bluuebunny/crossref_metadata_2025_split huggingface dataset:
Bottom‐up Synthesis of Piezoelectric Covalent Triazine‐based Nanotube for Hydrogen Peroxide Production from Water and Air
Authors: Guan Lijiang , Li Zhi , Wang Kai , Gong Li , Fang Yuanyuan , Yu Guipeng , Zhu Mingshan , Jin Shangbin 
Published: November 2024

AbstractCarbon nanotubes (CNTs) are nanoscale tubular materials with superior mechanical strength and electronic properties. However, the conventional CNTs are inherently non‐piezoelectric, mainly due to the lack of polar structures with pure carbon elements. The direct synthesis of fully conjugated and polarized organic nanotubes with desired piezoelectric properties remains a challenge. Herein, we report the bottom‐up synthesis of a new type of covalent triazine‐based nanotube (CTN‐1) as a novel piezoelectric material. The CTN‐1 comprises of high surface area, nitrogen‐rich and fully conjugated structure, which provides a series of merits for piezoelectric catalytic processes. These structural features combined with one‐dimensional tubular morphology endow CTN‐1 with excellent mechanical stimuli response and thus displaying prominent piezoelectric properties via pronounced nanocurvature effect. We further show that the CTN‐1 enables the efficient synthesis of H2O2 from water in the air via mechanical energy conversion, with an excellent piezocatalytic H2O2 evolution rate of 4115 μmol g−1 h−1, which exceeds other reported piezoelectric materials. The piezocatalysis by the CTN‐1 can be practically integrated into a self‐Fenton system, which exhibits excellent pollutant degradation capability. This work demonstrates the enormous potential of a new type of piezoelectric synthetic nanotube from organic frameworks for the in situ synthesis valuable chemicals.
Locking up G‐Quadruplexes with Light‐Triggered Staples Leads to Increased Topological, Thermodynamic, and Metabolic Stability
Authors: Barr Jack , Cadoni Enrico , Schellinck Sofie , Laudadio Emiliano , Martins José C. , Madder Annemieke 
Published: November 2024

AbstractG‐quadruplexes (G4 s) are secondary, tetraplexed DNA structures abundant in non‐coding regions of the genome, implicated in gene transcription processes and currently firmly recognised as important potential therapeutic targets. Given their affinity for human proteins, G4 structures are investigated as potential decoys and aptamers. However, G4 s tend to adopt different conformations depending on the exact environmental conditions, and often only one displays the specifically desired biological activity. Their less intensively studied counterparts, the elusive tetraplexed intercalated‐motifs (IMs) are typically unstable at neutral pH, hampering the investigation of their potential involvement in a biological context. We herein report on a photochemical method for “stapling” such tetraplexed‐structures, to increase their stability, lock their topology and enhance their enzymatic resistance, while maintaining biological activity. The chemical structure and topology of the stapled Thrombin Binding Aptamer (TBA) was spectroscopically characterised and rationalised in silico. The method was then extended to other biologically relevant G4‐ and IM‐prone sequences, hinting towards potential application of such stapled structures in a therapeutic context.
Visualization and Quantification of Single‐Base m6A Methylation
Authors: Zhang Qiushuang , Dai Yicong , Teng Xucong , Li Jinghong 
Published: November 2024

AbstractN6‐methyladenosine (m6A) has emerged as the most prevalent form of RNA modification found across various RNA classes. The detection and quantification of m6A RNA modifications under various physiological conditions are crucial for elucidating disease mechanisms and identifying potential therapeutic targets. However, visualizing intracellular m6A modifications at single‐base resolution remains a significant challenge. Existing methods based on high‐throughput sequencing or in vitro assays are not suitable for in situ m6A RNA imaging. In this work, we introduce the TadA8.20‐assisted N6‐methyladenosine RNA imaging at single‐base resolution (TARS) method for precise visualization and quantification of both A and m6A forms at specific RNA sites within single cells. Validation studies using TARS on MALAT1 lncRNA in HeLa cells and CCND1 mRNA in breast cancer cell lines demonstrated its high specificity and efficiency in mapping and quantifying m6A modifications at single‐base resolution. TARS represents a novel tool that advances m6A RNA modification research by offering accurate and detailed insights into m6A modifications at the single‐base level.
Structure Prediction and Computational Protein Design for Efficient Biocatalysts and Bioactive Proteins
Authors: Buller Rebecca , Damborsky Jiri , Hilvert Donald , Bornscheuer Uwe T. 
Published: November 2024

