bluuebunny/crossref_metadata_2025 huggingface dataset:
Effects of Verbal Framing of Video and Attitudes Toward Police on Mock Jurors' Judgements of Body‐Worn Camera Video
Authors: Park Jaihyun , Feigenson Neal R. , Cheng Ngayin
Published: November 2024

This study examined the effects of prosecution and defense opening statements describing video evidence on mock jurors' perceptions and interpretations of that evidence and ultimate judgments. Materials were based on an actual case in which a police officer was tried for murder after fatally shooting an unarmed driver at a traffic stop. The incident was recorded on the officer's body‐worn camera. Participants exposed to the prosecution's verbal framing of the video judged the officer to be significantly more responsible for the driver's death than those not so exposed. Partisan verbal framing also significantly affected what participants reported having seen, in some instances making them more likely to agree with factual statements that were unambiguously false. The effect of verbal framing on participants' responsibility judgments was mediated by its effect on their inferential judgments and emotional responses. Attitudes toward police also significantly affected responsibility judgments, inferential judgments, and emotional responses.
A Time‐Saving Method for Evaluating the Fatigue Strength of Carburized High‐Alloy Steel Containing Carbides
Authors: Xu Zikuan , Gu Xuezhong , Liu Xiaolong , Chen Weihao , Wang Bin , Zhang Peng , Yang Maosheng , Chi Hongxiao , Zhang Zhefeng
Published: November 2024

To propose a time‐saving method for evaluating the fatigue strength of carburized steel, the fatigue behavior and fracture mechanism of carburized 14Cr14Co13Mo5 steels are studied by the rotary bending fatigue tests. It is found that the fatigue crack initiation site changes from surface to internal after carburizing due to the residual compressive stress and carbide cluster caused by the carburization. Besides, a notable correlation between the stress intensity of the cracked carbides at fatigue crack initiation site and fatigue life is observed in the carburized samples. This correlation allows for the estimation of fatigue strength at long conditional life based on samples tested at relatively high stress amplitudes with short lives, achieving a prediction error within 10% for the material studied. A significant time saving of ≈65% compared to the staircase method is achieved. The proposed method has significant implications for improving the efficiency fatigue strength evaluation in carburized steels containing carbides.
High‐Performance Ultrasensitive Flexible Piezoelectric Thin Film Sensors via a Cost‐Effective Transfer Strategy
Authors: Xu Qianqian , Jia Miao , Zhou Peiqiong , Zhang Yan , Guo Wei , Zhao Senfeng , Zeng Hanmin , Zhang Jianxun , Yan Mingyang , Jiang Shumiao , Zhou Kechao , Zhang Dou , Bowen Chris
Published: November 2024

Currently, reported physical or chemical methods to produce flexible perovskite thin films rely on the use of expensive single crystal substrates or large‐scale precision equipment. Here, a high‐performance ultrasensitive piezoelectric sensor via a cost‐effective strategy is developed to enable the release of lead zirconate titanate (PZT) thin films from an inexpensive mica substrate, which are subsequently transferred to a flexible polyethylene terephthalate substrate. The weak van der Waals interaction between the mica/La0.7Sr0.3MnO3 heterostructures minimizes mechanical clamping effects and provides favorable lattice and thermal matching conditions for the growth of high‐quality thin films. The transferred thin films exhibit significantly improved mechanical and functional properties, including an outstanding piezoelectric response (474.2 pm V−1) and an excellent mechanical flexibility, with a bending radius up to 1 mm. The sensor formed via the new transfer strategy exhibits a highly sensitive response to wide‐angle bending (110 mV degree−1) and small pressure changes (1.8 V kPa−1), and is successfully employed for real‐time breathing monitoring and wireless gesture recognition, thereby demonstrating its significant potential in applications related to flexible electronics.
Rectangular Carbon Nitrides C4N Monolayers with a Zigzag Buckled Structure: Quasi‐1D Dirac Nodal Lines and Weak Topological Properties with Flat Edge States
Authors: Li Linyang , Li Jialei , Song Yuxuan , Yu Yawei , Guan Lixiu , Liu Xiaobiao , Chen Xin , Liu Guodong , Peeters François M.
Published: November 2024

Using first‐principles calculations, two C4N monolayers with a zigzag buckled (ZB) structure are proposed. The ZB C4N monolayers contain raised‐C (raised‐N) atoms with sp3 hybridization, different from the traditional 2D graphene‐like carbon nitride materials with sp2 hybridization. Interestingly, the band structures of the ZB C4N monolayers exhibit quasi‐1D Dirac nodal line resulting from the corresponding quasi‐1D structure of the zigzag carbon chains, which is essentially different from the conventional ring‐shaped nodal line. The quasi‐1D Dirac nodal line exhibits the following features: i) gapless Dirac points, ii) varying Fermi velocity, and iii) a slightly curved band along the high‐symmetry path. All these features are successfully explained by the proposed tight‐binding model that includes interactions up to the third nearest neighbor. The Fermi velocity of the 2D system can reach 105 m s−1, which is promising for applications in high‐speed electronic devices. The topological flat band structure of the corresponding 1D system determined by the Zak phase and band inversion is edge‐dependent, which is a weak topological state and can be explained by the 2D Su‐Schrieffer‐Heeger (SSH) model. The quasi‐1D Dirac Fermions and SSH edge states make the ZB C4N monolayers promising for nanoelectronics applications.
Understanding and Passivation of Surface Corrosion of Cu for Stable Low‐N/P‐Ratio Lithium‐Sulfur Battery
Authors: Luo Yufeng , Zhang Chi , Cai Jiehua , Wei Zhenyao , Huang Qiyao , Zheng Zijian
Published: November 2024

