cell voltage of 2.8 V. Theoretical modeling demonstrates that sulfate promotes CO2 transformation into a carboxyl intermediate followed by HCOOH generation, whose mechanism is significantly different from that of the traditional process via a formate intermediate for HCOOH production.
Robust, Efficient, and Recoverable Thermocells with Zwitterion‐Boosted Hydrogel Electrolytes for Energy‐Autonomous and Wearable Sensing
Authors: Lu Xin , Mo Ziwei , Liu Zhaopeng , Hu Yifeng , Du Chunyu , Liang Lirong , Liu Zhuoxin , Chen Guangming 
Published: April 2024

AbstractThe rapid growth of flexible quasi‐solid‐state thermocells (TECs) provides a fresh way forward for wearable electronics. However, their insufficient mechanical strength and power output still hinder their further applications. This work demonstrates a one‐stone‐two‐birds strategy to synergistically enhance the mechanical and thermoelectrochemical properties of the [Fe(CN)6]3−/4−‐based TECs. By introducing Hofmeister effect and multiple non‐covalent interactions via betaine zwitterions, the mechanical strength of the conventional brittle gelatin hydrogel electrolytes is substantially improved from 50 to 440 kPa, with a high stretchability approaching 250 %. Meanwhile, the betaine zwitterions strongly affect the solvation structure of [Fe(CN)6]3− ions, thus enlarging the entropy difference and raising the thermoelectrochemical Seebeck coefficient from 1.47 to 2.2 mV K−1. The resultant quasi‐solid‐state TECs exhibit a normalized output power density of 0.48 mW m−2 K−2, showing a notable improvement in overall performance compared to their counterparts without zwitterion regulation. The intrinsic thermo‐reversible property also allows the TECs to repeatedly self‐recover through sol‐gel transformations, ensuring reliable energy output and even recycling of TECs in case of extreme mechanical damages. An energy‐autonomous smart glove consisting of eighteen individual TECs is further designed, which can simultaneously monitor the temperature of different positions on any touched object, demonstrating high potential in wearable applications.
H8‐BINOL‐Derived Chiral η6‐Benzene Ligands: New Opportunities for the Ruthenium‐Catalyzed Asymmetric C−H Activation
Authors: Li Junxuan , Wang Guodong , Guo Weicong , Jiang Jijun , Wang Jun 
Published: April 2024

AbstractGiven the tremendous success of (p‐cymene)RuII‐catalyzed C−H activation over the past 20 years, the community has long been aware that the development of chiral η6‐benzene (Ben) ligands should be a potent strategy for achieving the attractive but incredibly underdeveloped ruthenium(II)‐catalyzed asymmetric C−H activation. However, it has rarely been achieved due to the severe difficulty in developing proper chiral Ben ligands. In particular, designing chiral Ben ligands by connecting a benzene fragment to a chiral framework including benzene rings remained an unsolved challenge until this effort. Here we present a novel class of axially chiral Ben ligands derived from readily available (S)‐5,5′,6,6′,7,7′,8,8′‐octahydro‐1,1′‐bi‐2‐naphthol ((S)‐H8‐BINOL) in 4–8 steps. Notably, when coordinated with ruthenium, such chiral Ben ligand containing three benzene rings only forms one of the three possible isomeric BenRuII complexes. The related chiral BenRuII catalysts could effectively catalyze the asymmetric C−H activation of N‐sulfonyl ketimines with alkynes, affording a range of chiral spirocyclic sultams in up to 99 % yield with up to >99 % ee. These catalysts are expected to find broad applications in future.
Built‐in Electric Fields in Heterostructured Lamellar Membranes Enable Highly Efficient Rejection of Charged Mass
Authors: Chen Chongchong , Wu Xiaoli , Chen Jingjing , Liu Siyu , Wang Yongzheng , Wu Wenjia , Zhang Jie , Wang Jingtao , Jiang Zhongyi 
Published: April 2024

