bluuebunny/crossref_metadata_2025_split huggingface dataset:
Revealing Steric‐Hindrance‐Dependent Buried Interface Defect Passivation Mechanism in Efficient and Stable Perovskite Solar Cells with Mitigated Tensile Stress
Authors: Zhou Qian , He Dongmei , Zhuang Qixin , Liu Baibai , Li Ru , Li Hongxiang , Zhang Zhongying , Yang Hua , Zhao Pengjun , He Yong , Zang Zhigang , Chen Jiangzhao 
Published: June 2022

AbstractInterface engineering is one feasible and effective approach to minimize the interfacial nonradiative recombination stemming from interfacial defects, interfacial residual stress, and interfacial energy level mismatch. Herein, a novel and effective steric‐hindrance‐dependent buried interface defect passivation and stress release strategy is reported, which is implemented by adopting a series of adamantane derivative molecules functionalized with CO (i.e., 2‐adamantanone (AD), 1‐adamantane carboxylic acid (ADCA), and 1‐adamantaneacetic acid (ADAA)) to modify SnO2/perovskite interface. All modifiers play a role in passivating interfacial defects, mitigating interfacial strain, and enhancing device performance. The steric hindrance of chemical interaction between CO in these molecules and perovskites as well as SnO2 is determined by the distance between CO and bulky adamantane ring, which gradually decreases from AD, ADCA, and ADAA. The experimental and theoretical evidences together confirmed steric‐hindrance‐dependent defect passivation effect and interfacial chemical interaction strength. The interfacial chemical interaction strength, defect passivation effect, stress release effect and thus device performance are negatively correlated with steric hindrance. Consequently, the ADAA‐modified device achieves a seductive efficiency up to 23.18%. The unencapsulated devices with ADAA maintain 81% of its initial efficiency after aging at 60 °C for 1000 h.
Convection Driven Ultrarapid Protein Detection via Nanobody‐Functionalized Organic Electrochemical Transistors
Authors: Koklu Anil , Wustoni Shofarul , Guo Keying , Silva Raphaela , Salvigni Luca , Hama Adel , Diaz‐Galicia Escarlet , Moser Maximilian , Marks Adam , McCulloch Iain , Grünberg Raik , Arold Stefan T. , Inal Sahika 
Published: June 2022

AbstractConventional biosensors rely on the diffusion‐dominated transport of the target analyte to the sensor surface. Consequently, they require an incubation step that may take several hours to allow for the capture of analyte molecules by sensor biorecognition sites. This incubation step is a primary cause of long sample‐to‐result times. Here, alternating current electrothermal flow (ACET) is integrated in an organic electrochemical transistor (OECT)‐based sensor to accelerate the device operation. ACET is applied to the gate electrode functionalized with nanobody–SpyCatcher fusion proteins. Using the SARS‐CoV‐2 spike protein in human saliva as an example target, it is shown that ACET enables protein recognition within only 2 min of sample exposure, supporting its use in clinical practice. The ACET integrated sensor exhibits better selectivity, higher sensitivity, and lower limit of detection than the equivalent sensor with diffusion‐dominated operation. The performance of ACET integrated sensors is compared with two types of organic semiconductors in the channel and grounds for device‐to‐device variations are investigated. The results provide guidelines for the channel material choice in OECT‐based biochemical sensors, and demonstrate that ACET integration substantially decreases the detection speed while increasing the sensitivity and selectivity of transistor‐based sensors.
Mechano‐Sensor for Proprioception Inspired by Ultrasensitive Slit‐Based Mechanosensilla
Authors: Wang Kejun , Zhang Lei , Gui Yuecheng , Fan Cheng , Sun Tao , Sun Lining , Wang Qian , Zhang Junqiu , Han Zhiwu 
Published: June 2022