The realization of a low negative/positive capacity (N/P) ratio is essential for attaining high energy density in lithium‐sulfur batteries (LSBs). However, it has been challenging to maintain the stability of the Li metal anode at low N/P ratios. Herein, it is revealed that the corrosion of the Cu current collector by dissolved intermediates of polysulfides ‐a largely overlooked perspective‐ significantly contributes to the instability of Li metal anode at low N/P ratios. The reduced Li/Li+ redox rates on the corroded Cu surface result in uneven and porous Li deposits that severely deteriorate cycling stability. To address this issue, an anti‐corrosion alloy coating is developed to passivate the Cu surface against polysulfides. LSBs with passivated current collectors at a low N/P ratio (1.5) and lean electrolyte (5 µL mgs
−1) show a ten fold extension in cycle and calendar life. This study not only provides the initial evidence of the impact of Cu corrosion on the failure mechanism of low N/P ratio LSBs but also proposes a practical yet effective strategy to stabilize high‐energy‐density LSBs.
Revolutionizing Micro‐Scale Energy Storage by 0D Carbon Nanostructures: Synthesis, Integration, Performance Optimization Mechanisms and Sustainable Applications
Authors: Nisa Fazal ul , Tahir Muhammad , Khalid Shehroz , Amin Naima , Yin Hongbo , Long Yihao , Tang Hui , Iiaz Kashif , Khan Arif Ullah , Naseem Mizna , Peng Zhen , Ma Zeyu , Wu Leixin , Uddin MD Faizan , Khan Abdul Jabbar , Qu Longbing , Ahmad Waheed , He Liang
Published: November 2024

The micro‐scale energy storage devices (MESDs) have experienced significant revolutions driven by developments in micro‐supercapacitors (MSCs) and micro‐batteries (MBs). This review summarizes the advancements of MSC and MB architecture, highlighting the electrode–electrolyte designs and the emergence of alkali metal ions aqueous batteries. The performance and synthesis of carbon quantum dots (CQDs), graphene quantum dots (GQDs), and their synergistic effects for energy storage applications are investigated. The focus is on integrating CQDs/GQDs into the MESDs for enhanced performance. The development of compositing CQD/GQD with other materials, reveals their capacitive and pseudocapacitive performance, extending the MESDs’ possibilities. Moreover, this review systematically covers various fabrication techniques from photolithography to printing techniques. The merits and practicality of each technique for fabricating MSCs and MBs are assessed. Electrochemical performance evaluation, capacitance enhancement, charge–discharge kinetics, and stability assessments are presented to demonstrate the efficiency of MESDs with practical applications. Despite significant progress, challenges remain, particularly in the scalability of fabrication and understanding long‐term stability. Nevertheless, the prospects are promising, with avenues in synthesis, fabrication, and electrochemical performance evaluation, which lead to a paradigm shift in MESDs. This review offers a broad perspective, combining innovations across diverse domains and directing the frontline of microelectronics.
Artificially Engineered Nanoprobes for Ultrasensitive Magnetic Resonance Imaging
Authors: Li Xuyan , Liu Qingshan , Wu Menglin , Wang Hao , Yang Jiang , Mu Xiaoyu , Zhang Xiao‐Dong
Published: November 2024

Magnetic resonance imaging (MRI) is a noninvasive and radiation‐free technique used for soft tissue. However, there are some limitations of the MRI modality, such as low sensitivity and poor image resolution. Artificially engineered magnetic nanoprobes have been extensively explored as a versatile platform for ultrasensitive MRI contrast agents due to their unique physiochemical characteristics and tunable magnetic properties. In this review, the emphasis is on recent progress in MRI nanoprobes with different structures and elements, including gadolinium‐, iron‐, manganese‐based and metal‐free nanoprobes. The key influencing factors and advanced engineering strategies for modulating the relaxation ratio of MRI nanoprobes are systematically condensed. Furthermore, the widespread and noninvasive visualization applications of MRI nanoprobes for real time monitoring of major organs and accurate disease diagnosing, such as cerebrovascular, ischemia, Alzheimer's disease, liver fibrosis, whole‐body tumors, inflammation, as well as multi‐mode imaging applications are summarized. Finally, the challenges and prospects for the future development of MRI nanoprobes are discussed, and promising strategies are specifically emphasized for improving biocompatibility, precisely engineering of optimal size, AI‐driven prediction and design, and multifunctional self‐assembly to enhance diagnostics. This review will provide new inspiration for artificial engineering and nanotechnology‐based molecular probes for medical diagnosis and therapy with ultrasensitive MRI.
Photothermal Nano‐Immunotherapy Against Methicillin‐Resistant Staphylococcus aureus (MRSA) Biofilm Infections
Authors: Xu Lei , Lu Baoliang , Xie Kai , Fan Wangyang , Fang Shiyuan , Zhu Junchen , Yang Jiazhao , Xu Bin
Published: November 2024

Methicillin‐resistant Staphylococcus aureus (MRSA) biofilm infections are a prevalent type of biofilm‐associated infection with a poor prognosis and antibiotic resistance. The senescence of immune cells in the immune microenvironment contributes to biofilm formation. In this study, Ti₃C₂ MXene‐PVA nanosheets loaded with metformin (Met@TiC) are developed for the treatment of MRSA biofilm infections. Nanosheets utilize near‐infrared light to induce photothermal effects and provide direct bactericidal activity against biofilm structures. Met, which is known for its anti‐inflammatory and anti‐senescence properties, modulates immune responses by revitalizing the function of senescent macrophages within the biofilm microenvironment, thereby enhancing their phagocytic and biofilm‐eradicating capabilities. The efficacy of this nanoplatform both in vitro and in an MRSA biofilm infection mouse model, demonstrating its potential as a photothermal nanoimmunotherapy for combating MRSA biofilm infections is validated. In summary, the Met@TiC nanoplatform offers a significant alternative to clinical solutions for MRSA biofilm infections.
Ultralow Dose Iron‐Copper Bimetallic Single‐Atom Nanozymes for Efficient Photothermal‐Chemodynamic Antibacterial and Wound Healing
Authors: Zhai Yujie , Pei Shenglin , Qin Xuhui , Zhang Lu , Liu Xijun , Cai Shuangqi , Zhang Weiqing
Published: November 2024

