bluuebunny/crossref_metadata_2025_split huggingface dataset:
Oxygen Vacancy‐Tailored Schottky Heterojunction Activates Interface Dipole Amplification and Carrier Inversion for High‐Performance Potassium‐Ion Batteries
Authors: Hsieh Yi‐Yen , Tuan Hsing‐Yu 
Published: August 2023

AbstractAn oxygen vacancy‐tailored Schottky heterostructure composed of polyvinylpyrrolidone‐assisted Bi2Sn2O7 (PVPBSO) nanocrystals and moderate work function graphene (mWFG, WF = 4.36 eV) is designed, which in turn intensifies the built‐in voltage and interface dipole across the space charge region (SCR), leading to the inversion of majority carriers for facilitating K+ transport/diffusion behaviors. Thorough band‐alignment experiments and interface simulations reveal the dynamics between deficient BSO and mWFG, and how charge redistribution within the SCR leads to carrier inversion, demonstrating the impact of different defect engineering degrees on the amplification of Schottky junctions. The ordered transport of bipolar carriers can boost electrons and K ions easily passing through the inner and outer surfaces of the heterostructure. With high activity and low resistance in electrochemical reactions, the PVPBSO/mWFG exhibits an attractive capacity of 430 mA h g−1 and a rate capability exceeding 2000 mA g−1, accompanied by minimal polarization and efficient utilization of conversion‐alloying reactions. The substantial cell capacity and high‐redox plateau of PVPBSO/mWFG//PB contribute to the practical feasibility of high‐energy full batteries, offering long‐cycle retention and high‐voltage output. This study emphasizes the direct importance of interface and junction engineering in improving the efficiency of diverse electrochemical kinetic and diffusion processes for potassium‐ion batteries.
Homogeneous Bridging Induces Compact and Scalable Perovskite Thick Films for X‐Ray Flat‐Panel Detectors
Authors: Chai Yingjun , Jiang Chaoyan , Hu Xudong , Han Jiguang , Wang Yao , Yang Wanqiu , Li Chongkang , Zeng Haibo , Li Xiaoming 
Published: August 2023

AbstractSolution‐processed organic–inorganic hybrid perovskite polycrystalline thick films have shown great potential in X‐ray detection. However, the preparation of compact perovskite thick films with large area is still challenging due to the limitation of feasible ink formulation and pinholes caused by solvent volatilization. Post‐treatment and hot‐pressing are usually involved to improve the film quality, which is however unsuitable for subsequent integration. In this work, a homogeneous bridging strategy is developed to prepare compact perovskite films directly. A stable perovskite slurry with suitable viscosity consisting of undissolved grains and supersaturated solution is formed by adding a weak coordination solvent to the pre‐synthesized microcrystalline powders. Small perovskite grains in situ grow from the saturated solution during the annealing, filling the pinholes and connecting the surrounding original grains. As a result, large‐area perovskite thick film with tight grain arrangement and ultralow current drift is blade‐coated to achieve X‐ray imaging. The optimal device displays an impressive mobility‐lifetime product of 2.2 × 10−3 cm2 V−1 and a champion ratio of sensitivity to the dark current density of 2.23 × 1011 µC Gyair−1 A−1. This work provides a simple and effective route to prepare high‐quality perovskite thick films, which is instructive for the development of perovskite‐based X‐ray flat‐panel detectors.
Boron‐Doped Nickel–Nitrogen–Carbon Single‐Atom Catalyst for Boosting Electrochemical CO2 Reduction
Authors: Song Jian , Lei Xue , Mu Jiali , Li Jingwei , Song Xiangen , Yan Li , Ding Yunjie 
Published: August 2023

AbstractTuning the coordination environment of the metal center in metal–nitrogen–carbon (M–N–C) single‐atom catalysts via heteroatom‐doping (oxygen, phosphorus, sulfur, etc.) is effective for promoting electrocatalytic CO2 reduction reaction (CO2RR). However, few studies are investigated establishing efficient CO2 reduction by introducing boron (B) atoms to regulate the M–N–C structure. Herein, a B‐C3N4 self‐sacrifice strategy is developed to synthesize B, N co‐coordinated Ni single atom catalyst (Ni‐BNC). X‐ray absorption spectroscopy and high‐angle annular dark field scanning transmission electron microscopy confirm the structure (Ni‐N3B/C). The Ni‐BNC catalyst presents a maximum CO Faradaic efficiency (FECO) of 98.8% and a large CO current density (jCO) of −62.9 mA cm−2 at −0.75 and −1.05 V versus reversible hydrogen electrode, respectively. Furthermore, FECO could be maintained above 95% in a wide range of potential windows from −0.65 to −1.05 V. In situ experiments and density functional theory calculations demonstrate the Ni‐BNC catalyst with B atoms coordinated to the central Ni atoms could significantly reduce the energy barrier for the conversion of *CO2 to *COOH, leading to excellent CO2RR performance.
Deciphering the Mechanism of Crystallization of UiO‐66 Metal‐Organic Framework
Authors: Semivrazhskaya Olesya O. , Salionov Daniil , Clark Adam H. , Casati Nicola P. M. , Nachtegaal Maarten , Ranocchiari Marco , Bjelić Saša , Verel René , van Bokhoven Jeroen A. , Sushkevich Vitaly L. 
Published: August 2023