AbstractSeparation membranes with homogeneous charge channels are the mainstream to reject charged mass by forming electrical double layer (EDL). However, the EDL often compresses effective solvent transport space and weakens channel‐ion interaction. Here, built‐in electric fields (BIEFs) are constructed in lamellar membranes by assembling the heterostructured nanosheets, which contain alternate positively‐charged nanodomains and negatively‐charged nanodomains. We demonstrate that the BIEFs are perpendicular to horizontal channel and the direction switches alternately, significantly weakening the EDL effect and forces ions to repeatedly collide with channel walls. Thus, highly efficient rejection for charged mass (salts, dyes, and organic acids/bases) and ultrafast water transport are achieved. Moreover, for desalination on four‐stage filtration option, salt rejection reaches 99.9 % and water permeance reaches 19.2 L m−2 h−1 bar−1. Such mass transport behavior is quite different from that in homogeneous charge channels. Furthermore, the ion transport behavior in nanochannels is elucidated by validating horizontal projectile motion model.
Thermal and Photoinduced Radical Cascade Annulation using Aryl Isonitriles: An Approach to Quinoline‐Derived Benzophosphole Oxides
Authors: Banjare Shyam Kumar , Lezius Lena , Horst Elena S. , Leifert Dirk , Daniliuc Constantin G. , Alasmary Fatmah A. , Studer Armido 
Published: April 2024

AbstractHerein, we present a radical cascade addition cyclization sequence to access quinoline‐based benzophosphole oxides from ortho‐alkynylated aromatic phosphine oxides using various aryl isonitriles as radical acceptors and inexpensive tert‐butyl‐hydroperoxide (TBHP) as a terminal oxidant in the presence of a catalytic amount of silver acetate. Alternatively, the same cascade can be realized through a sustainable photochemical approach utilizing 1,2,3,5‐tetrakis(carbazol‐9‐yl)‐4,6‐dicyanobenzene (4CzIPN) as an organic photocatalyst at room temperature. The introduced modular approach shows broad functional group tolerance and offers straightforward access to complex P,N‐containing polyheterocyclic arenes. These novel π‐extended benzophosphole oxides exhibit interesting photophysical and electrochemical properties such as absorption in the visible region, emission and reversible reduction at low potentials, which makes them promising for potential materials science applications. The photophysical properties can further be tuned by the addition of external Lewis and Brønsted acids.
Autonomic and hedonic response to affective touch in autism spectrum disorder
Authors: Capiotto Francesca , Romano Cappi Giulia , Mirlisenna Ilaria , Mazza Alessandro , Cicinelli Giovanni , Lauritano Chiara , Keller Roberto , Dal Monte Olga 
Published: April 2024

AbstractInterpersonal touch plays a crucial role in shaping relationships and encouraging social connections. Failure in processing tactile input or abnormal tactile sensitivity may hamper social behaviors and have severe consequences in individuals' relational lives. Autism Spectrum Disorder (ASD) is characterized by both sensory disruptions and social impairments, making affective touch an ideal meeting point for understanding these features in ASD individuals. By integrating behavioral and physiological measures, we investigated the effects of affective touch on adult individuals with ASD from both an implicit and explicit perspective. Specifically, at an implicit level, we investigated whether and how receiving an affective touch influenced participants' skin conductance tonic and phasic components. At the explicit level, we delved into the affective and unpleasant features of affective touch. Overall, we observed lower skin conductance level in ASD compared to TD subjects. Interestingly, the typically developing (TD) group showed an increased autonomic response for affective touch compared to a control touch, while ASD subjects' autonomic response did not differ between the two conditions. Furthermore, ASD participants provided higher ratings for both the affective and unpleasant components of the touch, compared to TD subjects. Our results reveal a noteworthy discrepancy in ASD population between the subjective experience, characterized by amplified hedonic but also unpleasant responses, and the physiological response, marked by a lack of autonomic activation related to affective touch. This insightful dissociation seems crucial for a deeper understanding of the distinctive challenges characterizing people with ASD and may have implications for diagnosis and therapeutic approaches.
Do local government sustainability initiatives impact corporate social sustainability practices?
Authors: Ida Atsuhiro , Yoshida Kenichi , Xie Jun , Tanaka Yoshitaka , Managi Shunsuke 
Published: April 2024

AbstractThis study quantifies the initiatives of local governments' Sustainable Development Goals (SDGs) and examines their impacts on regional corporate social sustainability practices. Our analysis reveals statistically significant results for corporate action on the following government initiatives on SDGs: BOD/COD effluent standard (6. clean water and sanitation and 14. life below water); number of students per personal computer (PC) (4. quality education); percent of female prefectural assembly members (5. gender equality and 16. peace, justice, and strong institutions); and minimum wage (1. no poverty and 2. zero hunger). These results are robust after controlling for peer effects by other firms in the surrounding regions. The evidence also indicates that these trends are more pronounced in footloose industries than in heavy industries.
When and How does in‐role pro‐environmental behavior spill over to extra‐role behavior: Two experimental studies in the retail and education industries
Authors: Guo Wenjing , Unsworth Kerrie , Bretter Christian , Davis Matthew 
Published: April 2024