The combination of photothermal and chemodynamic therapy (PTT‐CDT) using single‐atom nanozymes (SAzymes) shows great promise in combating pathogenic and drug‐resistant bacteria. However, the photothermal conversion efficiency and catalytic activity of SAzymes with solely metal sites remain inadequate, often requiring high doses for effectiveness. Herein, a bimetallic single‐atomic nanozymes with Fe and Cu active sites (FeCu BSNs) designed is reported for efficient treatment of bacterial infections through hyperthermia‐amplified nanozyme catalysis strategy. The FeCu BSNs demonstrate remarkable peroxidase (POD) activity with a specific activity (SA) of 752.25 U mg−1, which is 2.3 folds larger than that of Fe SAzymes (323.45 U mg−1). Additionally, their photothermal effect achieve a photothermal conversion efficiency up to 56.26%, which is two times higher that of Fe SAzymes (29.69%) and Cu SAzymes (25.55%). These enhancements can be attributed to the hybridization of Fe and Cu sites. The FeCu BSNs‐mediated PTT‐CDT combination therapy demonstrates potent antibacterial effects in both in vitro and in vivo models, attributed to high levels of reactive oxygen species (ROS) generation and hyperthermia. This study effectively validates the application of ultralow‐dose bimetallic single‐atom nanozymes in PTT‐CDT for wound healing, offering a promising approach for enhanced wound recovery.
Ultrasensitive Detection of Chemokines in Clinical Samples with Graphene‐Based Field‐Effect Transistors
Authors: Kaiser David , Meyerbroeker Nikolaus , Purschke Werner , Sell Simone , Neumann Christof , Winter Andreas , Tang Zian , Hüger Daniel , Maasch Christian , Bethge Lucas , Weimann Thomas , Ferwerda Gerben , de Jonge Marien I. , Schnieders Albert , Vater Axel , Turchanin Andrey
Published: November 2024

Due to their ultra‐high sensitivity, solution‐gated graphene‐based field‐effect transistors (SG‐GFET) have been proposed for applications in bio‐sensing. However, challenges regarding the functionalization of GFETs have prevented their applications in clinical diagnostics so far. Here GFET sensors based on van der Waals (vdW) heterostructures of single‐layer graphene layered with a molecular ≈1 nm thick carbon nanomembrane (CNM) are presented. The CNM acts as an ultrathin molecular interposer between the graphene channel and the analyte and allows bio‐functionalization without impairing the graphene properties including its charge carrier mobility. To achieve specificity and reliability in the detection of biomarkers in real patient samples, the functionalization incorporates biostable aptamers in the non‐natural l‐configuration and hydrophilic polyethylene glycol for avoiding non‐specific adsorption. A rapid (≈5 min) detection of the clinically relevant inflammatory mediator CXCL8/IL‐8 within the concentration range of 0.5 – 500 pM (5 – 5000 pg ml−1) is demonstrated in nasal swab samples collected from patients with respiratory tract infections. This detection range may aid in diagnostics of early‐stage infectious diseases making the reported approach promising for the development of future medical tools.
The Future of Biohybrid Regenerative Bioelectronics
Authors: Carnicer‐Lombarte Alejandro , Malliaras George G. , Barone Damiano G.
Published: November 2024

Biohybrid regenerative bioelectronics are an emerging technology combining implantable devices with cell transplantation. Once implanted, biohybrid regenerative devices integrate with host tissue. The combination of transplant and device provides an avenue to both replace damaged or dysfunctional tissue, and monitor or control its function with high precision. While early challenges in the fusion of the biological and technological components limited development of biohybrid regenerative technologies, progress in the field has resulted in a rapidly increasing number of applications. In this perspective the great potential of this emerging technology for the delivery of therapy is discussed, including both recent research progress and potential new directions. Then the technology barriers are discussed that will need to be addressed to unlock the full potential of biohybrid regenerative devices.
Additively Manufactured Biodegradable Zn‐Based Porous Scaffolds to Suppress Osteosarcoma and Promote Osteogenesis
Authors: Lu Yupu , Liu Aobo , Jin Siqi , Dai Jiabao , Yu Yameng , Wen Peng , Zheng Yufeng , Xia Dandan
Published: November 2024

Postoperative therapies for osteosarcoma present substantial challenges due to tumor recurrence and extensive bone defects. To tackle these challenges, laser powder bed fusion is utilized to fabricate biodegradable Zn‐Li porous scaffolds that supress tumors and promote osteogenesis. After the structure design and composition selection, the Zn‐0.8Li porous scaffold with Gyroid unit optimally balances the co‐release of Zn2+ and Li+ during degradation, resulting in favorable antitumor and osteogenic effects. In vitro, the Zn‐0.8Li scaffold significantly inhibits osteosarcoma progression by suppressing tumor cell proliferation, promoting apoptosis, alleviating migration, and simultaneously promotes osteogenic differentiation through the enhanced expression of osteogenic markers. In vivo, the Zn‐0.8Li scaffold inhibits the malignant osteosarcoma behavior and facilitates bone regeneration in areas with bone defects. Transcriptomic analysis further reveals that the simultaneous release of Zn2+ and Li+ from the biodegradable Zn‐0.8Li scaffold contributes to anti‐osteosarcoma activity by downregulating PI3K/Akt signaling pathways. Taken together, the Zn‐0.8Li porous scaffold fabricated using laser powder bed fusion with enhanced antitumor and osteogenic properties is a promising alternative for the postoperative management of osteosarcoma.
Multilevel Optical Storage, Dynamic Light Modulation, and Polarization Control in Filamented Memristor System
Authors: Korneluk Alexander , Stefaniuk Tomasz
Published: November 2024