AbstractInternal mechanosensors, as the core component of a proprioceptive system, provide vital mechanical information from intelligent devices for adaptive motor control, mechanical fault diagnosis, and machining condition monitoring. However, developing a sophisticated mechanosensory structure that can be widely used is highly desirable to significantly improve the detection performance of internal mechanosensors. Coincidentally, in nature, optimized microscale slits of arachnids (e.g., scorpions and spiders) are ingeniously used as a mechanosensory structure for internal mechanosensilla to efficiently detect the inevitable internal mechanical feedbacks caused by self‐motion and external mechanical stimuli. Biological slit‐based mechano‐sensilla provide an attractive bio‐inspired strategy to use the controllable slit as the sensory structure to improve the perceptual performance of internal mechanosensors. In this study, the structure‐deformation‐performance coupling relationship of slit‐based mechano‐sensilla is explored through experiment and theoretical analysis. An artificial slit‐based mechanosensor is developed by mimicking the combined deformation properties of the slit and the ultrathin cuticular membrane covering the slit tail. This bio‐inspired mechanosensor shows excellent performance in terms of mechanical stability, response time, and sensitivity to mechanical signals. The research on a practical application highlights the importance of the unique basic “design” principles of the slit‐based mechano‐sensilla in improving the proprioceptive capability of smart engineering devices.
Humidity Resistant Carbon Nanotubes‐Styrene Methyl‐Methacrylate Polymer Composite for Ultrafast Laser
Authors: Bao Yunliang , Dai Lilong , Jiang Junjie , Huang Zinan , Huang Qianqian , Rozhin Aleksey , Mou Chengbo 
Published: June 2022

AbstractCarbon nanotube (CNT)–polymer composite films are key elements in widespread photonic and optoelectronic applications. One particular successful application is to produce ultrashort optical pulses in the laser cavity. Nevertheless, such composite film may suffer from severe humidity/water degradation, from which the laser may even stop generating regular pulses. Here, surfactant‐free CNT–styrene methyl‐methacrylate polymer composite film is fabricated. Based on such film‐type saturable absorber, a self‐starting passively mode‐locked erbium‐doped fiber laser with the capability of generating≈1 ps pulses is demonstrated. From the perspective of experimental measurements and numerical simulations, the effectiveness of a saturable absorber in generating ultrashort pulses is confirmed. The operating composite film can survive under fully immersed water condition for 30 days. More importantly, after the non‐operating composite film has been fully soaked in the water tank for 2 days, it can still mode‐lock the laser as it is in dry air condition, confirming the humidity resistance capability. In addition, it is experimentally found that the mechanical packaging of the composite film has an impact on the survival time of composite film under water immersion.
Transition‐Metal‐Free Regioselective Direct C2, C4 Difunctionalization and C2, C4, C6 Trifunctionalization of Pyridines
Authors: Wang Dong , Xu Liqing , Zheng Shixin , Yang Xiaolong 
Published: June 2022

AbstractThis study reports the invention of di‐ or trifunctionalization of readily available pyridines (including all the pyridine substrates utilized in this paper, such as 3‐cyanopyridine and 3‐chloropyridine) through dearomative functionalization‐oxidative rearomatization under transition‐metal‐ and reductant‐free conditions. Although a two‐step operation is required, the crude product of the first step could be used in the next step directly. Typically, 3‐π‐EWG pyridines undergo difunctionalization, whereas 3‐σ‐EWG pyridines participate in trifunctionalization, affording multisubstituted piperidines. Computational studies provide detailed insights for their distinct reactivity in the title reaction.magnified image
Palladium‐Catalyzed Domino Cyclization/Direct Aminosulfonylation Between Aryl Iodides and Amines via the Insertion of Sulfur Dioxide
Authors: Lv Haiping , He Xiaochun , Shen Lin , Zhang Xuemei , Lian Zhong 
Published: June 2022