AbstractZirconium‐containing metal‐organic framework (MOF) with UiO‐66 topology is an extremely versatile material, which finds applications beyond gas separation and catalysis. However, after more than 10 years after the first reports introducing this MOF, understanding of the molecular‐level mechanism of its nucleation and growth is still lacking. By means of in situ time‐resolved high‐resolution mass spectrometry, Zr K‐edge X‐ray absorption spectroscopy, magic‐angle spinning nuclear magnetic resonance spectroscopy, and X‐ray diffraction it is showed that the nucleation of UiO‐66 occurs via a solution‐mediated hydrolysis of zirconium chloroterephthalates, whose formation appears to be autocatalytic. Zirconium‐oxo nodes form directly and rapidly during the synthesis, the formation of pre‐formed clusters and stable non‐stoichiometric intermediates are not observed. The nuclei of UiO‐66 possess identical to the crystals local environment, however, they lack long‐range order, which is gained during the crystallization. Crystal growth is the rate‐determining step, while fast nucleation controls the formation of the small crystals of UiO‐66 with a narrow size distribution of about 200 nanometers.
PDI‐Based Organic Small Molecule Regulated by Inter/Intramolecular Interactions for Efficient Solar Vapor Generation
Authors: Shao Changxiang , Guo Bingpeng , Lu Bing , Yu Jiahui , Kong Huijun , Wang Baolei , Ding Meichun , Li Chenwei 
Published: August 2023

AbstractOrganic small molecules with processing feasibility, structural diversity, and fine‐tuned properties have the potential applications in solar vapor generation. However, the common defects of narrow solar absorption, low photothermal conversion efficiency, and photobleaching result in limited materials available and unsatisfactory evaporation performance. Herein, the perylene diimide (PDI) derivatives are exploited as stable sunlight absorbers for solar vapor generation. Particularly, the N,N'‐bis(3,4,5‐trimethoxyphenyl)−3,4,9,10‐perylenetetracarboxylic diimide (PDI‐DTMA) is well‐designed with donor–acceptor–donor configuration based on plane rigid PDI core. The efficient photothermal conversion is enabled through strong intermolecular π–π stacking and intramolecular charge transfer, as revealed by experimental demonstration and theoretical calculation. The PDI‐DTMA with a narrow band gap of 1.17 eV exhibits expanded absorption spectrum and enhanced nonradiative transition capability. The 3D hybrid hydrogels (PPHs) combining PDI‐DTMA and polyvinyl alcohol are constructed. With the synergistic effect of solar‐to‐heat conversion, thermal localization management, water activation, and unobstructed water transmission of PPHs, the high water evaporation rates can reach 3.61–10.07 kg m−2 h−1 under one sun. The hydrogels also possess great potential in seawater desalination and sewage treatment. Overall, this work provides valuable insights into the design of photothermal organic small molecules and demonstrates their potentials in solar water evaporation.
Asymmetric Dehydrative Allylation Using Soft Ruthenium and Hard Brønsted Acid Combined Catalyst
Authors: Tanaka Shinji , Kitamura Masato 
Published: August 2023

AbstractAsymmetric Pd‐catalyzed Tsuji‐Trost‐type allylation is an important catalytic reaction toward chiral natural and unnatural product syntheses. We successfully modified a desalt‐type reaction using allyl ester or halide to a dehydrative one using allylic alcohol via the establishment of two redox‐mediated donor acceptor bifunctional catalyst systems. These systems were cationic CpRu‐Cl‐Napy‐PyCOOH and cationic CpRu‐Naph‐diPIM‐dioxo‐iPr/p‐TsOH and were designed on the basis of the soft ruthenium and hard Brønsted acid combined catalyst concept. The complementary use of the two chiral catalysts for dehydrative asymmetric allylation expands the application scope facilitating the utilization of both aliphatic and aromatic allylic alcohols with various nucleophiles in the substrate. In this account, the design, synthesis, and application of these catalysts were reported.
Applications of Carbon‐Based Materials in Activated Peroxymonosulfate for the Degradation of Organic Pollutants: A Review
Authors: Hao Liangyun , Zhang Junkai , Liu Jia , Min Yuting , Chen Chunguang 
Published: August 2023

