bluuebunny/crossref_metadata_2025_split huggingface dataset:
Super‐Droplet‐Repellent Carbon‐Based Printable Perovskite Solar Cells
Authors: Mai Cuc Thi Kim , Halme Janne , Nurmi Heikki A. , da Silva Aldeliane M. , Lorite Gabriela S. , Martineau David , Narbey Stéphanie , Mozaffari Naeimeh , Ras Robin H. A. , Hashmi Syed Ghufran , Vuckovac Maja 
Published: May 2024

AbstractDespite attractive cost‐effectiveness, scalability, and superior stability, carbon‐based printable perovskite solar cells (CPSCs) still face moisture‐induced degradation that limits their lifespan and commercial potential. Here, the moisture‐preventing mechanisms of thin nanostructured super‐repellent coating (advancing contact angle >167° and contact angle hysteresis 7°) integrated into CPSCs are investigated for different moisture forms (falling water droplets vs water vapor vs condensed water droplets). It is shown that unencapsulated super‐repellent CPSCs have superior performance under continuous droplet impact for 12 h (rain falling experiments) compared to unencapsulated pristine (uncoated) CPSCs that degrade within seconds. Contrary to falling water droplets, where super‐repellent coating serves as a shield, water vapor is found to physisorb through porous super‐repellent coating (room temperature and relative humidity, RH 65% and 85%) that increase the CPSCs performance for 21% during ≈43 d similarly to pristine CPSCs. It is further shown that water condensation forms within or below the super‐repellent coating (40 °C and RH 85%), followed by chemisorption and degradation of CPSCs. Because different forms of water have distinct effects on CPSC, it is suggested that future standard tests for repellent CPSCs should include rain falling and condensate formation tests. The findings will thus inspire the development of super‐repellent coatings for moisture prevention.
Coordination Confined Silver‐Organic Framework for High Performance Electrochemical Deionization
Authors: Wei Dun , Ouyang Baixue , Cao Yiyun , Yan Lvji , Wu Bichao , Chen Peng , Zhang Tingzheng , Jiang Yuxin , Wang Haiying 
Published: May 2024

AbstractSilver (Ag) is deemed a promising anode material for capacitive deionization (CDI) due to its high theoretical capacity and efficient selectivity to Cl−. However, the strong volume change during the conversion reaction significantly undermines the cycling performance of the Ag electrode. Additionally, achieving well‐dispersed Ag in the active matrix is challenging, as Ag electrodes prepared by conventional thermal reduction tend to agglomerate. Herein, the organic linker confinement strategy is proposed, applying metal–organic framework (MOF) chemistry between Ag nodes and organic ligands to construct Ag‐based MOF. The uniform dispersion of Ag at the molecular level, confined in the organic matrix, efficiently enhances the utilization of active sites, and strengthens the interfacial stability of Ag. Consequently, the Ag‐MOF for the CDI anode exhibits an excellent Cl− removal capacity of 121.52 mg g−1 at 20 mA g−1 in 500 mg L−1 NaCl solution, and a high Ag utilization rate of 60.54%. After 100 cycles, a capacity retention of 96.93% is achieved. Furthermore, the Cl− capture mechanism of Ag‐MOF is elucidated through density functional theory (DFT) calculations, ex situ XRD, ex situ Raman and XPS. This ingenious electrode design can offer valuable insights for the development of high‐performance conversion electrodes for CDI applications.
Leaky Integrate‐and‐Fire Model and Short‐Term Synaptic Plasticity Emulated in a Novel Bismuth‐Based Diffusive Memristor
Authors: Zawal Piotr , Abdi Gisya , Gryl Marlena , Das Dip , Sławek Andrzej , Gerouville Emilie A. , Marciszko‐Wiąckowska Marianna , Marzec Mateusz , Hess Grzegorz , Georgiadou Dimitra G. , Szaciłowski Konrad 
Published: May 2024

AbstractMemristors, being prospective work‐horses of future electronics offer various types of memory (volatile and nonvolatile) along with specific computational functionalities. Further development of memristive technologies depends on the availability of suitable materials. These materials should be easily available, stable, and preferably of low toxicity. Commonly used materials are lead halide perovskites, however, they are highly toxic and unstable under ambient conditions. Therefore a novel material is developed on the basis of bismuth iodide. In reaction with butylammonium iodide, it yields a novel compound, butylammonium iodobismuthate (BABI). Here, a diffusive memristor is introduced based on this compound and evaluates its memristive and neuromorphic properties. In contrast to nonvolatile memristors, the BABI memristors exhibit diffusive dynamics, which enable them to store the information only for short periods of time. This property is utilized to mimic the short‐term synaptic plasticity described by the leaky integrate‐and‐fire model of a biological neuron. Combined with high switching uniformity and self‐rectifying behavior, these devices show high classification accuracy for MNIST handwritten datasets, paving the way for their application in neuromorphic computing systems.
Dry Electrode Processing for High‐Performance Molten Salt Batteries
Authors: Wang Kuangyu , Wu Yulong , Yang Cheng , Yu Maosheng , Lei Chong , Zhang Yingchuan , Ding Tiezheng , Long Yuanzheng , Liu Kai , Li Meicheng , Wu Hui 
Published: May 2024