The electrochemical metallization (ECM) mechanism is emerging as a promising approach for the development of optical memristors—nonvolatile memory systems proposed for use as artificial synapses in neuromorphic computing applications. ECM memristors offer exceptional operating dynamics and power efficiency compared to other systems, but challenges with reproducible cycle‐to‐cycle state switching and the absence of advanced optical functionalities hinder their integration into photonic systems. In this work, an ECM free‐standing memristor structure is proposed, which simultaneously offers wavelength‐dependent multilevel nonvolatile optical storage, volatile light modulation, and dynamic polarization control. It is demonstrated that in the presence of a resonance, the optical readout provides noise‐free, robust, and significantly more accurate information about the memristor's state than electrical measurement. The use of light allows to gain insight into the intermediate electrical levels of the device as it transitions between high and low resistance states and to recover the complete record of applied voltages even when stochastic filament ruptures occur. Finally, the investigations show that spectroscopic ellipsometry provides real‐time information on the dynamics of cation movement and the corresponding permittivity changes at the interfaces between the switching layer and the electrodes, thus becoming a complementary characterization method for ECM memristors alongside state‐of‐the‐art techniques.
Tandem Upgrading of Bio‐Furans to Benzene, Toluene, and p‐xylene by Pt1Sn1 Intermetallic Coupling Ordered Mesoporous SnO2 Catalyst
Authors: Xiao Shoukang , Wang Li , Chen Liyu , Li Yingwei , Shen Kui
Published: November 2024

Benzene, toluene, and p‐xylene (BTpX) are among the most important commodity chemicals, but their productions still heavily rely on fossil resources and thus pose serious environmental burdens and energy crisis. Herein, the tandem upgrading of bio‐furans is reported to high‐yield BTpX by rationally constructing a versatile Pt1Sn1 intermetallic coupling ordered‐mesoporous SnO2 (OM‐SnO2) catalyst. It is shown that with increasing reduction temperature from 200 to 350 °C, Pt nanoparticles (NPs) are first formed on OM‐SnO2, then converted to Pt3Sn1 intermetallic nanoparticles (iNPs), and finally to Pt1Sn1 iNPs with a gradually‐thickened SnO2 overlayer. Impressively, the Pt1Sn1 iNPs and defect‐rich OM‐SnO2 in the optimized Pt@OM‐SnO2 can serve as the highly‐active species for the hydrogenolysis of 5‐hydroxymethylfuran to 2,5‐dimethylfuran and the aromatization of 2,5‐dimethylfuran with acrylic acid to p‐xylene, affording the highest yields of 99.1% and 96.1%, respectively. More importantly, it can perfectly realize the tandem upgrading of furan, furfural and 5‐hydroxymethylfuran to benzene, toluene and p‐xylene with high yields of 94.6%, 94.2% and 95.2%, respectively, representing a new tandem catalytic system to realize the high‐yield BTpX productions from their corresponding bio‐furans. This catalyst also shows good recyclability and excellent scalability, which together with its superior activity/selectivity suggest a high potential for sustainable BTpX productions.
Integrated Transcriptome Analysis Reveals Novel Molecular Signatures for Schizophrenia Characterization
Authors: Ni Tong , Sun Yu , Li Zefeng , Tan Tao , Han Wei , Li Miao , Zhu Li , Xiao Jing , Wang Huiying , Zhang Wenpei , Ma Yitian , Wang Biao , Wen Di , Chen Teng , Tubbs Justin , Zeng Xiaofeng , Yan Jiangwei , Gui Hongsheng , Sham Pak , Guan Fanglin
Published: November 2024

Schizophrenia (SCZ) is a complex psychiatric disorder presenting challenges for characterization. The current study aimed to identify and evaluate disease‐responsive essential genes (DREGs) to enhance the molecular characterization of SCZ. RNA‐sequencing data from PsychENCODE (536 SCZ patients, 832 controls) and peripheral blood transcriptome data from 144 recruited subjects (59 SCZ patients, 6 non‐SCZ psychiatric patients, 79 controls) are analyzed. Shared differential expression genes are obtained using three algorithms. Support vector machine (SVM)‐based recursive feature elimination is employed to identify DREGs. The biological relevance of these DREGs is examined through protein–protein interaction network, pathway enrichment, polygenic scoring, and brain tissue expression. Key DREGs are validated in SCZ animal models. A DREGs‐based machine‐learning model for SCZ characterization is developed and its performance is assessed using multiple datasets. The analysis identified 184 DREGs forming an interconnected network involved in synaptic plasticity, inflammation, neuronal development, and neurotransmission. DREGs exhibited distinct expression in SCZ‐related brain regions and animal models. Their genetic contributions are comparable to genome‐wide polygenic risk scores. The DREG‐based SVM model demonstrated high performance (AUC 85% for SCZ characterization, 79% for specificity). These findings provide new insights into the molecular mechanisms underlying SCZ and emphasize the potential of DREGs in improving SCZ characterization.
Dual‐Vibration‐Assisted Charge Transport Through Hexabenzocoronene in Single‐Molecule Junctions
Authors: Zhang Miao , Wang Boyu , Jia Hongxing , Xie Xinmiao , Hao Jie , Zhou Li , Du Pingwu , Wang Jinying , Jia Chuancheng , Guo Xuefeng
Published: November 2024