AbstractIn recent years, water pollution has posed a serious threat to aquatic organisms and humans. Advanced oxidation processes (AOPs) based on activated peroxymonosulfate (PMS) show high oxidation, good selectivity, wide pH range and no secondary pollution in the removal of organic pollutants in water. Carbon‐based materials are emerging green catalysts that can effectively activate persulfates to generate radical and non‐radical active species to degrade organic pollutants. Compared with transition metal catalysts, carbon‐based materials are widely used in SR‐AOPs because of their low cost, non‐toxicity, acid and alkali resistance, large specific surface area, and scalable surface charge, which can be used for selective control of specific water pollutants. This paper mainly presents several carbon‐based materials used to activate PMS, including raw carbon materials and modified carbon materials (heteroatom‐doped and metal‐doped), analyzes and summarizes the mechanism of activating PMS by carbon‐based catalysts, and discusses the influencing factors (temperature, pH, PMS concentration, catalyst concentration, inorganic anions, inorganic cations and dissolved oxygen) in the activation process. Finally, the future challenges and prospects of carbon‐based materials in water pollution control are also presented.
Entropy generation analysis of CNT‐based nanofluid flows induced by a moving plate
Authors: Sarfraz Mahnoor , Khan Masood 
Published: August 2023

AbstractCarbon nanotubes have garnered considerable interest from academia and industry due to their unique properties and potential applications. This study examines fluid flow induced by a plate moving at a constant velocity towards/receding from normal stagnation point flow. The plate's surface is immersed with ethylene glycol and two types of carbon nanotubes: single‐walled and multi‐walled. The Reynolds number, proportional to the plate's velocity, governs the flow. Thermal transport analysis includes Ohmic heating, heat source/sink effects for constant wall temperature and prescribed surface temperature, and entropy generation analysis. Similarity ansatz is used to obtain non‐dimensional ordinary differential equations, and numerical and asymptotic solutions are computed using MATLAB's bvp4c routine (finite difference‐based approach). By varying the relevant parameters, the study interprets the behavior of entropy generation, Bejan number, skin frictions, Nusselt number, flow, and energy profiles. The numerical solutions are observed to match their asymptotic behaviors within an intermediate range of small and large Reynolds numbers for the wall stress parameter. The magnetic parameter produces a resistive force that reduces fluid flow but enhances the system's energy. Moreover, understanding the flow and heat transfer characteristics of CNT‐based nanofluids induced by a moving plate can provide insights into the design and optimization of thermal systems, including efficient heat exchangers used in power generation, chemical, and petrochemical industries.
Cell-Free Synthesis and Electrophysiological Analysis of Multipass Voltage-Gated Ion Channels Tethered in Microsomal Membranes
Authors: Pandey Yogesh , Dondapati Srujan Kumar , Wüstenhagen Doreen , Kubick Stefan 
Published: August 2023

AbstractCell-free protein synthesis (CFPS) has emerged as a powerful tool for the rapid synthesis and analysis of various structurally and functionally distinct proteins. These include ‘difficult-to-express’ membrane proteins such as large multipass ion channel receptors. Owing to their membrane localization, eukaryotic CFPS supplemented with endoplasmic reticulum (ER)-derived microsomal vesicles has proven to be an efficient system for the synthesis of functional membrane proteins. Here we demonstrate the applicability of the eukaryotic cell-free systems based on lysates from the mammalian Chinese Hamster Ovary (CHO) and insect Spodoptera frugiperda (Sf21) cells. We demonstrate the efficiency of the systems in the de novo cell-free synthesis of the human cardiac ion channels: ether-a-go-go potassium channel (hERG) KV11.1 and the voltage-gated sodium channel hNaV1.5.
Graphical Abstract
Characterization of Peptide-Based Nanomaterials
Authors: Edwards-Gayle Charlotte J. C. , Wychowaniec Jacek K. 
Published: August 2023