AbstractThe ability to predict and design protein structures has led to numerous applications in medicine, diagnostics and sustainable chemical manufacture. In addition, the wealth of predicted protein structures has advanced our understanding of how life's molecules function and interact. Honouring the work that has fundamentally changed the way scientists research and engineer proteins, the Nobel Prize in Chemistry in 2024 was awarded to David Baker for computational protein design and jointly to Demis Hassabis and John Jumper, who developed AlphaFold for machine‐learning‐based protein structure prediction. Here, we highlight notable contributions to the development of these computational tools and their importance for the design of functional proteins that are applied in organic synthesis. Notably, both technologies have the potential to impact drug discovery as any therapeutic protein target can now be modelled, allowing the de novo design of peptide binders and the identification of small molecule ligands through in silico docking of large compound libraries. Looking ahead, we highlight future research directions in protein engineering, medicinal chemistry and material design that are enabled by this transformative shift in protein science.
Unraveling the Configuration Modulation in Spiro‐Based Through‐Space Charge Transfer Materials
Authors: Qu Yang‐Kun , Zheng Qi , Zhou Dong‐Ying , Cui Lin‐Song , Liao Liang‐Sheng , Jiang Zuo‐Quan 
Published: November 2024

AbstractThermally activated delayed fluorescence (TADF) materials hold promise for optoelectronic applications. Among various design strategies, through‐space charge transfer (TSCT) systems offer the potential for enhanced performance. However, the relationship between molecular configuration and TSCT properties remains unclear compared to traditional through‐band charge transfer materials. In this study, we investigated the influence of spatial configuration on TSCT features and electronic properties of triplet excited states in these TSCT materials. By manipulating the spatial arrangement between donor and acceptor segments using different spiro skeletons, a series of TSCT materials (DMB2‐DMB5) was synthesized. Together with the parent molecule, DM‐B, these materials exhibited completely different TADF characteristics, demonstrating the impact of spatial arrangements on their optoelectronic properties. Thus, the external quantum efficiency of these materials ranged from as high as 28.0 % (DMB2) to as low as 3.6 % (DMB5) due to variations in their TADF characteristics. Our findings highlight the significance of spatial configuration, beyond distance alone, in influencing TSCT properties when donor and acceptor segments are sufficiently close. This insight provides valuable guidance for developing advanced TSCT materials and advancing TADF systems with improved performance and functionality.
Subtle Modifications in Interface Configurations of Iron/Cobalt Phthalocyanine‐Based Electrocatalysts Determine Molecular CO2 Reduction Activities
Authors: Xin Yinger , Musgrave Charles B. , Su Jianjun , Li Jiangtong , Xiong Pei , Meng‐Jung Li Molly , Song Yun , Gu Qianfeng , Zhang Qiang , Liu Yong , Guo Weihua , Cheng Le , Tan Xuefeng , Jiang Qiu , Xia Chuan , Zhong Tang Ben , Goddard William A. , Ye Ruquan 
Published: November 2024

AbstractStrain engineering has emerged as a powerful approach in steering material properties. However, the mechanism and potential limitations remain poorly understood. Here we report that subtle changes in molecular configurations can profoundly affect, conducively or adversely, the catalytic selectivity and product turnover frequencies (TOFs) of CO2 reduction reaction. Specifically, introducing molecular curvature in cobalt tetraaminophthalocyanine improves the multielectron reduction activity by favorable *CO hydrogenation, attaining methanol Faradaic efficiency up to 52 %. In stark contrast, strained iron phthalocyanine exacerbates *CO poisoning, leading to decreased TOFCO by >50 % at −0.5 VRHE and a rapid current decay. The uniform dispersion is crucial for optimizing electron transfer, while activity is distinctly sensitive to the local atomic environment around the active sites. Specifically, local strain either enhances binding to intermediates or poisons the catalytic sites. Our comprehensive analysis elucidates the intricate relationship between molecular structure and activities, offering insights into designing efficient heterogeneous molecular interfaces.
Highly Conductive Multifunctional Iron‐Incorporated Polythiophene Nanocomposite: A Nanocatalyst for Nitrobenzene Reduction in Aqueous Medium and an Efficient Room Temperature Methanol Gas Sensor
Authors: Devi Shrutipriya , Kalita Amar Jyoti , Chetia Rupkamal , Mazumder Lakhya J. , Guha Ankur K. , Chetia Bolin , Konwer Surajit 
Published: November 2024

