bluuebunny/crossref_metadata_2025_split huggingface dataset:
Engineering Nanozymes for Tumor Therapy via Ferroptosis Self‐Amplification
Authors: Liu Shuyu , Wei Yi , Liang Yuan , Du Pengye , Lei Pengpeng , Yu Duo , Zhang Hongjie 
Published: April 2024

AbstractFerroptosis induction is an emerging strategy for tumor therapy. Reactive oxygen species (ROS) can induce ferroptosis but are easily consumed by overexpressed glutathione (GSH) in tumor cells. Therefore, achieving a large amount of ROS production in tumor cells without being consumed is key to efficiently inducing ferroptosis. In this study, a self‐amplifying ferroptosis‐inducing therapeutic agent, Pd@CeO2‐Fe‐Co‐WZB117‐DSPE‐PEG‐FA (PCDWD), is designed for tumor therapy. PCDWD exhibits excellent multi‐enzyme activities due to the loading of Fe‐Co dual atoms with abundant active sites, including peroxidase‐like enzymes, catalase‐like enzymes, and glutathione oxidases (GSHOx), which undergo catalytic reactions in the tumor microenvironment to produce ROS, thereby inducing ferroptosis. Furthermore, PCDWD can also deplete GSH in tumor cells, thus reducing the consumption of ROS by GSH and inhibiting the expression of GSH peroxidase 4. Moreover, the photothermal effect of PCDWD can not only directly kill tumor cells but also further enhance its own enzyme activities, consequently promoting ferroptosis in tumor cells. In addition, WZB117 can reduce the expression of heat shock protein 90 by inhibiting glucose transport, thereby reducing the thermal resistance of tumor cells and further improving the therapeutic effect. Finally, X‐ray computed tomography imaging of PCDWD guides it to achieve efficient tumor therapy.
Advancing MR‐TADF OLED Toward True‐Blue CIE Value via Asymmetric Host Materials with Amorphous Morphology
Authors: Han Chih‐Pin , Shi Emily Hsue‐Chi , Chen Chieh An , Hsu Chao‐Hsien , Chen Chia‐Hsun , Wu Chi‐Chi , Lee Yi‐Ting , Chiu Tien‐Lung , Lee Jiun‐Haw , Leung Man‐kit , Chou Pi‐Tai 
Published: April 2024

AbstractThe new host materials are reported to boost the multiple resonance‐induced thermally activated delayed fluorescence (MR‐TADF) based pure deep‐blue organic light emitting diodes (OLEDs) toward further shortening the emission full width at the half maximum (FWHM). Based on an unusual asymmetric design concept, two new host compounds Bz2cb and Bz2cbz are synthesized. Despite possessing a compact and rigid molecular packing in crystal, Bz2cbz shows pure amorphous morphology via vapor deposition, as confirmed by the grazing‐incidence wide‐angle X‐ray scattering (GIWAXS) analysis. Via incorporating a promising MR‐TADF emitter, ν‐DABNA‐O‐Me, into Bz2cb and Bz2cbz films, highly pure deep‐blue OLEDs are successfully demonstrated. Remarkably, the Bz2cbz device exhibits a 464 nm electroluminescence (EL) with narrow FWHM of 22 nm, accompanied by the reduction of the 0–1 vibronic sideband, and a maximum external quantum efficiency (EQEmax) of 28.2%, which, overall, reaches the true‐blue Commission Internationale de l'Eclairage coordinates (CIE) of (0.13, 0.07) and the high blue index of 253. The amorphous film formation turns out to be an important factor that is previously unrecognized to externally fine‐tune the MR‐TADF OLEDs toward even higher color purity.
2D‐Material‐Fused High‐Emittance Plasmo–Photonic Metasurfaces
Authors: Iwanaga Masanobu , Yang Xu , Karanikolas Vasilios , Kuroda Takashi , Sakuma Yoshiki 
Published: April 2024