AbstractIn this chapter, we will thoroughly discuss characterization techniques used to elucidate the exact structure and define properties of peptide-based nanomaterials. In particular we divide methods into:Quality control performance (mass spectroscopy and high-performance liquid chromatography.Spectroscopy (Fourier transform infrared spectroscopy, Raman spectroscopy, circular and linear dichroism, nuclear magnetic resonance and fluorescence spectroscopy).Microscopy (scanning and transmission electron microscopies, atomic force microscopy, optical and polarized light microscopy).Scattering (small angle X-ray and neutron scattering, X-ray diffraction).Bulk structures (mainly hydrogels) rheological characterization.The methodology is described for molecular structures, self-assembled nanostructures and aggregates, as well as hybrid, composite and/or conjugated nanomaterials and their bulk forms. Both common, as well as more exotic versions of all methods are presented in the context of peptide-based nanomaterials. Where utilized, examples of combinatorial use of techniques are demonstrated. Representative studies accompany the discussion and usefulness of all presented methods.
Truth machines: synthesizing veracity in AI language models
Authors: Munn Luke , Magee Liam , Arora Vanicka 
Published: August 2023

AbstractAs AI technologies are rolled out into healthcare, academia, human resources, law, and a multitude of other domains, they become de-facto arbiters of truth. But truth is highly contested, with many different definitions and approaches. This article discusses the struggle for truth in AI systems and the general responses to date. It then investigates the production of truth in InstructGPT, a large language model, highlighting how data harvesting, model architectures, and social feedback mechanisms weave together disparate understandings of veracity. It conceptualizes this performance as an operationalization of truth, where distinct, often-conflicting claims are smoothly synthesized and confidently presented into truth-statements. We argue that these same logics and inconsistencies play out in Instruct’s successor, ChatGPT, reiterating truth as a non-trivial problem. We suggest that enriching sociality and thickening “reality” are two promising vectors for enhancing the truth-evaluating capacities of future language models. We conclude, however, by stepping back to consider AI truth-telling as a social practice: what kind of “truth” do we as listeners desire?
Femoral nerve block using lower concentration ropivacaine preserves quadriceps strength while providing similar analgesic effects after knee arthroscopy
Authors: Zhang Tao , Zhang Tingting , Niu Xiaoyin , Li Lantao , Gu Jiaji , Chen Minghui , Zhao Xuan 
Published: August 2023

AbstractPurposeFemoral nerve block (FNB) is widely used in patients undergoing knee arthroscopy. However, the most commonly used concentration of ropivacaine (0.2% or above) may cause an unexpected decrease in the muscle strength of the quadriceps. Therefore, a lower concentration of ropivacaine (0.1%) for FNB was administered to investigate the effect on quadriceps strength and postoperative pain after knee arthroscopy.MethodsThis was a double‐blind, randomized, controlled trial (ChiCTR2000041404). A total of 83 patients scheduled for elective knee arthroscopy were randomized to receive 0.1% or 0.2% ropivacaine for FNB under ultrasound guidance. The primary outcomes were quadriceps strength and numerical rating scale (NRS) pain score. Quadriceps strength was measured before surgery and 6 h and 24 h after surgery, while NRS score was recorded before surgery, at the postanaesthesia care unit (PACU), and 6 h and 24 h after surgery. Multiple linear regression tests were used to compare the differences in quadriceps strength and NRS score between the two groups. Two‐factor analysis of variance, using the factors group and time of measurement, was used for repeated NRS scores. Secondary outcomes included knee mobility, side effects, patient satisfaction, and length of hospital stay.ResultsThe mean (SD) quadriceps strength at 6 h after surgery was 7.5 (5.7) kg for the 0.1% ropivacaine group and 3.0 (4.4) kg for the 0.2% ropivacaine group. The mean difference adjusted for baseline characteristics was − 5.2 (95% CI − 7.2 to − 3.1) kg (P < 0.001). There was no significant difference between the two groups in quadriceps strength at 24 h after surgery. The mean differences in the average NRS score and maximum NRS score in the PACU were − 0.6 (P = 0.008) and − 1.0 (P < 0.001), respectively. There was no significant difference in NRS score at 6 h or 24 h after surgery. Two‐factor analysis of variance showed no significant difference in the interaction factors of time and group for average NRS score and maximum NRS score.ConclusionsCompared with 0.2% ropivacaine, 0.1% ropivacaine for FNB preserved quadriceps strength at 6 h after knee arthroscopy while providing similar analgesic effects.Level of evidenceI.
A novel germline hyperactivating JAK2 mutation L604F
Authors: Dvořáček Lukáš , Marková Jana , Holoubek Aleš , Grebeňová Dana , Kundrát David , Kuželová Kateřina , Schwarz Jiří 
Published: August 2023