AbstractA palladium‐catalyzed domino cyclization/direct aminosulfonylation of aryl iodides with amines via the insertion of SO2 (from SOgen) was presented. This method could produce a series of oxindole‐based sulfonamides in moderate‐to‐good yields. A scale‐up reaction and two synthetic applications demonstrated the robustness and practicality of this transformation.magnified image
Artificial Synapse Based on Bio‐Hierarchical Porous Memristor Driven by Multilevel‐Ions Migration
Authors: Zhang Jingjing , Ji Yuhang , Gao Qin , Gao Juan , Geng Xueli , Li Haoze , Shi Hongliang , Wang Mei , Xiao Zhisong , Chu Paul K. , Huang Anping 
Published: June 2022

AbstractArtificial synapse with memristive characteristics has immense potential for neuromorphic computing due to their non‐volatile, adjustable conductance, and high integration. Herein, an artificial synapse based on the bio‐inspired hierarchical porous structure is demonstrated, which is composed of mixed‐dimensional porous MoS2 nanosheets (NS) and porous SiOx. The device produces analog memristive characteristics with a high on‐off ratio of 106 and a long retention time of 105 s. Diversity of synaptic plasticity is achieved, such as paired‐pulse facilitation, spike‐timing‐dependent plasticity, multilevel long‐term memory, and associative learning functions. Inspired by the hierarchical migration and storage of electrolyte ions in the natural bamboo membrane, the memristive mechanism is proposed. The systematical analysis of Raman scattering and conductive mechanism reveals multilevel‐ions dynamic in hierarchical porous structure, which results in multistep formation and maintenance of conductive paths for Li‐ions. The bio‐inspired synaptic device with multifunctional synaptic characteristics is expected to play an important role in the future applications of neuromorphic computing and artificial intelligence.
Industrial‐Level CO2Electroreduction Using Solid‐Electrolyte Devices Enabled by High‐Loading Nickel Atomic Site Catalysts
Authors: Wang Shuguang , Qian Zhengyi , Huang Qizheng , Tan Yingjun , Lv Fan , Zeng Lingyou , Shang Changshuai , Wang Kai , Wang Guoqing , Mao Yandong , Wang Yan , Zhang Qinghua , Gu Lin , Guo Shaojun 
Published: June 2022

AbstractTransition‐metal atomic site catalysts (ASCs) are a new class of catalytic system for CO2electroreduction, however, their practical application is greatly hindered by the challenge that it's still difficult for them to simultaneously achieve industrial‐level current density and high selectivity. Herein a new strategy is reported for hundreds of gram‐scale and low‐cost production of Ni‐ASCs on 3D porous nanocarbon with high‐loading NiN3sites for greatly boosting the electroreduction of CO2to CO with both industrial‐level current density and high selectivity. It is discovered that although Ni‐ASCs with high‐loading (Ni‐ASCs/4.3 wt.%) and low‐loading (Ni‐ASCs/0.8 wt.%) both show above 95% Faradic efficiency for CO (FECO) under a wide potential range in H‐cell, in flow cell, Ni‐ASCs/0.8 wt.% can only achieve FECOof 43.6% at a current density of 343.9 mA cm−2, significantly lower than those (95.1%, 533.3 mA cm−2) of Ni‐ASCs/4.3 wt.% under same potential, first revealing the important role of high‐loadings of single atom sites in promoting the high‐selectivity electrolysis at industrial‐level current density. Most importantly, it is demonstrated that Ni‐ASCs/4.3 wt.%‐based membrane electrode assembly (MEA) exhibits outstanding durability at industrial‐level current density of 360.0 mA cm−2, which is one of the best performances for the realistic electroreduction of CO2to CO in the reported ASCs‐based MEA systems.
Revealing the Transient Formation Dynamics and Optoelectronic Properties of 2D Ruddlesden‐Popper Phases on 3D Perovskites
Authors: Kodalle Tim , Moral Raphael F. , Scalon Lucas , Szostak Rodrigo , Abdelsamie Maged , Marchezi Paulo E. , Nogueira Ana F. , Sutter‐Fella Carolin M. 
Published: June 2022