AbstractTransition metal dichalcogenides (TMDC) are a family of atomic‐layer 2D materials (2dMs). Many researches have attempted to reinforce the unique properties by incorporating artificially designed nanostructures. Here, a highly photoluminescence (PL) enhancing platform is reported that is formed by combining high‐emittance plasmo–photonic metasurfaces with a large‐area 2dM, which is a continuous monolayer of TMDC of cm2 dimension. It is experimentally demonstrated that the 2dM‐PL intensity at room temperature is enhanced by more than 1030‐fold in comparison with that observed on the flat gold film regions. The enhancement is associated with spectral transformation indicating a resonant effect of the metasurfaces. It is moreover revealed that the confocal PL image originates from a coherent single‐mode emission that forms a photon number distribution obeying the Poisson probability distribution. Thus, the 2dM‐fused metasurfaces function as efficient coherent quantum light sources. PL decay‐time analysis also reveals the coexistence of two components in the enhanced PL. The fast component exhibits a lifetime of 18 ps whereas the slow component decays at 4.4 ns. Both components are most likely to undergo radiative processes, which indicates that metal‐induced PL quenching is suppressed on these 2dM‐fused metasurfaces. The long lifetime component is ascribed to an excitonic intervalley transition.
High‐Performance White Emission from Cu‐Based Perovskite Compound
Authors: Zhang Wei , Chu Zema , Jiang Ji , Zhang Siyao , Hao Huiying , Wei Tongbo , Zhang Xingwang , You Jingbi 
Published: April 2024

AbstractThe white emissions based on lead‐free perovskites with broadband emission due to self‐trapped excitons (STEs) are considered as an ideal candidate for next‐generation white light‐emitting diodes (WLEDs). Recently, copper‐based halide perovskites Cs3Cu2I5@CsCu2I3 composites films with a high color‐rendering index (CRI) have been developed for WLEDs. However, the Cs3Cu2I5@CsCu2I3 composites generally exhibit a relatively low photoluminescence quantum yield (PLQY). Herein, a high PLQY up to 86.75% copper‐based perovskite Gua3Cu2I5 (Gua = guanidine) films with a broadband strong yellow STEs emission centered at 544 nm is synthesized. By combining with efficient blue STEs emission Cs3Cu2I5 component via composition engineering of Cs3Cu2I5@Gua3Cu2I5, a high PLQY of up to 96.1% is achieved on the white emission composites films. Moreover, a high CRI of 93 WLEDs is achieved by integrating Cs3Cu2I5@Gua3Cu2I5 composites film onto a UV LED chip. These findings provide a simple and effective strategy for designing highly efficient white light‐emitting diodes.
Liquid–Liquid Phase Separation‐Mediated Photocatalytic Subcellular Hybrid System for Highly Efficient Hydrogen Production
Authors: Yu Xiaoxuan , Li Hui , Xu Chengchen , Xu Zhengwei , Chen Shuheng , Liu Wang , Zhang Tianlong , Sun Hongcheng , Ge Yan , Qi Zhenhui , Liu Junqiu 
Published: April 2024

AbstractPlant chloroplasts have a highly compartmentalized interior, essential for executing photocatalytic functions. However, the construction of a photocatalytic reaction compartment similar to chloroplasts in inorganic–biological hybrid systems (IBS) has not been reported. Drawing inspiration from the compartmentalized chloroplast and the phenomenon of liquid–liquid phase separation, herein, a new strategy is first developed for constructing a photocatalytic subcellular hybrid system through liquid–liquid phase separation technology in living cells. Photosensitizers and in vivo expressed hydrogenases are designed to coassemble within the cell to create subcellular compartments for synergetic photocatalysis. This compartmentalization facilitates efficient electron transfer and light energy utilization, resulting in highly effective H2 production. The subcellular compartments hybrid system (HM/IBSCS) exhibits a nearly 87‐fold increase in H2 production compared to the bare bacteria/hybrid system. Furthermore, the intracellular compartments of the photocatalytic reactor enhance the system's stability obviously, with the bacteria maintaining approximately 81% of their H2 production activity even after undergoing five cycles of photocatalytic hydrogen production. The research brings forward visionary prospects for the field of semi‐artificial photosynthesis, offering new possibilities for advancements in areas such as renewable energy, biomanufacturing, and genetic engineering.
Li Stripping Behavior of Anode‐Free Solid‐State Batteries Under Intermittent‐Current Discharge Conditions
Authors: Lee Kiwoong , Sakamoto Jeff 
Published: April 2024

AbstractAnode‐free manufacturing holds promise to enable high energy densities and lower Lithium (Li)‐metal solid‐state batteries (LMSSBs). Nevertheless, in contrast to thick Li foil (>50 µm), the stripping capacity of in situ‐formed Li (10–30 µm) is limited due to diminished creep flow, resulting in reduced accessible capacity. This study explores the correlation between stripping capacity and surface roughness of garnet Li7La3Zr2O12 (LLZO) solid electrolyte. The results reveal that stripping capacity can be enhanced through the surface modification of solid electrolytes. Additionally, this study scrutinizes the stripping behavior of in situ Li under intermittent‐current discharge conditions, which are more relevant to the operational conditions of electric vehicles (EVs). It is demonstrated that, when compared to constant‐current stripping, intermittent‐current stripping effectively suppresses void formation and enhances the stripping capacity of in situ Li by 40%. It is considered that the intermittent current inhibits the accumulation of Li vacancies, thereby delaying the void formation. These findings provide valuable insights into the development of high‐performance anode‐free LMSSBs for EVs.
Redefining hyperviscosity in acute leukemia: Potential implications for red cell transfusions in the microvasculature
Authors: Musick Jamie O. , Williams Evelyn K. , Fibben Kirby S. , Zhang Dan Y. , Caruso Christina , Sakurai Yumiko , Tran Reginald , Kemp Melissa L. , Lam Wilbur A. 
Published: April 2024