AbstractMolten salt batteries (MSBs) are renowned for their rapid reaction kinetics, high safety, and cost‐effectiveness. However, their electrode design faces challenges due to polymer binder incompatibility in molten salt electrolytes (MSEs). To address this, an expanded graphite (EG) electrode is proposed through a dry electrode processing method for MSE‐based aluminum‐ion batteries. This method facilitates the fabrication of large‐area electrodes featuring high active material loadings of up to ≈60 mg cm−2. Notably, the EG electrode exhibits remarkable rate performance, achieving a specific capacity of 84.4 mAh g−1 in the AlCl3‐NaCl‐KCl MSE at 125 °C with a current density of 5 A g−1. This outstanding performance can be attributed to its rapid multi‐step intercalation reaction kinetics and well‐developed pore structure. Leveraging the chemical stability and fibrillization binding mechanism of the polytetrafluoroethylene binder, the electrode demonstrates longevity over 10,000 cycles, despite experiencing a three‐fold volume expansion. Additionally, a 100‐mAh‐scale Al‐EG full‐cell cycled 100 times with an energy efficiency of 78.7% at 500 mA underscores its potential for large‐scale applications. Considering the broad applicability of this approach, it can also provide crucial references and insights for electrode design across various MSB systems.
A 2D Metallic KCu4S3 Anode for Fast‐Charging Sodium‐Ion Batteries
Authors: Lu Chengyi , Liu Lei , He Song , Li Boxin , Du Zhuzhu , Du Hongfang , Wang Xuefei , Zhang Shaowei , Ai Wei 
Published: May 2024

AbstractThe search for advanced electrode materials to solve slow ion diffusion and poor conductivity issues has spurred the development of fast‐charging sodium‐ion batteries (SIBs). Herein, a 2D metallic anode, KCu4S3, is reported expertly crafted using a KSCN molten salt approach, laying the foundation for fast‐charging SIBs. It is found that the mixed metal‐valence states within this compound provide substantial advantages, particularly in enhancing the high‐rate capability and ensuring long‐term durability. The mechanism that appears to facilitate these benefits can be traced to the formation of NaCu2S2 intermediate, which assist in electron transfer during Na+ (de)intercalation. In situ observations confirm the sodiation products of NaCu2S2 and sodium polysulfide can recover to the original phase upon desodiation. Such distinctive characteristics endow KCu4S3 with remarkable electrochemical performances, including an impressive capacity of 355 mAh g−1 at 20 A g−1 and 100% capacity retention within 3000 cycles. Moreover, the full cell exhibits a high energy density of 332 Wh kg−1 and retains 92% of its capacity across 150 cycles at 1 A g−1. This work opens new horizons in the field of fast‐charging materials, making a significant step forward in shaping the future of SIBs.
An assessment of agroforestry as a climate‐smart practice: Evidences from farmers of northwestern region of Bangladesh
Authors: Ali Md. Manik , Ahmad Babor , Bari Md Shafiqul , Pal Abinash Chandra , Rahman Md. Lutfor , Sarmin Israt Jahan 
Published: May 2024

AbstractAgroforestry systems have grown significantly in popularity in Bangladesh during recent years due to their favorable effects on the environment and human health. These systems are essential for supporting sustainable agriculture because they increase diversity, improve food security, and provide revenue. This study's main objective is to show how agroforestry is a widely used ecological and climate‐resilient practice in Bangladesh. The research explores investment analysis, adoption‐influencing factors, and a strength, weakness, opportunities, and threats (SWOT) analysis of agroforestry practices. A total of 340 respondents were chosen for this extensive study using a multistage random selection technique. The results showed a discrepancy in practice, with farmers exhibiting a high degree of awareness but limited application. Financial analysis employing metrics such as benefit‐cost ratio, net present value, and internal rate of return favored agroforestry, indicating its economic viability and potential benefits for adopters. Additionally, the adoption of agroforestry was found to be significantly influenced by a binary logistic regression model that highlighted several important features, including larger farm sizes, younger age groups, greater education levels, training experiences, frequent extension visits, and enhanced market access. The study also identified barriers to adoption, such as a lack of trained labor, poor technical assistance, and education. This thorough analysis clarifies the opportunities and constraints for agroforestry implementation in Bangladesh. It suggests broad adoption by means of focused training initiatives that empower farmers, provide observable advantages, and promote nationwide acceptance.
Gold‐Catalysierte Heck Reaktion: Wunschtraum oder Wirklichkeit? Korrespondenz zu “Unlocking the Chain Walking Process in Gold Catalysis”
Authors: Budzelaar Peter H. M. , Bochmann Manfred , Landrini Martina , Rocchigiani Luca 
Published: May 2024