Gaining deep understanding and effective regulation of the charge transport mechanism within molecular junctions is essential for the development of electronic devices. In this work, a series of hexabenzocoronene‐based single‐molecule junctions are successfully constructed, and their temperature‐dependent charge transport properties are studied. It is found that rotational vibrations of both benzene and hexabenzocoronene rings are sequentially excited as the temperature increases, and the electron‐vibration coupling enhances charge tunneling. In addition, the transition temperature between distinct vibration‐assisted tunneling modes and the activation energies show strong correlations with the molecular vibration frequency and molecular length. This study unveils the distinct dual‐vibration‐assisted molecular tunneling mechanism, significantly enhancing the ability to precisely control molecular charge transport and develop functional molecular devices.
Aqueous Ammonia Sensor with Neuromorphic Detection
Authors: Vyshniakova Kateryna , Hosseini Mohammad Javad Mirshojaeian , Bai Huiwen , Fatahi Masoome , Malacco Victor Marco Rocha , Donkin Shawn S , Voyles Richard M , Nawrocki Robert A.
Published: November 2024

A hybrid inorganic–organic neuromorphic sensor utilizing a thin film zinc oxide (ZnO) detector with organic neuromorphic pre‐processing is developed to quantify ammonia in aqueous environments, including biological analytes. Impedimetric ZnO sensor, connected to an organic somatic circuit, reliably and accurately detects changes in electrical impedance to measure and quantify variations in the concentration of ammonia. The sensing mechanism of the ZnO thin film sensor is hypothesized to be the cause of the decrease in resistance of a solution with an increase in ammonia concentration. It is found that the surface oxide of the ZnO layer reacts with even very low concentrations of ammonia (), leading to changes in resistivity. This makes the sensor capable of detecting ammonia in a range of concentrations between 0.0001 and 0.1 M. A neuromorphic circuit converts the analog change of ammonia concentration expressed as a change of sensor impedance to the digitized frequency of spikes. Detecting such a low ammonia concentration is critical for environmental monitoring and medical diagnosis. The digitized nature of neuromorphic signal pre‐processing makes it more resilient for signal transmission in the presence of noise and serves as a demonstration of “smart sensing.”
Phase Change Memory: A Review on Electrical Behavior and Use in Analog In‐Memory‐Computing (A‐IMC) Applications
Authors: Boniardi Mattia , Baldo Matteo , Allegra Mario , Redaelli Andrea
Published: November 2024

Recent development and progress of Artificial Intelligence (AI) algorithms made clear that this topic is a paradigm shift with respect to the past. High throughput and ability to do complex tasks makes AI a great field of opportunity. This advancement is somehow limited by the physical implementation of the chips that are still bound to the historical von‐Neumann Architecture with processing units and memory hardware spatially separated. The way data is bussed and processed needs disruptive innovation, rather than an evolutionary approach, too. In Analog In‐Memory Computing (A‐IMC) the typical properties of resistance‐based memory technologies are used to both store and compute information. This allows for incredibly high parallelism and removes the problems related to the known von‐Neumann bottleneck. In the present work, A‐IMC networks based on resistive memories and on the Phase Change Memory (PCM) technology, in particular, are extensively discussed. After a first review of the general features of PCM devices, their application to A‐IMC is described, aiming at a full description of the current technological scenario.
Self‐Assembled Monolayer Dyes for Contact‐Passivated and Stable Perovskite Solar Cells
Authors: Isikgor Furkan H. , Pradhan Rakesh R. , Zhumagali Shynggys , Maksudov Temur , Naphade Dipti , Petoukhoff Christopher E. , Khan Jafar I. , Hnapovskyi Vladyslav , Harrison George T. , Combe Craig , Liu Jiang , Marsh Adam , Alharbi Essa A. , Heeney Martin , Laquai Frédéric , Schwingenschlögl Udo , Anthopoulos Thomas D. , De Wolf Stefaan
Published: November 2024

Surface modification of transparent conductive oxides (TCOs) with carbazole‐based self‐assembled monolayers (SAMs) is an effective method toward the formation of highly efficient hole‐selective contacts, enabling the fabrication of high‐performance perovskite solar cells (PSCs). However, the lack of long‐term structural and performance stability of the TCO/SAM/perovskite stack endangers the market entry of PSCs. Here, it is demonstrated that these challenges can be overcome by employing dyes as multi‐functional SAMs, simultaneously facilitating charge transport, passivating interfacial defects, and acting as a “molecular adhesive” layer, preserving structural integrity of the contact stack. Particularly, the surface modification of ITO with a dye (N719) monolayer is shown to create a hole‐selective contact for the fabrication of p–i–n PSCs with power conversion efficiencies reaching 24%. The N719 SAM‐based PSCs have also shown superior stability compared to state‐of‐the‐art PSCs incorporating carbazole SAMs and polyarylamine hole‐selective contacts by preserving ≈90% of their initial PCE under continuous light and thermal stress tests for 1000 h. The robustness of the ITO/N719/perovskite stack is attributed to its low interfacial trap density, UV resilience and strong adhesion capability. These findings place dye SAMs as a promising alternative for improving the performance of next‐generation photovoltaics.
Visualizing Performances Losses of Perovskite Solar Cells and Modules: From Laboratory to Industrial Scales
Authors: Yan Genghua , Yuan Ye , Kaba Mory , Kirchartz Thomas
Published: November 2024

While the efficiencies of lab‐sized perovskite solar cells are continuously rising, a variety of challenges have to be overcome to realize remotely similar efficiencies in an industrial context. Any changes in the preparation process, device size, device architecture, and material type are likely to result in efficiency loss. To date, there have been no solutions that can produce large‐area modules with performance comparable to that of laboratory devices. However, depending on the type of deposition process, the dominant loss mechanisms differ significantly, which can guide the further optimization of processes and devices. In this study, a meta‐analysis of state‐of‐the‐art perovskite solar cells and modules with different preparation methods, area sizes, and material compositions, is presented. Moreover, the efficiency losses are divided into five figures of merit and they are visualized to discuss the efficiency‐limiting loss mechanisms that must be overcome for commercialization.
Self‐Supported Metallic Alkaline Hydrogen Evolution Electrocatalysts Tolerant for Ampere‐Level Current Densities
Authors: Xiong Hao , Zhuang Rong , Cheng Bo , Liu Dengke , Du Yuxuan , Wang Hongyue , Liu Ye , Xu Fei , Wang Hongqiang
Published: November 2024