AbstractHyperleukocytosis is an emergency of acute leukemia leading to blood hyperviscosity, potentially resulting in life‐threatening microvascular obstruction, or leukostasis. Due to the high number of red cells in the circulation, hematocrit/hemoglobin levels (Hct/Hgb) are major drivers of blood viscosity, but how Hct/Hgb mediates hyperviscosity in acute leukemia remains unknown. In vivo hemorheological studies are difficult to conduct and interpret due to issues related to visualizing and manipulating the microvasculature. To that end, a multi‐vessel microfluidic device recapitulating the size‐scale and geometry of the microvasculature was designed to investigate how Hct/Hgb interacts with acute leukemia to induce “in vitro” leukostasis. Using patient samples and cell lines, the degree of leukostasis was different among leukemia immunophenotypes with respect to white blood cell (WBC) count and Hct/Hgb. Among lymphoid immunophenotypes, severe anemia is protective against in vitro leukostasis and Hct/Hgb thresholds became apparent above which in vitro leukostasis significantly increased, to a greater extent with B‐cell acute lymphoblastic leukemia (ALL) versus T‐cell ALL. In vitro leukostasis in acute myeloid leukemia was primarily driven by WBC with little interaction with Hct/Hgb. This sets the stage for prospective clinical studies assessing how red cell transfusion may affect leukostasis risk in immunophenotypically different acute leukemia patients.
Stereoselective Synthesis of Polysubstituted Tetrahydropyrans by Brønsted Acid‐Mediated Hydroxyalkoxylation of Silylated Alkenols
Authors: Díez‐Poza Carlos , Val Patricia , López Enol , Barbero Asunción 
Published: April 2024

AbstractA convenient route for the preparation of tetrahydropyran (THP) derivatives with a quaternary and tertiary vicinal stereocenters is reported. The atom economy acid‐catalyzed cyclization of allylsilyl alcohols provided polysubstituted tetrahydropyrans in good yields and excellent diastereoselectivities (>95 : 5). In comparison with the traditional oxymercuration procedure, this approach resulted to be more efficient in both yield and stereocontrol.
Automatic classification of AD pathology in FTD phenotypes using natural speech
Authors: Cho Sunghye , Olm Christopher A. , Ash Sharon , Shellikeri Sanjana , Agmon Galit , Cousins Katheryn A. Q. , Irwin David J. , Grossman Murray , Liberman Mark , Nevler Naomi 
Published: April 2024

AbstractINTRODUCTIONScreening for Alzheimer's disease neuropathologic change (ADNC) in individuals with atypical presentations is challenging but essential for clinical management. We trained automatic speech‐based classifiers to distinguish frontotemporal dementia (FTD) patients with ADNC from those with frontotemporal lobar degeneration (FTLD).METHODSWe trained automatic classifiers with 99 speech features from 1 minute speech samples of 179 participants (ADNC = 36, FTLD = 60, healthy controls [HC] = 89). Patients’ pathology was assigned based on autopsy or cerebrospinal fluid analytes. Structural network‐based magnetic resonance imaging analyses identified anatomical correlates of distinct speech features.RESULTSOur classifier showed 0.88 0.03 area under the curve (AUC) for ADNC versus FTLD and 0.93 0.04 AUC for patients versus HC. Noun frequency and pause rate correlated with gray matter volume loss in the limbic and salience networks, respectively.DISCUSSIONBrief naturalistic speech samples can be used for screening FTD patients for underlying ADNC in vivo. This work supports the future development of digital assessment tools for FTD.Highlights
We trained machine learning classifiers for frontotemporal dementia patients using natural speech.
We grouped participants by neuropathological diagnosis (autopsy) or cerebrospinal fluid biomarkers.
Classifiers well distinguished underlying pathology (Alzheimer's disease vs. frontotemporal lobar degeneration) in patients.
We identified important features through an explainable artificial intelligence approach.
This work lays the groundwork for a speech‐based neuropathology screening tool.
Results from the long‐term extension of PRIME: A randomized Phase 1b trial of aducanumab
Authors: Chen Tianle , O'Gorman John , Castrillo‐Viguera Carmen , Rajagovindan Rajasimhan , Curiale Gioacchino G. , Tian Ying , Patel Dakshaben , von Rosenstiel Philipp , von Hehn Christian , Salloway Stephen , Hock Christoph , Nitsch Roger M. , Haeberlein Samantha Budd , Sandrock Alfred , Singhal Priya 
Published: April 2024