AbstractIn zwei vielbeachteten Veröffentlichungen wurde vor kurzem über die Bildung von arylierten Heck‐Olefinen durch Katalyse mit MeDalPhosAuCl/AgOTf (J. Am. Chem. Soc. 2023, 145, 8810) und ihre Cyclisierung zu Tetralinen berichtet (Angew. Chem. Int. Ed. 2023, e202312786). Es wurde behauptet, es handle sich dabei um den erstmaligen Nachweis von Gold‐katalysierten Alken‐Insertionen in Au‐Aryl‐Bindungen, β‐H‐Eliminierung und Kettenwanderung durch Au−H. Wir zeigen hier, dass es sich dabei tatsächlich aber um einen Zweistufenprozess handelt, wobei nur der erste Schritt, die Bildung eines Alkyltriflat‐Esters als primäres organisches Produkt durch die wohlbekannte Alken‐Heteroarylierungssequenz, einen Gold‐Katalysator involviert. Die nachfolgende Umsetzung zu Heck‐Olefinen sowie deren Cyclisierung zu Tetralinen ist klassische, H+‐initiierte Carbokationenchemie. Diese Schritte finden auch unter Gold‐freien Bedingungen statt, mit identischen Resultaten. Literaturberichte über neuartige Reaktivität von Gold‐Katalysatoren, wie Kettenwanderung durch das hypothetische [LAuH]2+ Dikation, entbehren jeder faktischen Grundlage.
NETosis‐Inspired Cell Surface‐Constrained Framework Nucleic Acids Traps (FNATs) for Cascaded Extracellular Recognition and Cellular Behavior Modulation
Authors: Gong Hangsheng , Zhang Yihan , Xue Yuan , Fang Bowen , Li Yuting , Zhu Xudong , Du Yi , Peng Pai 
Published: May 2024

AbstractUpon pathogenic stimulation, activated neutrophils release nuclear DNA into the extracellular environment, forming web‐like DNA structures known as neutrophil extracellular traps (NETs), which capture and kill bacteria, fungi, and cancer cells. This phenomenon is commonly referred to as NETosis. Inspired by this, we introduce a cell surface‐constrained web‐like framework nucleic acids traps (FNATs) with programmable extracellular recognition capability and cellular behavior modulation. This approach facilitates dynamic key chemical signaling molecule recognition such as adenosine triphosphate (ATP), which is elevated in the extracellular microenvironment, and triggers FNA self‐assembly. This, in turn, leads to in situ tightly interwoven FNAs formation on the cell surface, thereby inhibiting target cell migration. Furthermore, it activates a photosensitizer‐capturing switch, chlorin e6 (Ce6), and induces cell self‐destruction. This cascade platform provides new potential tools for visualizing dynamic extracellular activities and manipulating cellular behaviors using programmable in situ self‐assembling DNA molecular devices.
Elektrokatalytische formale C(sp2)−H Alkylierung via Nickel‐katalysierter elektrophiler Kreuzkupplung mit vielseitigen Arylsulfoniumsalzen
Authors: Michiyuki Takuya , Homölle Simon L. , Pandit Neeraj K. , Ackermann Lutz 
Published: May 2024

AbstractDie Synthese sp3‐hybridsierter kohlenstoffreicher Moleküle ist aufgrund ihrer Bedeutung und ihres Erfolgs insbesondere in klinischen Studien von besonderem Interesse. In dieser Arbeit wurde das Einbringen von aliphatischen Ketten auf ein aromatisches Gerüst durch eine Nickel‐katalysierte C(sp2)−C(sp3) elektrophile Kreuzkupplungen mit Arylsulfoniumsalzen erreicht. So konnten einfach, nichtpräfunktionalisiere Arene durch die Bildung von Aryldibenzothiopheniumsalze alkyliert werden. Durch den elektrochemischen Ansatz können potenziell gefährliche chemische Redoxreagenzien vermieden werden. Insbesondere die Ein‐Topf Alkylierung erwies sich als praktikabel, was die Robustheit unseres Ansatzes unterstreicht.
Anion‐Reinforced Solvation Structure Enables Stable Operation of Ether‐Based Electrolyte in High‐Voltage Potassium Metal Batteries
Authors: Gu Mengjia , Zhou Xunzhu , Yang Qian , Chu Shenxu , Li Lin , Li Jiaxin , Zhao Yuqing , Hu Xing , Shi Shuo , Chen Zhuo , Zhang Yu , Chou Shulei , Lei Kaixiang 
Published: May 2024