ABSTRACTThis study reports the synthesis and application of a polythiophene–iron oxide (PTh‐Fe0‐Fe2O3) nanocomposite as a highly effective catalyst for the selective reduction of nitro aromatics in an aqueous environment. The nanocomposite was synthesized using in situ chemical polymerization, with Fe0‐Fe2O3 nanoparticles created from ferric chloride solution using Camellia sinensis leaf extract as a reducing and stabilizing agent at room temperature. Characterization techniques, including XRD, FTIR, SEM–EDX, TEM, XPS, and UV–Vis spectroscopy, confirmed the successful integration of Fe0‐Fe2O3 into the polythiophene matrix. The nanocomposite demonstrated higher electrical conductivity compared to PTh alone, ranging from 20 S/cm at 313 K to 53 S/cm at 373 K. Magnetic studies indicated a saturation magnetization of 23.1 emu/g, lower than the 42.6 emu/g of Fe0‐Fe2O3 nanoparticles, attributed to the non‐magnetic nature of PTh. Under optimal conditions (4‐nitrobenzaldehyde [1 mmol], catalyst [0.04 g], and water [5 mL] in air), the catalyst achieved a 94% yield in the reduction of nitrobenzenes within 7 h, demonstrating broad applicability and retaining significant catalytic activity over six cycles. Furthermore, the PTh‐ Fe0‐Fe2O3 nanocomposite exhibited notable methanol gas sensing capabilities, with a sensitivity of 52.6 at 200‐ppm methanol. The sensor exhibited a response time of 60 s and a recovery time of 80 s, attributed to its n‐type semiconductor characteristics and abundant oxidative‐reductive sites. Computational studies supported the methanol sensing mechanism, highlighting significant O… S interactions and stable non‐covalent interactions between methanol and the nanocomposite. This study is the first to introduce a novel magnetic nanocatalyst for the cost‐effective and eco‐friendly reduction of nitroarenes, while also demonstrating its applicability in gas sensing. The research highlights an environmentally sustainable synthesis process and enhanced material properties, showcasing the nanocatalyst's potential for diverse applications.
Discovery of Imidazo[1,2‐a]pyrimidine–Schiff Base Derivatives as Potent Antifungal Agents Against Fusarium oxysporum f. sp. albedinis: Synthesis, Crystal Structure, Biological Evaluation, Homology Modeling, and Docking Analysis
Authors: Azzouzi Mohamed , El Hadad Salah Eddine , Ouchaoui Abderrahim Ait , Benabbes Redouane , Neffa Mounsef , Abboud Mohamed , Touzani Rachid , Hammouti Belkheir , Oussaid Adyl , Salghi Rachid , Chaouiki Abdelkarim 
Published: November 2024

ABSTRACTBayoud disease, which is caused by the fungus Fusarium oxysporum f. sp. albedinis (FOA), is a severe threat to date palm cultivation in North Africa and the Middle East; thus, effective antifungal treatments are urgently required. In response to this, the present study develops, characterizes, and tests imidazo[1,2‐a]pyrimidine–Schiff base derivatives as potential antifungal compounds. A series of these derivatives (labeled IMP‐1 to IMP‐6) was obtained using a facile conventional synthetic route that holds the potential for scalable production. The structures of the samples were characterized using traditional spectroscopic techniques, while IMP‐1 and IMP‐3 were subjected to single‐crystal X‐ray diffraction analysis to verify the structural assignment of the synthesized compounds. Screening analysis of the antifungal activity of the IMPs against FOA demonstrated remarkable inhibition effects, with IC50 values ranging from 4.7 to 2.6 μg/mL. In particular, IMP‐6 demonstrated exceptional potency, with an inhibition rate exceeding 97% at a low concentration of only 16.42 μM, thus outperforming many previously reported antifungal compounds. Homology modeling and molecular docking analysis were also conducted to understand how these novel antifungal agents interact with their target, with the experimental and theoretical approaches producing consistent results.
Enhanced Energy Storage Properties of PP/PA11 Dielectric Composite Films With PP‐g‐MAH as Compatibilizer
Authors: Liu Xiaomeng , Xie Junhao , Zhong Shaoyuan , Sun Shulin 
Published: November 2024