Electrocatalytic water splitting is an attractive approach for large‐scale hydrogen generation, critical for global carbon neutrality. However, the prevalent commercialized alkaline water electrolysis is generally conducted at low current densities due to sluggish kinetics and high overpotential, severely hampering high‐efficiency hydrogen production. Exploration of hydrogen evolution reaction (HER) electrocatalysts that can reliably operate at ampere‐level current densities under low overpotentials is thus a primary challenge. In contrast to extensive studies using powdery electrocatalysts, the self‐supported metallic catalytic cathode has become a burgeoning direction toward ampere‐level current densities, owing to their integrated design with intensive interfacial binding, high conductivity and mechanical stability with industrial tolerance/adaption. Recent years have witnessed tremendous research advances in designing self‐supported metallic electrocatalysts. Therefore, this flourishing area is specially summarized. Beginning with the introduction to the theory and mechanism of alkaline HER, the engineering strategies on self‐supported metallic electrodes are systematically summarized, including metal and alloy construction, heterostructure engineering, doping manipulation, and surface design. Meanwhile, particular emphasis is focused on the relationship between structure, activity, and stability under ampere‐level HER. Finally, the existing challenges, requirements of industrial‐scale application, and future direction for designing electrocatalysts are summarized, aiming to provide a better solution for industrial alkaline water electrolysis.
Effect of voxelotor on cerebral perfusion and cerebral oxygen metabolism and cardiac stress in adult patients with sickle cell disease
Authors: Konté Kadère , Afzali‐Hashemi Liza , Baas Koen P. A. , Schrantee Anouk , Wood John C. , Nur Erfan , Nederveen Aart J. , Biemond Bart J.
Published: November 2024

Sickle cell disease (SCD) is complicated by silent cerebral infarcts (SCIs), for which anemia is an important risk factor. Despite normal oxygen delivery (OD), cerebral vascular reserve (CVR), and cerebral metabolic rate of oxygen (CMRO2) are diminished in SCD, possibly causing the formation of SCIs. Voxelotor inhibits polymerization by increasing the hemoglobin oxygen binding, ameliorating hemolytic anemia. Furthermore, anemia is related to cardiac complications. Our aims were to assess the effect of voxelotor on markers of cerebral perfusion, cerebral oxygen metabolism, and markers of cardiac stress in SCD patients. Cerebral hemodynamics and oxygen metabolism were measured with MRI before and after 3 months of voxelotor treatment (1500 mg/day) in 18 adults with SCD (HbSS/HbSβ0‐thalassemia). Hemoglobin levels significantly increased (p = .001) and markers of hemolysis decreased (p < .05). OD increased from 6.5 (IQR, 6.0–7.1) mL O2/100 g/min to 8.1 (IQR, 7.2–8.7) mL O2/100 g/min (p = .001). CBF and CVR did not change. CMRO2 decreased from 2.0 (IQR, 1.9–2.1) mL O2/100 g/min to 1.9 (IQR, 1.6–2.1) mL O2/100 g/min (p = .03). N‐terminal pro‐B type natriuretic peptide (NT‐proBNP) levels decreased (p = .048) and maximum tricuspid regurgitation flow velocity (TRVmax) normalized in all but one patient with increased TRVmax. Voxelotor treatment in patients with severe SCD did not decrease CBF despite increased Hb levels. Cerebral oxygen metabolism slightly decreased, despite raised OD, most likely due to drug‐induced increase in oxygen binding. Nonetheless, voxelotor improved clinically validated markers of cardiac stress.
Meta‐Analysis of the Heritability of Childhood Height From 560 000 Pairs of Relatives Born Between 1929 and 2004
Authors: Dewau Reta , Boomsma Aafke , Doyle Caitlin , Byrne Stephanie , Hyppönen Elina , Lee Sang Hong , Benyamin Beben
Published: November 2024

Background

Childhood height is commonly used to measure children's health and nutritional status. It is used to define stunting, where a child is considered stunted if their height is shorter than two standard deviations below the Child Growth Standards median. Studies have shown that genetic and environmental factors contribute to childhood height, so understanding these contributions is important for stunting research. This systematic review and meta‐analysis examined the contribution of these factors across study designs and ancestries.

Methods

A systematic search found 28 twin and 26 family studies spanning from birth to 17 years. We identified 162 293 twin, 380 195 parent‐offspring, and 19 965 sibling pairs born between 1929 and 2004. These datasets were meta‐analyzed using a random effects model. The review is registered in PROSPERO (ID CRD42023432550).

Results

The estimated heritability (h
2) of height from twin design increased from birth to 17 years. For children under 5 years, the estimated heritability was 0.57 (95%CI, 0.52–0.61) for European, 0.48 (0.39–0.57) for Asian, and 0.46 (0.40–0.51) for multi ancestries. Heritability estimated from parent‐offspring design was 0.46 (95%CI, 0.28–0.62) at birth and 0.76 (95%CI, 0.70–0.80) at 17 years. Meanwhile, the estimated heritability from sibling design remained constant across ages at 0.70 (95%CI, 0.52–0.83).

