bluuebunny/crossref_metadata_2025 huggingface dataset:
Concordance of the ACR TI-RADS Classification With Bethesda Scoring and Histopathology Risk Stratification of Thyroid Nodules
Authors: Huang Elaine Y. F. , Kao Nern Hoong , Lin Snow Yunni , Jang Isabelle J. H. , Kiong Kimberley Liqin , See Anna , Venkatanarasimha Nanda , Lee Kristen Alexa , Lim Chwee Ming
Published: September 2023

Importance

Although most thyroid nodules are benign, 10% to 15% of them harbor cancer. Thyroid ultrasonography is useful for risk stratification of nodules, and American College of Radiology Thyroid Imaging Reporting and Data System (ACR TI-RADS) classification provides recommendations for fine-needle aspiration cytology (FNAC) based on objective ultrasonographic features of these nodules.

Objective

To validate the concordance of ACR TI-RADS classification with Bethesda classification and histopathology.

Design, Setting, and Participants

This retrospective cohort study was performed to evaluate the concordance of ACR TI-RADS classification with Bethesda classification and histopathology and was conducted in Singapore General Hospital Outpatient Otolaryngology clinic in March 2021 to May 2021. Data analysis was performed in May 2021.

Main Outcomes and Measures

Results were deemed concordant when ACR TI-RADS recommendations aligned with Bethesda scores. Conversely, results were classified as nonconcordant with Bethesda scores and/or histopathology results when nodules that were recommended for FNAC yielded benign results or nodules that were not recommended for FNAC yielded malignant results.

Results

A total of 446 patients (370 women [83%]; mean [range] age, 60 [24-89] years) who underwent ultrasonography of the thyroid and ultrasonography-guided thyroid FNACs were identified. A total of 492 of 630 nodules (78.1%) were benign on FNAC (Bethesda II). Score 3 ACR TI-RADS nodules yielded the highest negative predictive values: 94.6% (95% CI, 92.9%-95.9%; P < .001) compared with Bethesda scoring and 100.0% (95% CI, 15.8%-100.0%; P = .003) compared with histopathology. Score 4 or 5 ACR TI-RADS nodules yielded positive predictive values of 2.8% and 16.2%, respectively, compared with Bethesda scoring and 6.1% and 66.7%, respectively, compared with histopathology. Small (<1.5 cm) ACR TI-RADS nodules of scores of 4 and 5 that were not recommended for FNAC yielded a malignant risk of 5.7% and 25.0% on Bethesda 5 and 6, respectively. On surgical excision, 5 of 46 (10.9%) ACR TI-RADS 4 nodules and 15 of 21 (71.4%) of ACR TI-RADS 5 nodules were confirmed to be malignant. Among nodules initially not recommended for FNAC, histopathology-proven cancer was found in 4 of 13 (30.7%) and 3 of 6 (50.0%) of nodules, respectively.

Conclusions and Relevance

These findings suggest that ACR TI-RADS score 3 nodules have a low risk of cancer and should be considered for FNAC only if nodules are 2.5 cm or larger. Patients with small (<1.5 cm) ACR TI-RADS 4 and 5 nodules should be appropriately counseled for FNAC to exclude cancer.
Business vs After-Hours Use of an Artificial Intelligence–Powered Digital Health Platform Among Insured Patients
Authors: Graham Sarah A. , Pickus Sarah K. , Lockwood Kimberly G. , Buch Lauren S. , Dunn Patrick , Paruthi Jason
Published: September 2023

This cross-sectional study assesses usage patterns of an AI-powered patient digital health platform.
Limbic network co‐localization predicts pharmacoresistance in dysplasia‐related epilepsy
Authors: Cohen Nathan T. , Chang Phat , Gholipour Taha , Oluigbo Chima , Vezina L. Gilbert , Xie Hua , Zhang Anqing , Gaillard William D.
Published: September 2023

To evaluate the role of focal cortical dysplasia co‐localization to cortical functional networks in the development of pharmacoresistance. One hundred thirty‐six focal cortical dysplasia patients with 3.0 T or 1.5 T MRI were identified from clinical databases at Children's National Hospital. Clinico‐radio‐pathologic factors and network co‐localization were determined. Using binomial logistic regression, limbic network co‐localization (odds ratio 4.164 95% confidence interval 1.02–17.08,p = 0.048), and focal to bilateral tonic–clonic seizures (4.82, 1.30–18.03,p = 0.019) predicted pharmacoresistance. These findings provide clinicians with markers to identify patients with focal cortical dysplasia‐related epilepsy at high risk of developing pharmacoresistance and should facilitate earlier epilepsy surgical evaluation.
Cutting Performance and Wear Behavior of Self‐Developed Silicon Nitride Ceramic End Mills with Optimized Structure for High‐Speed Machining of GH4099
Authors: Sun Hewu , Zou Bin , Xue Kai , Chen Wei , Liu Jikai
Published: September 2023