ABSTRACTAs an energy storage capacitor film material, polypropylene (PP) suffers from its low dielectric constant and limited energy density. To overcome the defects of pure PP, the PP‐based all‐organic composite films with multiple interfaces have been constructed to enhance the dielectric and energy storage properties. In this research, PA11 was used to blend with PP with polypropylene grafted maleic anhydride (PP‐g‐MAH) as compatibilizer. The prepared PP/PP‐g‐MAH/PA11 composites formed the typical “sea‐island” structure and double interfaces between PP/PP‐g‐MAH and PP‐g‐MAH/PA11. The higher molecular polarity of PP‐g‐MAH, PA11, and interfacial polarization significantly increases the dielectric constant of the composite films. Furthermore, the formation of interface traps suppressed the migration of charge carriers, resulting in lower leakage current and higher breakdown strength of the PP/PP‐g‐MAH/PA11 composite films. Density functional theory (DFT) simulation further proved the confinement of space charges. Energy storage results showed the optimal PP/PP‐g‐MAH/PA11‐2 film achieved high energy density (4.49 J/cm3) and excellent charge/discharge efficiency (97.4%), which behaved good application prospect in the field of thin film capacitors.
Design of Hydrolysis, Enzymatic and Soil‐Degradation Diglycolate‐Based Copolyesters With Good Mechanical and Thermal Properties
Authors: Dong Liming , Li Deling , Zhuang Wenchang , Ding Yue 
Published: November 2024

ABSTRACTIn this paper, a series of poly(butylene diglycolate‐co‐succinate‐co‐furandicarboxylate) (PBSFD) and poly(butylene diglycolate‐co‐adipate‐furandicarboxylate) (PBAFD) copolymers were synthesized to enhance the degradation rate of PBAF and PBSF. The structure and properties were tested. PBAFD and PBSFD copolymers display impressive biodegradability when catalyzed by candida antarctica lipase B. The weight loss of copolymers was more than 75% after 14 days degradation. Compared to PBSFD copolymers, the PBAFDs owned better soil degradability, resulting in weight loss was 89.1% when the molar ratio of diglycolic acid was 30% after 70 days degradation. Also, the stress of PBAFD30 was 17.1 Mpa, and the elongation at break was more than 900%. The temperature of 5% mass loss of PBAFD30 was as high as 371.3°C. Thus, PBAFD and PBSFD copolymers have good application prospects in single‐use packaging materials.
Tunable Luminescence of Glyoxylic Acid Modified Poly (Vinyl Alcohol) Film Codoped With Eu2+ and Eu3+
Authors: Chen Wanping , Wang Ke , Ren Baoru 
Published: November 2024

ABSTRACTPoly(vinyl alcohol) (PVA), a high‐consumption polymer, is currently facing the problem of overcapacity. The development of modified PVA with novel properties is an alternative way to solve this problem. In this work, glyoxylic acid was used as a bridging agent to indirectly bond europium ions to PVA molecule chain. The luminescence properties of the modified PVA materials were investigated by adjusting the reaction conditions such as pH value, heating treatment methods, reaction temperature, and doping concentration. Upon excitation at 394 nm, a strong and tunable luminescence is achieved due to the existence of both blue emission from Eu2+ and red emission from Eu3+. The luminescence properties are explained based on the reduction of Eu3+, the existence form of europium ions, and the arranged regulation of PVA molecules. The modified PVA materials have potential applications in the fields of displaying and lighting if their luminescence properties are further improved in the future.
Effect of Bio‐Based Plasticizers From Modified Vegetable Oils in a New Formulation of PVC Materials
Authors: Akter Sharmin , Rahman Md Mahbubur , Auerbach Marcel , Langer Beate 
Published: November 2024