AbstractUsing in situ photoluminescence measurements during the spin‐coating and annealing steps, this study probes the formation of 2D layers on 3D triple cation perovskite films comparing phenylethylammonium and 2‐thiophenemethylammonium iodide bulky cations. This study elucidates the formation mechanisms of the surface layers for both cases and reveals two regimes during 2D layer formation: a kinetic‐driven and a thermodynamic‐driven process. These driving forces result in different compositions of the 2D/3D interface for each treatment, namely, different ratios of pure 2D (n = 1) and quasi‐2D (n > 1) structures. This study shows that a higher ratio of quasi‐2D phases is more beneficial for device performance, as pure‐2D layers may hamper current extraction. Due to a more evenly distributed formation energy profile among 2D and quasi‐2D phases, highly concentrated 2‐thiophenemethylammonium iodide appears to be more suited for effective surface passivation than its phenylethylammonium analog.
A consecutive‐competitive reaction system for assessing homogeneous and heterogeneous liquid–liquid mixing efficiency
Authors: Zhang Yi‐Dong , Wang Ze‐Xin , Zhang Liang‐Liang , Sun Bao‐Chang , Chu Guang‐Wen , Chen Jian‐Feng 
Published: June 2022

AbstractHere, the consecutive‐competitive reaction system about aspirin and sodium hydroxide was proposed as a unified chemical probe to characterize the homogenous and heterogeneous liquid–liquid mixing. The kinetics of the reaction system was clearly studied. Then the mixing efficiencies were assessed in a standard stirred tank with this chemical probe and the obtained segregation index (XS) could well characterize the mixing performance. Based on the incorporation model, the estimation formula of micromixing time was established as . The chemical probe could show the influence of stirring intensity, interphase resistance, and two‐phase ratio on the mixing efficiency sensitively when it was extended to heterogeneous mixing. Using this chemical probe, we found the mixing efficiencies of homogeneous and heterogeneous process tended to be the same at sufficiently high stirring intensity. The reason for this phenomenon was unveiled by investigating the dispersed phase size and calculating mass transfer time.
Bio‐inspirierte Ti3C2Tx MXene‐basierte Ionen‐Diodenmembran Für die Hocheffiziente Wandlung Osmotischer in Elektrische Energie
Authors: Ding Li , Zheng Mengting , Xiao Dan , Zhao Zihao , Xue Jian , Zhang Shanqing , Caro Jürgen , Wang Haihui 
Published: June 2022

AbstractBio‐inspirierte asymmetrische nanofluidische Ionenkanäle mit ionischem Diodenverhalten sind Forschungsziel, weil sie die effektive Umwandlung osmotischer Energie (sogenannte “blaue Energie”) in Elektrizität erlauben, insbesondere, wenn sie die Möglichkeit einer weiteren Oberflächenmodifizierung bieten. Zweidimensionale (2D) Metallcarbide und ‐nitride, bekannt als MXene, kombinieren hydrophile Oberflächen mit einstellbaren Oberflächenladungseigenschaften und bieten einen kurzschrittigen Weg zur Herstellung asymmetrischer nanofluidischer Ionenkanäle. Hier berichten wir über eine mechanisch robuste, flexible und scale up‐freundliche asymmetrische Ionen‐Diodenmembran auf Ti3C2Tx‐MXene‐Basis mit einem hochgradig gleichgerichteten Ionenstrom und demonstrieren ihre potenzielle Verwendung in der Wandlung osmotischer in elektrische Energie durch Umkehrelektrodialyse. Unter dem Salzkonzentrationsgradienten von synthetischem Meerwasser und Flusswasser beträgt die Leistungsdichte unseres Ionendioden‐Membran‐basierten Generators 8.6 W m−2 und bis zu 17.8 W m−2 bei einem 500‐fachen Salzgradienten und übertrifft damit den Stand der Technik. Das Design einer ionischen Membran vom Diodentyp auf MXene‐Basis bietet eine einfache und allgemeine Strategie für die Entwicklung von großflächigen 2D‐nanofluiden Systemen mit selektivem unidirektionalem Ionentransport.
Alcohols as Alkylating Agents in the Cation‐Induced Formation of Nitrogen Heterocycles
Authors: Cox Lydia , Zhu Yuxiang , Smith Philip J. , Christensen Kirsten E. , Sidera Portela Mireia , Donohoe Timothy J. 
Published: June 2022