AbstractElectrolytes with anion‐dominated solvation are promising candidates to achieve dendrite‐free and high‐voltage potassium metal batteries. However, it's challenging to form anion‐reinforced solvates at low salt concentrations. Herein, we construct an anion‐reinforced solvation structure at a moderate concentration of 1.5 M with weakly coordinated cosolvent ethylene glycol dibutyl ether. The unique solvation structure accelerates the desolvation of K+, strengthens the oxidative stability to 4.94 V and facilitates the formation of inorganic‐rich and stable electrode‐electrolyte interface. These enable stable plating/stripping of K metal anode over 2200 h, high capacity retention of 83.0 % after 150 cycles with a high cut‐off voltage of 4.5 V in K0.67MnO2//K cells, and even 91.5 % after 30 cycles under 4.7 V. This work provides insight into weakly coordinated cosolvent and opens new avenues for designing ether‐based high‐voltage electrolytes.
Zeolitic Imidazolate Frameworks as Solid‐State Nanomachines
Authors: Nam Joohan , Kim Seokjin , Jin Eunji , Lee Soochan , Cho Hye Jin , Min Seung Kyu , Choe Wonyoung 
Published: May 2024

AbstractMachines have continually developed with the needs of daily life and industrial applications. While the careful design of molecular‐scale devices often displays enhanced properties along with mechanical movements, controlling mechanics within solid‐state molecular structures remains a significant challenge. Here, we explore the distinct mechanical properties of zeolitic imidazolate frameworks (ZIFs)—frameworks that contain hidden mechanical components. Using a combination of experimental and theoretical approaches, we uncover the machine‐like capabilities of ZIFs, wherein connected composite building units operate similarly to a mechanical linkage system. Importantly, this research suggests that certain ZIF subunits act as core mechanical components, paving an innovative view for the future design of solid‐state molecular machines.
Alkene 1,3‐Difluorination via Transient Oxonium Intermediates
Authors: Dean Alice C. , Randle E. Harvey , Lacey Andrew J. D. , Marczak Giorio Guilherme A. , Doobary Sayad , Cons Benjamin D. , Lennox Alastair J. J. 
Published: May 2024

AbstractThe 1,3‐difunctionalization of unactivated alkenes is an under‐explored transformation that leads to moieties that are otherwise challenging to prepare. Herein, we report a hypervalent iodine‐mediated 1,3‐difluorination of homoallylic (aryl) ethers to give unreported 1,3‐difluoro‐4‐oxy groups with moderate to excellent diastereoselectivity. The transformation proceeds through a different mode of reactivity for 1,3‐difunctionalization, in which a regioselective addition of fluoride opens a transiently formed oxonium intermediate to rearrange an alkyl chain. The optimized protocol is scalable and shown to proceed well with a variety of functional groups and substitution on the alkenyl chain, hence providing ready access to this fluorinated, conformationally controlled moiety.
[2+1] Cycloadditions Modulate the Hydrophobicity of Ni‐N4 Single‐Atom Catalysts for Efficient CO2 Electroreduction
Authors: Shu Siyan , Song Tao , Wang Cheng , Dai Hao , Duan Lele 
Published: May 2024

AbstractMicroenvironment regulation of M‐N4 single‐atom catalysts (SACs) is a promising way to tune their catalytic properties toward the electrochemical CO2 reduction reaction. However, strategies that can effectively introduce functional groups around the M‐N4 sites through strong covalent bonding and under mild reaction conditions are highly desired. Taking the hydrophilic Ni‐N4 SAC as a representative, we report herein a [2+1] cycloaddition reaction between Ni‐N4 and in situ generated difluorocarbene (F2C:), and enable the surface fluorocarbonation of Ni‐N4, resulting in the formation of a super‐hydrophobic Ni‐N4‐CF2 catalyst. Meanwhile, the mild reaction conditions allow Ni‐N4‐CF2 to inherit both the electronic and structural configuration of the Ni‐N4 sites from Ni‐N4. Enhanced electrochemical CO2‐to‐CO Faradaic efficiency above 98 % is achieved in a wide operating potential window from −0.7 V to −1.3 V over Ni‐N4‐CF2. In situ spectroelectrochemical studies reveal that a highly hydrophobic microenvironment formed by the −CF2− group repels asymmetric H‐bonded water at the electrified interface, inhibiting the hydrogen evolution reaction and promoting CO production. This work highlights the advantages of [2+1] cycloaddition reactions on the covalent modification of N‐doped carbon‐supported catalysts.
Patterned Photonic Actuators with Dynamic Shape‐Morphing and Color‐Changing Capabilities Fabricated by Athermal Embossing Technology
Authors: Qian Nina , Hu Jun , Huang Shuai , Liu Zhiyang , Wang Meng , Keller Patrick , Yang Hong 
Published: May 2024