AbstractINTRODUCTIONAducanumab selectively targets aggregated forms of amyloid beta (Aβ), a neuropathological hallmark of Alzheimer's disease (AD).METHODSPRIME was a Phase 1b, double‐blind, randomized clinical trial of aducanumab. During the 12‐month placebo‐controlled period, participants with prodromal AD or mild AD dementia were randomized to receive aducanumab or placebo. At week 56, participants could enroll in a long‐term extension (LTE), in which all participants received aducanumab. The primary endpoint was safety and tolerability.RESULTSAmyloid‐related imaging abnormalities–edema (ARIA‐E) were the most common adverse event. Dose titration was associated with a decrease in the incidence of ARIA‐E. Over 48 months, aducanumab decreased brain amyloid levels in a dose‐ and time‐dependent manner. Exploratory endpoints suggested a continued benefit in the reduction of clinical decline over 48 months.DISCUSSIONThe safety profile of aducanumab remained unchanged in the LTE of PRIME. Amyloid plaque levels continued to decrease in participants treated with aducanumab.Highlights
PRIME was a Phase 1b, double‐blind, randomized clinical trial of aducanumab.
We report cumulative safety and 48‐month efficacy results from PRIME.
Amyloid‐related imaging abnormalities–edema (ARIA‐E) were the most common adverse event (AE); 61% of participants with ARIA‐E were asymptomatic.
Dose titration was associated with a decrease in the incidence of ARIA‐E.
Aducanumab decreased levels of amyloid beta (Aβ) in a dose‐ and time‐dependent manner.
Investigating reliable amyloid accumulation in Centiloids: Results from the AMYPAD Prognostic and Natural History Study
Authors: Bollack Ariane , Collij Lyduine E. , García David Vállez , Shekari Mahnaz , Altomare Daniele , Payoux Pierre , Dubois Bruno , Grau‐Rivera Oriol , Boada Mercè , Marquié Marta , Nordberg Agneta , Walker Zuzana , Scheltens Philip , Schöll Michael , Wolz Robin , Schott Jonathan M. , Gismondi Rossella , Stephens Andrew , Buckley Christopher , Frisoni Giovanni B. , Hanseeuw Bernard , Visser Pieter Jelle , Vandenberghe Rik , Drzezga Alexander , Yaqub Maqsood , Boellaard Ronald , Gispert Juan Domingo , Markiewicz Pawel , Cash David M. , Farrar Gill , Barkhof Frederik ,   AMYPAD consortium
Published: April 2024

AbstractINTRODUCTIONTo support clinical trial designs focused on early interventions, our study determined reliable early amyloid‐β (Aβ) accumulation based on Centiloids (CL) in pre‐dementia populations.METHODSA total of 1032 participants from the Amyloid Imaging to Prevent Alzheimer's Disease–Prognostic and Natural History Study (AMYPAD‐PNHS) and Insight46 who underwent [18F]flutemetamol, [18F]florbetaben or [18F]florbetapir amyloid‐PET were included. A normative strategy was used to define reliable accumulation by estimating the 95th percentile of longitudinal measurements in sub‐populations (NPNHS = 101/750, NInsight46 = 35/382) expected to remain stable over time. The baseline CL threshold that optimally predicts future accumulation was investigated using precision‐recall analyses. Accumulation rates were examined using linear mixed‐effect models.RESULTSReliable accumulation in the PNHS was estimated to occur at >3.0 CL/year. Baseline CL of 16 [12,19] best predicted future Aβ‐accumulators. Rates of amyloid accumulation were tracer‐independent, lower for APOE ε4 non‐carriers, and for subjects with higher levels of education.DISCUSSIONOur results support a 12–20 CL window for inclusion into early secondary prevention studies. Reliable accumulation definition warrants further investigations.
The Future of Chemical Sciences is Sustainable
Authors: Mitchell Sharon , Martín Antonio J. , Guillén‐Gosálbez Gonzalo , Pérez‐Ramírez Javier 
Published: April 2024