AbstractA Ti(Oi‐Pr)4 promoted 5‐ or 6‐endo‐trig cyclisation to make nitrogen heterocycles is presented. The utilisation of HFIP as a key solvent enables the stereoselective preparation of di‐ & tri‐substituted pyrrolidines and piperidines while forming a new C−C bond at the same time. The process is triggered by a cationic intermediate generated from an allylic or benzylic alcohol and leads to the simultaneous generation of both a C−C and a C−N bond in a single step. Notably, either 2,3‐trans‐ or 2,3‐cis‐substituted heterocycles can be obtained by using a nucleophilic amine bearing different substituents. Lastly, the stereoselective synthesis of enantiopure products was achieved by using readily available enantiopure acyclic starting materials.
Zirconium‐oxo Nodes of MOFs with Tunable Electronic Properties Provide Effective ⋅OH Species for Enhanced Methane Hydroxylation
Authors: Fang Geqian , Hu Jin‐Nian , Tian Ling‐Chan , Liang Jin‐Xia , Lin Jian , Li Lin , Zhu Chun , Wang Xiaodong 
Published: June 2022

AbstractDirect conversion of methane to high value‐added oxygenates under mild conditions has attracted extensive interest. However, the over‐oxidation of target products is usually unavoidable due to the easily excessive activation of C−H bond on the sites of supported metal species. Here, we identified the most efficient Zr‐oxo nodes of UiO‐66 metal‐organic frameworks (MOFs) catalysts for the selective oxidation of methane with H2O2. These nodes were modified by three types of benzene 1, 4‐dicarboxylates (NH2‐BDC, H2BDC, and NO2‐BDC). Detailed characterizations and DFT calculations revealed that these ligands can effectively tune the electronic properties of Zr‐oxo nodes and the H2BDC ligand led to optimal electronic density of Zr‐oxo nodes in UiO‐66. Thus the UiO‐66‐H catalyst promoted the formation of ⋅OH species that adsorbed on Zr‐oxo nodes, and facilitated the activation of methane with a lower energy barrier and subsequent conversion to hydroxylation oxygenates with 100 % selectivity.
Bioinspired Ti3C2TxMXene‐Based Ionic Diode Membrane for High‐Efficient Osmotic Energy Conversion
Authors: Ding Li , Zheng Mengting , Xiao Dan , Zhao Zihao , Xue Jian , Zhang Shanqing , Caro Jürgen , Wang Haihui 
Published: June 2022

AbstractBioinspired asymmetric nanofluidic ion channels with ionic diode behavior that can boost the osmotic energy (so‐called blue energy) conversion are highly desirable, especially if they can be easily constructed and modified. Two‐dimensional (2D) metal carbides and nitrides, known as MXenes, combine hydrophilic surfaces and tunable surface charge properties, providing a shortcut to prepare asymmetric nanofluidic ion channels. Here, we report a mechanically robust, flexible, and scale‐up‐friendly asymmetric Ti3C2TxMXene‐based ionic diode membrane with a highly rectified current and demonstrate its potential use in reverse electrodialysis osmotic energy conversion. Under the salinity gradient of synthetic seawater and river water, our ionic diode membrane‐based generator‘s power density is 8.6 W m−2and up to 17.8 W m−2at a 500‐fold salinity gradient, outperforming the state‐of‐the‐art membranes. The design of MXene‐based ionic diode‐type membrane provides a facile and general strategy in developing large‐scale 2D nanofluidics and selective ion transport.
Hexagonal Planar [B6H6] within a [B6H12] Borate Complex: Structure and Bonding of [(Cp*Ti)2(μ‐ɳ6 : ɳ6‐B6H6)(μ‐H)6]
Authors: Kar Sourav , Bairagi Subhash , Haridas Anagha , Joshi Gaurav , Jemmis Eluvathingal D. , Ghosh Sundargopal 
Published: June 2022