AbstractStimuli‐responsive patterned photonic actuators, characterized by their patterned nano/microscale structures and capacity to demonstrate synergistic color changes and shape morphing in response to external stimuli, have attracted intense scientific attention. However, traditional patterned photonic actuator systems still face limitations such as cumbersome and time‐consuming preparation processes and small‐scale deformations. Herein, we introduce a facile approach involving an athermal embossing technique to rapidly fabricate patterned photonic actuators based on near‐infrared (NIR) light‐responsive liquid crystal elastomers. The resulting patterned photonic actuators demonstrate remarkable features, including brilliant angle‐dependent structural color, complex three‐dimensional actuation, and good color durability under NIR light stimulation. As illustrative demonstrations of the proof‐of‐concept, we fabricate two light‐fuelled patterned photonic soft actuators: a butterfly‐inspired actuator that can produce wing‐flapping dynamic changes in structural color, and an origami crane‐shaped actuator with shape memory, structural color information storage, and dynamic display properties. This strategy provides distinct insights into the design and fabrication of various patterned photonic soft robotic devices and intelligent actuators.
Intermolecular Enantioselective Amination Reactions Mediated by Visible Light and a Chiral Iron Porphyrin Complex
Authors: Ahmed Hussayn , Ghosh Biki , Breitenlechner Stefan , Feßner Malte , Merten Christian , Bach Thorsten 
Published: May 2024

AbstractIn the presence of 1 mol % of a chiral iron porphyrin catalyst, various 3‐arylmethyl‐substituted 2‐quinolones and 2‐pyridones underwent an enantioselective amination reaction (20 examples; 93–99 % ee). The substrates were used as the limiting reagents, and fluorinated aryl azides (1.5 equivalents) served as nitrene precursors. The reaction is triggered by visible light which allows a facile dediazotation at ambient temperature. The selectivity of the reaction is governed by a two‐point hydrogen bond interaction between the ligand of the iron catalyst and the substrate. Hydrogen bonding directs the amination to a specific hydrogen atom within the substrate that is displaced by the nitrogen substituent either in a concerted fashion or by a rebound mechanism.
Stabilizing Few‐Atom Platinum Clusters by Zinc Single‐Atom‐Glue for Efficient Anti‐Markovnikov Alkene Hydrosilylation
Authors: Li Ruilong , Yu Ge , Lin Ze , Lin Xingen , Du Junyi , Gao Xiaoping , Su Chenliang , Wu Yuen 
Published: May 2024

AbstractFew‐atom metal clusters (FAMCs) exhibit superior performance in catalyzing complex molecular transformations due to their special spatial environments and electronic states, compared to single‐atom catalysts (SACs). However, achieving the efficient and accurate synthesis of FAMCs while avoiding the formation of other species, such as nanoparticles and SACs, still remains challenges. Herein, we report a two‐step strategy for synthesis of few‐atom platinum (Pt) clusters by predeposition of zinc single‐atom‐glue (Zn1) on MgO nanosheets (Ptn−Zn1/MgO), where FAMCs can be obtained over a wide range of Pt contents (0.09 to 1.45 wt %). Zn atoms can act as Lewis acidic sites to allow electron transfer between Zn and Pt through bridging O atoms, which play a crucial role in the formation and stabilization of few‐atom Pt clusters. Ptn−Zn1/MgO exhibited a high selectivity of 93 % for anti‐Markovnikov alkene hydrosilylation. Moreover, an excellent activity with a turnover frequency of up to 1.6×104 h−1 can be achieved, exceeding most of the reported Pt SACs. Further theoretical studies revealed that the Pt atoms in Ptn−Zn1/MgO possess moderate steric hindrance, which enables high selectivity and activity for hydrosilylation. This work presents some guidelines for utilizing atomic‐scale species to increase the synthesis efficiency and precision of FAMCs.