Conclusions

The heritability estimates of childhood height were slightly higher in European ancestries, but in general, they did not significantly differ across ancestry groups. While the shared environmental effects on height peak in early childhood, the estimated heritability increase in late teens. Unique environmental factors play a small, but significant role throughout childhood.
Promotion of Metal‐Free Catalytic Coupling of Fluorinated Halogenated Hydrocarbons By a Base for the Synthesis of Difluoromethyl Heterocyclic Amines
Authors: Zhong Man , Li Xin‐Yue , Zhang Jin , Chen Li , Hu Yun‐Long , Li Yang
Published: November 2024

The selective functionalization of difluoromethyl groups (−CF2) is a promising approach and an attractive synthetic route for accessing fluorine‐containing moieties with medicinal benefits. Here, we report a case of a C−N coupling reaction between bromodifluoropropene with heterocyclic amines, such as indole, pyrrole, and imidazole, promoted by an alkali without the use of transition metal catalysis. This reaction differs from existing methods in that it does not undergo a difluoromethylation isomerization reaction but directly retains the structure of the terminal olefin. This chemical conversion process has a wide substrate range, good functional group tolerance, and an ideal reaction conversion rate, making it an effective new method for the difluoropropenation of heterocyclic amines.
Hubbard Gap Closure‐Induced Dual‐Redox Li‐Storage Mechanism as the Origin of Anomalously High Capacity and Fast Ion Diffusivity in MOFs‐Like Polyoxometalates
Authors: Wang Xinran , Li Songjie , Wu Feng , Chen Hailong , Wenxing Chen W. , Zhao Wenbin , Kang Kaidi , Guo Ruiqi , Sun Yuheng , Zhai Liqing , Zhao Ran , Gao Aolei , Bai Ying , Wu Chuan
Published: November 2024

MOFs‐like polyoxometalate (POMs) electrodes, harvesting combined advantages of interlocking porosity and multi‐electron transfer reaction, have already emerged as promising candidates for lithium‐ion batteries (LIBs), yet the origins of the underlying redox mechanism in such materials remain a matter of uncertainty. Of critical challenges are the anomalously high storage capacities beyond their theoretical values and the fast ion diffusivity that cannot be satisfactorily comprehended in the theory of crystal lattice. Herein, for the first time we decode t2g electron occupation‐regulated dual‐redox Li‐storage mechanism as the true origin of extra capacity in POMs electrodes. The lattice and electronic transition of active centers and reaction intermediates were systematically decoupled through density functional theory (DFT) and a suite of structural spectroscopic investigations, such as X‐ray absorption near‐edge spectroscopy (XANES), soft X‐ray absorption spectroscopy (sXAS) and 7Li solid‐state nuclear magnetic resonance (NMR). Enhanced V‐t2g orbital occupation by Li coordination significantly triggers the Hubbard gap closure and reversible Li deposition/dissolution at surface region. Conjugated V−O‐Li configuration at interlayers endow Li+ ion pathways along pore walls as the dominant contribution to the low migration barrier and fast diffusivity. As a result, remarkable cycle stability (~100 % capacity retention after 2000 cycles at 1 A g−1), extremely high specific capacity (1200 mAh g−1 at 100 mA g−1) and excellent rate performance (404 mAh g−1 at 8 A g−1) were achieved, providing new understandings on the underlying mechanism of POMs electrodes and pivotal guidance for dual‐storage materials.
Nickel‐Catalyzed Difluoroalkylation of β,γ‐Unsaturated α‐Amino Nitrile Derived Lithium Reagents
Authors: Tong Fei‐Fei , Luo Yun‐Cheng , Zhao Hai‐Yang , Fu Xia‐Ping , Zhang Xingang
Published: November 2024

Organolithium reagents, known for their low cost, ready availability, and high reactivity, allow fast cross‐coupling under ambient conditions. However, their direct cross‐coupling with fluoroalkyl electrophiles remains a formidable challenge due to the easy formation of thermo‐unstable fluoroalkyl lithium species during the reaction, which are prone to decomposition via rapid α/β‐fluoride elimination. Here, we exploit heteroatom‐stabilized allylic anions to harness the exceptional reactivity of organolithium reagents, enabling the compatibility of difluoroalkyl halides and facilitating versatile and precise fluorine functionality introduction under mild conditions. In this process, a nickel‐catalyzed difluoroalkylation of β,γ‐unsaturated α‐amino nitrile derived lithium reagents (N‐stabilized allyl lithium reagents) with various difluoroalkyl bromides has been developed, opening a new avenue to access fluorinated compounds through catalytic cross‐coupling of organolithium reagents with fluoroalkyl electrophiles. This approach allows for the efficient and precise construction of secondary C(sp3)−CF2R bonds, previously challenging in transition‐metal‐catalyzed fluoroalkylation reactions due to β‐hydride elimination. The rapid fluorine‐editing of drugs demonstrates the synthetic versatility and utility of this protocol, showing the perspective in modern drug discovery.
Hexafluorphosphat‐induzierter Wasserstoff‐Isotopenaustausch (HIE) in fluorierten Umgebungen: Deuterierung aromatischer Verbindungen durch Aktivierung starker Bindungen
Authors: Ni Yang , Lebelt Jonathan , Barp Milena , Kreuter Florian , Buttkus Hannah , Jin Jiaye , Kretzschmar Martin , Tonner‐Zech Ralf , Asmis Knut R. , Gulder Tanja
Published: November 2024

Effiziente und milde Methoden zur Late‐Stage‐Deuterierung von Kohlenstoffgerüsten sind stark nachgefragt. In dieser Arbeit beschreiben wir eine einfache und äußerst effektive Syntheseroute für den Wasserstoffisotopenaustausch (HIE) in aromatischen Verbindungen unter milden Reaktionsbedingungen. Unsere Methode verwendet katalytische Mengen an Hexafluorphosphatsalz (PF6−) in deuteriertem 1,1,1,3,3,3‐Hexafluorisopropanol (HFIP‐d1) und D2O, wodurch Phenole, Aniline, Anisole und heterozyklische Verbindungen in hohen Ausbeuten mit exzellenter Deuterium‐Inkorporationsrate umgesetzt werden konnten. Somit wurde eine Vielzahl deuterierter, aromatischer Verbindungen zugänglich. Spektroskopische und theoretische Untersuchungen zeigten ein aktives Wasserstoffbrückennetzwerk, aufgebaut durch HFIP‐d1, wodurch die inerte P−F‐Bindung in PF6− für den Angriff von D2O aktiviert wurde. Das so in situ entstehende DPO2F2 ermöglicht HIE, wodurch ein neuartiger Weg zu deuterierten Synthese‐Bausteinen, Arzneistoffen und Naturstoffderivaten mit hohem Deuteringsgrad durch die Aktivierung von starken Bindungen ermöglicht wird.
Distinctive Photomechanical Shape Change of p‐Phenylenediacrylic Acid Dimethyl Ester Single Crystals Induced by a Spatially Heterogeneous Photoreaction
Authors: Kitagawa Daichi , Tomoda Rei , Ramos Sebastian A. , Beran Gregory J. O. , Bardeen Christopher J. , Kobatake Seiya
Published: November 2024