AbstractBy integrating theories of goal proximity and crowding‐out, this research investigates how and when employees' performance of in‐role pro‐environmental behaviors will spill over to future engagement in extra‐role pro‐environmental behaviors. Using two experiments with employees from the retail (N = 338) and education (N = 448) industries, we found a conditional positive spillover effect, mediated by pro‐environmental goal commitment. More specifically, when employees with low intrinsic pro‐environmental motivation received feedback that they had progressed in their in‐role pro‐environmental performance, their extra‐role pro‐environmental behavior intentions increased due to an increased commitment to the pro‐environmental goal. However, when employees had high intrinsic pro‐environmental motivation, this spillover effect was negative (Study 1) or non‐significant (Study 2). To summarize, the positive spillover effect only occurs when employees are not highly intrinsically motivated. Our findings uncover a missing piece in organizational environmental management literature and carry important implications for employee‐oriented initiatives.
A finite‐state machine‐based control design for thermal and state‐of‐charge balancing of lithium iron phosphate battery using flyback converters
Authors: Zabetian‐Hosseini Asal , Ghazanfari Amin , Boulet Benoit 
Published: April 2024

AbstractBattery cell balancing plays a vital role in maximizing the performance of the battery system by enhancing battery system capacity and prolonging the battery system life expectancy. Active cell balancing using power converters is a promising approach to maintaining uniform state of charges (SoCs) and temperatures across battery cells. The SoC balancing function in the battery management system (BMS) increases the battery pack capacity, and the temperature balancing function mitigates variations in the aging of battery cells due to unbalanced temperatures. In this work, a finite‐state machine‐based control design is proposed for lithium iron phosphate (LFP) battery cells in series to balance SoCs and temperatures using flyback converters. The primary objective of this design is to ensure balanced SoCs by the end of the charging session while mitigating the temperature imbalance during the charging process. To achieve the SoC and temperature balancing functions using the same balancing circuits, a finite‐state machine control design decides on the operating mode, and a balancing strategy balances either temperature or SoC depending on the operating mode. The proposed control design has the advantages of low computational burden, simple implementation compared to the optimization‐based controller found in the literature, and the proposed balancing strategy offers faster balancing speed compared to conventional methods. The effectiveness of the proposed strategy is validated on battery cell RC models in series with unbalanced SoCs and temperatures.
New Indole Alkaloids from the Fungus Talaromyces assiutensis JTY2
Authors: Zhu Hong‐Quan , Feng Shuo , Xie Rong‐Kun , Zhu Zheng‐Tian , Lou Yong‐Hao , Zhou Xue‐Ming , Song Xin‐Ming 
Published: April 2024

AbstractThree new indole alkaloids, named talatensindoids A−C (1–3), together with two known biogenetically related indole alkaloids tryptamine (4) and L‐tryptophan (5) were isolated from the Talaromyces assiutensis JTY2 based on the guidance of OSMAC approach. The structures of these indole alkaloids were determined by comprehensive spectroscopic analyses. The absolute configuration of 3 was confirmed by X‐ray crystallographic analysis. Compound 1 represent the rare example of a chlorine‐substituted indole alkaloid from natural products. The inhibitory activity of compounds 1–5 against two phytopathogenic fungi and three phytopathogenic bacteria was evaluated. Compound 1 exhibited broad spectrum antibacterial activities.
The Role of Microbial Diversity in Lignocellulosic Biomass Degradation: A Biotechnological Perspective
Authors: Rasool Ghulam , Irfan Muhammad 
Published: April 2024