AbstractSomatic JAK2 mutations are the main molecular cause of the vast majority of polycythemia vera (PV) cases. According to a recent structural model, the prevalent acquired V617F mutation improves the stability of the JAK2 dimer, thereby enhancing the constitutive JAK2 kinase activity. Germline JAK2 mutations usually do not largely alter JAK2 signaling, although they may modulate the impact of V617F. We found an unusual germline JAK2 mutation L604F in homozygous form in a young PV patient, along with a low allele burden JAK2 V617F mutation, and in her apparently healthy sister. Their father with a PV-like disease had L604F in a heterozygous state, without V617F. The functional consequences of JAK2 L604Fmutation were compared with those induced by V617F in two different in vitro model systems: (i) HEK293T cells were transfected with plasmids for exogenous JAK2-GFP expression, and (ii) endogenous JAK2 modifications were introduced into HeLa cells using CRISPR/Cas9. Both mutations significantly increased JAK2 constitutive activity in transfected HEK293T cells. In the second model, JAK2 modification resulted in reduced total JAK2 protein levels. An important difference was also detected: as described previously, the effect of V617F on JAK2 kinase activity was abrogated in the absence of the aromatic residue F595. In contrast, JAK2 hyperactivation by L604F was only partially inhibited by the F595 change to alanine. We propose that the L604F mutation increases the probability of spontaneous JAK2 dimer formation, which is physiologically mediated by F595. In addition, L604F may contribute to dimer stabilization similarly to V617F.
„Bad or Evil“ – vom Gassenjungen zum Präsidenten
Authors: Herpertz Stephan 
Published: August 2023

ZusammenfassungObschon Ende 2021 die Welt über Monate den russischen Aufmarsch an den Grenzen zu der Ukraine beobachten konnte, überraschte die am 24.02.2022 beginnende Invasion der Ukraine durch russische Truppen die meisten westlichen Beobachter. Mindestens ebenso überraschend zeigte sich die Stärke des ukrainischen Widerstands, die der russischen „Spezialoperation“ und dem Präsidenten der Russischen Föderation, Wladimir Putin, ein Desaster bescherte. Wer ist aber der Mann, dem es gelang, westliche Regierungen und die NATO bis zu dem Tag des Angriffs zu täuschen, der sich aber gleichzeitig so täuschen ließ. So mancher namhafte deutsche Politiker pflegte mit ihm viele Jahre enge Kontakte bis hin zu innigen Freundschaften und machte ihn zu dem wichtigsten Energielieferanten und dies trotz seiner Vernichtungskriege in Tschetschenien, Georgien, Syrien und im Donbass. Politiker fast aller Parteien in Europa haben sich nunmehr von ihm abgewandt. Für die meisten Menschen gilt er als das Böse schlechthin, und doch ist wenig über ihn bekannt. Die vorliegende Arbeit unternimmt nicht den Versuch einer Charakter- bzw. Persönlichkeitsstudie. Das Anliegen des Autors besteht vielmehr darin, zeitgeschichtliche und biografische Fäden zusammenzuführen, das Ende der Sowjetunion und des Kommunismus, die Transformation der ökonomischen Ordnung und der Werdegang Putins vom Gassenjungen in St. Petersburg zum Präsidenten der Russischen Föderation.
Motor performance and functional connectivity between the posterior cingulate cortex and supplementary motor cortex in bipolar and unipolar depression
Authors: Marten Lara E. , Singh Aditya , Muellen Anna M. , Noack Sören M. , Kozyrev Vladislav , Schweizer Renate , Goya-Maldonado Roberto 
Published: August 2023

AbstractAlthough implicated in unsuccessful treatment, psychomotor deficits and their neurobiological underpinnings in bipolar (BD) and unipolar (UD) depression remain poorly investigated. Here, we hypothesized that motor performance deficits in depressed patients would relate to basal functional coupling of the hand primary motor cortex (M1) and the posterior cingulate cortex (PCC) with the supplementary motor area (SMA). We performed a longitudinal, naturalistic study in BD, UD and matched healthy controls comprising of two resting-state functional MRI measurements five weeks apart and accompanying assessments of motor performance using a finger tapping task (FTT). A subject-specific seed-based analysis describing functional connectivity between PCC-SMA as well as M1-SMA was conducted. The basal relationships with motor performance were investigated using linear regression models and all measures were compared across groups. Performance in FTT was impaired in BD in comparison to HC in both sessions. Behavioral performance across groups correlated significantly with resting state functional coupling of PCC–SMA, but not of M1-SMA regions. This relationship was partially reflected in a reduced PCC–SMA connectivity in BD vs HC in the second session. Exploratory evaluation of large-scale networks coupling (SMN–DMN) exhibited no correlation to motor performance. Our results shed new light on the association between the degree of disruption in the SMA–PCC anticorrelation and the level of motor impairment in BD.