Understanding photoreaction dynamics in crystals is important for predicting the dynamic property changes accompanying these photoreactions. In this work, we investigate the photoreaction dynamics of p‐phenylenediacrylic acid dimethyl ester (p‐PDAMe) in single crystals that show reaction front propagation, in which the photoreaction proceeds heterogeneously from the edge to the center of the crystal. Moreover, we find that p‐PDAMe single crystals exhibit a distinctive crystal shape change from a parallelogram to a distorted shape resembling a fluttering flag, then to a rectangle as the photoreaction proceeds. Density functional theory calculations predict the crystal structure after the photoreaction, providing a reasonable explanation of the distinctive crystal shape change that results from the spatially heterogeneous photoreaction. These results prove that the spatially heterogeneous photoreaction dynamics have the ability to induce novel crystal shape changes beyond what would be expected based on the equilibrium reactant and product crystal shapes.
Low‐temperature CO2 Hydrogenation to Olefins on Anorthic NaCoFe Alloy Carbides
Authors: Han Jianxiang , Han Yu , Yu Jiafeng , Sun Yannan , Cui Xiwen , Ge Qingjie , Sun Jian
Published: November 2024

The hydrogenation of carbon dioxide to olefins (CTO) represents an ideal pathway towards carbon neutrality. However, most current CTO catalysts require a high‐temperature condition of 300–450 °C, resulting in high energy consumption and possible aggregation among active sites. Herein, we developed an efficient iron‐based catalyst modified with high‐sodium content (7 %) and low‐cobalt content (2 %), achieving a CO2 conversion of 22.0 % and an olefin selectivity of 55.9 % at 240 °C and 1000 mL/g/h, and it is even active at 180 °C and 4000 mL/g/h with more than 25 % olefins in hydrocarbons. The catalyst was kept stable under continuous operating conditions of 500 hours. Numerous characterizations and calculations reveal high content of sodium as an electronic promoter enhances the stability of the active anorthic Fe5C2 phase at low temperatures. Further incorporating the above catalyst with cobalt, as a structural promoter, causes Fe species to form a FexCoy alloying phase, which in turn facilitates the formation of higher active anorthic (FexCoy)5C2 phase, different from the conventional carbides and alloy carbides. An in‐depth investigation of the synergistic effects of structural and electronic promoters can improve catalyst performance, increase reaction efficiency and cost‐effectiveness, and provide profound insights for understanding and optimizing CO2 hydrogenation reactions.
Stereoselective Synthesis of 1,n‐Dicarbonyl Compounds Through Palladium‐Catalyzed Ring Opening/Isomerization of Densely Substituted Cyclopropanols
Authors: Teschers Charlotte S. , Cohen Anthony , Marek Ilan
Published: November 2024

We report a highly diastereoselective protocol for the synthesis of 1,4‐ and 1,5‐dicarbonyl compounds from densely substituted cyclopropanols. The methodology involves a palladium‐catalyzed ring opening reaction followed by a “metal‐walk” and oxidation of a remote hydroxyl group. The methodology represents a new application of cyclopropanols as initiation sites for chain walking remote functionalization. Importantly, this approach provides a straightforward access to highly valuable succinaldehyde derivatives bearing vicinal quaternary and tertiary stereocenters as single diastereomers.
A Microporous Hydrogen‐Bonded Organic Framework with Open Pyrene Sites Isolated by Hydrogen‐Bonded Helical Chains for Efficient Separation of Xenon and Krypton
Authors: He Lei , Li Yunbin , Li Lu , Wang Zhitao , Chen Yanting , Yuan Furong , Lan Gaoyan , Chen Chenxin , Xiang Shengchang , Chen Banglin , Zhang Zhangjing
Published: November 2024

Achieving efficient xenon/krypton (Xe/Kr) separation in emerging hydrogen‐bonded organic frameworks (HOFs) is highly challenging because of the lack of gas‐binding sites on their pore surfaces. Herein, we report the first microporous HOF (HOF‐FJU‐168) based on hydrogen‐bonded helical chains, which prevent self‐aggregation of the pyrene core, thereby preserving open pyrene sites on the pore surfaces. Its activated form, HOF‐FJU‐168a is capable of separating Xe/Kr under ambient conditions while achieving an excellent balance between adsorption capacity and selectivity. At 296 K and 1 bar, the Xe adsorption capacity of HOF‐FJU‐168a reached 78.31 cm3/g, with an Xe/Kr IAST selectivity of 22.0; both values surpass those of currently known top‐performing HOFs. Breakthrough experiments confirmed its superior separation performance with a separation factor of 8.6 and a yield of high‐purity Kr (>99.5 %) of 184 mL/g. Furthermore HOF‐FJU‐168 exhibits excellent thermal and chemical stability, as well as renewability. Single‐crystal X‐ray diffraction and molecular modeling revealed that the unique electrostatic surface potential around the open pyrene sites creates a micro‐electric field, exerting a stronger polarizing effect on Xe than on Kr, thereby enhancing host‐Xe interactions.