AbstractLignocellulosic biomass, such as plant residues and agricultural waste, holds immense potential as a renewable resource for the production of biofuels, chemicals, and animal feed. However, the efficient degradation of lignocellulose into fermentable sugars remains a significant challenge. Recent research has highlighted the critical role of microbial diversity in lignocellulosic biomass degradation, offering new insights from a biotechnological perspective. The comprehension and utilization of microbial diversity are crucial for developing efficient biotechnological strategies for lignocellulosic biomass degradation. By uncovering the intricate relationships between microbial communities and their enzymatic machinery, researchers can optimize degradation processes, enhance biofuel production, and contribute to a more sustainable bio‐based economy. Microorganisms, including bacteria, fungi, and archaea, possess diverse enzymatic capabilities, allowing them to secrete a plethora of lignocellulolytic enzymes. Microbial organisms inhabiting extreme environments, such as the rumen, hot and cold springs, deep sea trenches, and acidic and alkaline pH environments, exhibit significant potential in generating enzymes, including hemicellulolytic and lignocellulolytic enzymes, which possess superior biochemical properties essential for industrial bioconversion applications. This review explores the ability of lignocellulosic enzymes from microbial sources to efficiently break down the lignocellulosic biomass and their potential applications in industrial biotechnology.
KpsS1 Mediates the Glycosylation of Pseudaminic Acid in Acinetobacter Baumannii
Authors: Cheung Yan Chu , Guo Xing , Yang Xuemei , Wei Ruohan , Chan Edward Waichi , Li Xuechen , Chen Sheng 
Published: April 2024

AbstractPseudaminic acid (Pse) is found in the polysaccharide structures of the cell surface of various Gram‐negative pathogenic bacteria including Acinetobacter baumannii and considered as an important component of cell surface glycans including oligosaccharides and glycoproteins. However, the glycosyltransferase that is responsible for the Pse glycosylation in A. baumannii remains unknown yet. In this study, through comparative genomics analysis of Pse‐positive and negative A. baumannii clinical isolates, we identified a potential glycosyltransferase, KpsS1, located right downstream of the Pse biosynthesis genetic locus. Deletion of this gene in an Pse‐positive A. baumannii strain, Ab8, impaired the glycosylation of Pse to the surface CPS and proteins, while the gene knockout strain, Ab8ΔkpsS1, could still produce Pse with 2.86 folds higher amount than that of Ab8. Furthermore, impairment of Pse glycosylation affected the morphology and virulence potential of A. baumannii, suggesting the important role of this protein. This study will provide insights into the further understanding of Pse in bacterial physiology and pathogenesis.
Wavelength‐Dependent Activation of Photoacids and Bases
Authors: Utroša Petra , Carroll Joshua A. , Žagar Ema , Pahovnik David , Barner‐Kowollik Christopher 
Published: April 2024

AbstractPhotoacids and bases allow remote control over pH in reaction solutions, which is of fundamental importance to an array of applications. Herein, we determine the wavelength‐by‐wavelength resolved photoreactivity of triarylsulfonium hexafluorophosphate salts as a representative photoacid generator and p‐(benzoyl)benzyl triethylammonium tetraphenylborate as a photobase generator, constructing a wavelength‐resolved photochemical action plot for each of the compounds. We monitor the pH change of the solution on‐line within the cavity of the laser vial and demonstrate a marked mismatch between the absorption spectrum of the photoacid and base with the photochemical action plot, unveiling reactivity at very low absorptivities. Our findings are of critical importance for the use of photoacids and bases, unambiguously demonstrating that absorption is no guide to chemical reactivity with critical consequences for the wavelength employed in applications of photoacids and bases.
Insight into the Effect of Methylglyoxal on the Conformation, Function, and Aggregation Propensity of α‐Synuclein
Authors: Mariño Laura , Belén Uceda Ana , Leal Francisco , Adrover Miquel 
Published: April 2024

AbstractIt is well‐known that people suffering from hyperglycemia have a higher propensity to develop Parkinson's disease (PD). One of the most plausible mechanisms linking these two pathologies is the glycation of neuronal proteins and the pathological consequences of it. α‐Synuclein, a key component in PD, can be glycated at its fifteen lysine. In fact, the end products of this process have been detected on aggregated α‐synuclein isolated from in vivo. However, the consequences of glycation are not entirely clear, which are of crucial importance to understand the mechanism underlying the connection between diabetes and PD. To better clarify this, we have here examined how methylglyoxal (the most important carbonyl compound found in the cytoplasm) affects the conformation and aggregation propensity of α‐synuclein, as well as its ability to cluster and fuse synaptic‐like vesicles. The obtained data prove that methylglyoxal induces the Lys‐Lys crosslinking through the formation of MOLD. However, this does not have a remarkable effect on the averaged conformational ensemble of α‐synuclein, although it completely depletes its native propensity to form soluble oligomers and insoluble amyloid fibrils. Moreover, methylglyoxal has a disrupting effect on the ability of α‐synuclein to bind, cluster and fusion synaptic‐like vesicles.