AbstractIsolation of planar [B6H6] is a long‐awaited goal in boron chemistry. Several attempts in the past to stabilize [B6H6] were unsuccessful due to the domination of polyhedral geometries. Herein, we report the synthesis of a triple‐decker sandwich complex of titanium [(Cp*Ti)2(μ‐η6 : η6‐B6H6)(μ‐H)6] (1), which features the first‐ever experimentally achieved nearly planar six‐membered [B6H6] ring, albeit within a [B6H12] borate. The small deviation from planarity is a direct consequence of the predicted structural pattern of the middle ring in 24 Valence Electron Count (VEC) triple‐decker complexes. The large ring size of [B6H6] in 1 brings the metal–metal distance into the bonding range. However, significant electron delocalization from the M−M bonding orbital to the bridging hydrogen and B−B skeleton in the middle decreases its bond strength.
Silicate composition of sungrazing comet C/1965 S1 (Ikeya‐Seki)
Authors: Petrov Dmitry V. , Zhuzhulina Elena A. 
Published: June 2022

AbstractThe sungrazing comets, that pass extremely close to the Sun, are rare, but are of considerable scientific interest due to their unusual polarimetric properties. This paper is devoted to the interpretation of polarimetric observational data from comet Ikeya‐Seki (C/1965 S1), also known as the “Big Comet of 1965.” The data of polarimetric observations of this comet at a wavelength of 0.53 μm are sharply out of the general range of other observed comets in the wavelength range of 0.52–0.55 μm. The phase curve of comet Ikeya‐Seki, unlike all other comets, has an incredibly steep slope, the exact explanation of which has not been given so far. In this work, we reproduce this slope using computer simulation. It was shown that irregularly shaped particles under no parameters can give such a sharp slope in the degree of linear polarization. However, the use of spherical particles is able to reproduce this slope quite accurately. The best fit is achieved using Fe‐rich silicate (fayalite) particles with a radius of ≈0.633 μm. Therefore, when studying near‐solar comets, it is necessary to consider the effect on the scattering pattern of regular shape particles as well as the presence of Fe‐rich silicate (fayalite) material.
BIM‐Pilotprojekte Huntebrücke und Grawiedebrücke – Erfahrungen mit dem Werkzeug BIM in der Entwurfsplanung
Authors: von der Haar Christoph , Gudat Alexander , Thiele Dietmar , Göhlmann Joachim 
Published: June 2022

AbstractDie Entwurfsplanungen für die Ersatzneubauten der Huntebrücke und der Grawiedebrücke wurden von der Niedersächsischen Landesbehörde für Straßenbau und Verkehr (NLStBV) als BIM‐Pilotprojekte ausgewählt. Während die Grawiedebrücke mit einer Gesamtstützweite von 9 m eine Landstraße über die Grawiede überführt, überführt die Huntebrücke mit einer Gesamtstützweite von 441 m die Autobahn 29 östlich von Oldenburg über die Seeschifffahrtsstraße Hunte. Diese beiden sehr gegensätzlichen Bauwerke werden im Rahmen des folgenden Beitrags vorgestellt und die Erfahrungen seitens der Entwurfsverfasser mit dem Werkzeug BIM geschildert. Beide Ersatzneubauten wurden dreidimensional modelliert, die Bauabläufe mit den Modellen verknüpft und anschließend die Mengenermittlungen und Kostenberechnungen anhand der Modelle durchgeführt. Damit entsprach die Modellierungstiefe einer vollständigen 5D‐BIM‐Simulation. Es werden die Vorteile und die Herausforderungen, die aus der Planung der Ersatzneubauten mit der Methode BIM resultierten, aufgezeigt.