ABSTRACTThis study investigates the performance of polyvinyl chloride (PVC) plasticized with diisononyl phthalate (DINP), rapeseed oil epoxidized ester (ROE), and rapeseed oil carbonated ester (ROC). The formulations were evaluated for surface resistance, wettability, migration, mechanical properties, and resistance to aging and thermal degradation. PVC/ROC exhibited the highest surface resistance of 1.5 × 1016 Ω, indicating superior electrical insulation. Wettability tests showed PVC/ROE with the highest contact angle at 63°, while PVC/ROC and PVC/DINP demonstrated lower contact angles of 44° and 43°, respectively. Migration tests revealed that PVC/ROC had the lowest migration rates: 0.1% in distilled water and 1.5% in 95% ethanol. Mechanical testing under algae exposure demonstrated that PVC/ROC achieved the highest tensile strength of 43 MPa and a strain at break of 200%. After 1008 h of thermo‐oxidative aging, PVC/ROC retained superior tensile strength and hardness, while PVC/ROE showed a slight decrease. PVC/ROC also demonstrated improved thermal stability at 255°C compared with DINP (245°C). These results confirm that ROC is an effective bio‐based plasticizer, providing enhanced mechanical properties, reduced migration, and greater durability compared to conventional DINP, offering a sustainable alternative for diverse PVC applications in medical, automotive, and packaging industries.
Accelerating Drug Discovery With High‐Throughput Crystallographic Fragment Screening and Structural Enablement
Authors: Fearon Daren , Powell Ailsa , Douangamath Alice , Dias Alexandre , Tomlinson Charles W. E. , Balcomb Blake H. , Aschenbrenner Jasmin C. , Aimon Anthony , Barker Isabel A. , Brandão‐Neto José , Collins Patrick , Dunnett Louise E. , Fairhead Michael , Gildea Richard J. , Golding Mathew , Gorrie‐Stone Tyler , Hathaway Paul V. , Koekemoer Lizbé , Krojer Tobias , Lithgo Ryan M. , Maclean Elizabeth M. , Marples Peter G. , Ni Xiaomin , Skyner Rachael , Talon Romain , Thompson Warren , Wild Conor F. , Winokan Max , Wright Nathan David , Winter Graeme , Shotton Elizabeth J. , von Delft Frank , Bertram Felicity , Coe Paul A. , Mikolajek Halina , Nidamarthi Kutumbarao H. V. , O'Donnell Garry , Watt Grant , Williams Mark A. 
Published: November 2024

ABSTRACTFragment‐based drug discovery is a well‐established method for the identification of chemical starting points for development into clinical candidates. Historically, crystallographic fragment screening was perceived to be low‐throughput and time consuming. However, thanks to advances in synchrotron capabilities and the introduction of dedicated facilities, such as the XChem platform at Diamond Light Source, there have been substantial improvements in throughput and integration between sample preparation, data collection and hit identification. Herein we share our experiences of establishing a crystallographic fragment screening facility, our learnings from operating a user programme for ten years and our perspective on applying structural enablement to rapidly progress initial fragment hits to lead‐like molecules.
Giant Inverse Barocaloric Effect of Ferroelectric Salts Driven by Negative Thermal Expansion
Authors: Dai Yin , Wu Menghao 
Published: November 2024

AbstractRefrigeration technologies based on the barocaloric effect have garnered significant attention, while their potential applications are limited by the poor performance of current materials. Here it is proposed that ferroelectric ionic salts with covalent‐like bondings like LiI may become ideal candidates. The pressure‐induced phase transition between two phases with distinct densities and entropies leads to tremendous negative thermal expansion (with volume reduced by 13%) and inverse barocaloric effect, which are facilitated by the low transition barriers due to the long‐range Coulomb interaction. Using ab initio‐based training database, we trained the machine learning potential of LiI based on a deep neutral network‐based mode, and this simulations of its barocaloric effect reveal a high entropy change and thermal conductivity, and in particular, the estimated adiabatic temperature change, pressure sensitivity and relative cooling power are all unprecedented. This prediction provides a high‐performance barocaloric mechanism for practical applications and also expands the scope of barocaloric materials to simple and facile binary salts.