AbstractChemistry, a vital tool for sustainable development, faces a challenge due to the lack of clear guidance on actionable steps, hindering the optimal adoption of sustainability practices across its diverse facets from discovery to implementation. This Scientific Perspective explores established frameworks and principles, proposing a conciliated set of triple E priorities anchored on Environmental, Economic, and Equity pillars for research and decision making. We outline associated metrics, crucial for quantifying impacts, classifying them according to their focus areas and scales tackled. Emphasizing catalysis as a key driver of sustainable synthesis of chemicals and materials, we exemplify how triple E priorities can practically guide the development and implementation of processes from renewables conversions to complex customized products. We summarize by proposing a roadmap for the community aimed at raising awareness, fostering academia–industry collaboration, and stimulating further advances in sustainable chemical technologies across their broad scope.
High‐Performance Thermoelectric Fibers from Metal‐Backboned Polymers for Body‐Temperature Wearable Power Devices
Authors: Wang Ning , Zeng Kaiwen , Zheng Yuanyuan , Jiang Hongyu , Yang Yibei , Zhang Yifeng , Li Dingke , Yu Sihui , Ye Qian , Peng Huisheng 
Published: April 2024

AbstractMetal‐backboned polymers (MBPs), with a unique backbone consisting of bonded metal atoms, are promising for optic, electric, magnetic, and thermoelectric fields. However, the application of MBP remains relatively understudied. Here, we develop a shear‐induced orientation method to construct a flexible nickel‐backboned polymer/carbon nanotube (NBP/CNT) thermoelectric composite fiber. It demonstrated a power factor of 719.48 μW ⋅m−1 K−2, which is ca. 3.5 times as high as the bare CNT fiber. Remarkably, with the regulation of carrier mobility and carrier concentration of NBP, the composite fiber further showed simultaneous increases in electrical conductivity and Seebeck coefficient in comparison to the bare CNT fiber. The NBP/CNT fiber can be integrated into fabrics to harvest thermal energy of human body to generate an output voltage of 3.09 mV at a temperature difference of 8 K. This research opens a new avenue for the development of MBPs in power supply.
Best Practices for Experiments and Reports in Photocatalytic Methane Conversion
Authors: Jiang Yuheng , Li Siyang , Fan Yingying , Tang Zhiyong 
Published: April 2024

AbstractEfficiently converting methane into valuable chemicals via photocatalysis under mild condition represents a sustainable route to energy storage and value‐added manufacture. Despite continued interest in this area, the achievements have been overshadowed by the absence of standardized protocols for conducting photocatalytic methane oxidation experiments as well as evaluating the corresponding performance. In this review, we present a structured solution aimed at addressing these challenges. Firstly, we introduce the norms underlying reactor design and outline various configurations in the gas–solid and gas–solid–liquid reaction systems. This discussion helps choosing the suitable reactors for methane conversion experiments. Subsequently, we offer a comprehensive step‐by‐step protocol applicable to diverse methane‐conversion reactions. Emphasizing meticulous verification and accurate quantification of the products, this protocol highlights the significance of mitigating contamination sources and selecting appropriate detection methods. Lastly, we propose the standardized performance metrics crucial for evaluating photocatalytic methane conversion. By defining these metrics, the community could obtain the consensus of assessing the performance across different studies. Moving forward, the future of photocatalytic methane conversion necessitates further refinement of stringent experimental standards and evaluation criteria. Moreover, development of scalable reactor is essential to facilitate the transition from laboratory proof‐of‐concept to potentially industrial production.
Efficient and Selective Construction of 412 Metalla‐links Using Weak C−H⋅⋅⋅Halogen Interactions
Authors: Zhang Hai‐Ning , Huang Xi , Jin Guo‐Xin 
Published: April 2024

AbstractThrough a coordination‐driven self‐assembly method, four
metalla‐links and one tetranuclear monocycle were constructed with high selectivity and yield by adjusting the substituent species of the building blocks, as evidenced using X‐ray crystallographic analysis, electrospray ionization‐time‐of‐flight/mass spectrometry (ESI‐TOF/MS), elemental analysis and detailed solution‐state nuclear magnetic resonance (NMR) spectroscopy. Based on X‐ray crystallographic analysis and independent gradient model analysis, a significant factor leading to the formation of
metalla‐links was the introduction of F, Cl, Br and I atoms, which generated additional weak C−H⋅⋅⋅X (X=F, Cl, Br and I) interactions. Furthermore, the dynamic conversion of
metalla‐links to monocyclic rings in methanol solution was systematically investigated using quantitative 1H NMR techniques.