Ceramic tool materials possess a wide range of potential in machining nickel‐based superalloys due to their superior wear resistance, high‐temperature hardness, and strong chemical stability. Herein, a structural optimization scheme of self‐developed silicon nitride ceramic end mill based on stiffness enhancement and performance improvement is proposed, and the key geometric angular parameters scope of the self‐developed ceramic end mills are prioritized via the finite‐element simulation method. Through precision grinding manufacturing and sandblasting pretreatment, the cutting performance and tool wear behavior of three optimized self‐developed silicon nitride ceramic end mills (called S4‐1, S4‐2, S4‐3 respectively) are comprehensively analyzed in comparison, including cutting force, milling temperature, surface quality, and tool life. The results indicate that the cutting force and cutting temperature of all the optimized ceramic end mills are effectively restrained compared with the nonoptimized ceramic tool(S4), and the final workpiece surface roughness is significantly reduced. Further, better surface quality can be obtained by optimized ceramic mills. In terms of tool life, ceramic end mill with optimized construction in best can be increased by up to 1.9 times. The wear mechanism and pattern of the three optimized ceramic milling tools are similar, which is adhesive wear, diffusion wear, and notch wear. Overall, the effectiveness of the optimization scheme for ceramic end mill is successfully verified.
Highly Malleable Personalized Prostheses with Hierarchical Microstructure Boost the Long‐Term Osteointegration in Irregular Craniofacial Reconstruction
Authors: Liu Quanying , Tong Lei , Chen Manyu , Wang Peilei , Luo En , Liang Jie , Zhang Xingdong , Fan Yujiang , Sun Yong
Published: September 2023

The desired clinical bone prostheses should achieve satisfactory interface integration and osteoinduction, as well as good surgical convenience. Here, a highly malleable 3D printed prosthesis with compressive strength at 13 MPa is constructed by dopamine, polyvinyl alcohol, and micro‐sized hydroxyapatite (86 wt%) as composite bioinks, which is endowed with good plasticity and can quickly match irregular defects by easily trimming. Spatially decorated collagen and hyaluronan greatly enriched the hierarchical microstructure and biological activity of malleable prosthesis. This prosthesis accelerates the proliferation and osteogenic differentiation of stem cells, regulates M2 polarization of macrophage, and promotes endogenous stem cell recruitment and early angiogenesis. Meanwhile, it significantly reinforces biomineralized deposition and vascularization, reaches full coverage of new bone in the rabbit cranial defect after 15 weeks (Φ = 10 mm), and achieves well osseointegration capacity with interfacial binding strength at 71.2% of the natural skull. This osteoinductive prosthesis provides a new design idea for bone filling.
Magnetically Actuated Adhesives with Switchable Adhesion
Authors: Zhao Jinsheng , Lu Taiping , Zhang Yixing , Zhang Chong , Pan Chengfeng , Tan Yu , Zhu Jiaqi , Li Bing , Zhang Li , Shi Mingxing , Li Xiangyu
Published: September 2023

Smart adhesives with the ability to rapidly switch, achieve high adhesion tuning ratios, and provide precise control hold tremendous potential in various fields ranging from micromanipulation to manufacturing. Despite significant progress, an efficient and robust adhesive switch remains a rarity. In this study, a design strategy for magnetically actuated adhesives that exhibit switchable adhesion between high and low levels exceeding 50 times is proposed. The non‐contact actuation of the magnetic field induces a pre‐designed deformation of the magnetic tentacles, resulting in both interface cracks at the adhesion interface and a push force on the target object. Consequently, the pull‐off force can be precisely adjusted according to the strength of the magnetic field. This proposed adhesive also exhibits ultrafast detachment (<1.0 s). Tentative experiments are conducted for transfer‐print technology and on‐demand detachment, which demonstrate the advantages of magnetically actuated adhesives in a non‐contact manner. The proposed strategy of switching adhesion may be particularly useful for practical applications that require highly precise and swiftly controlled movements.
4D Oriented Dynamic Scaffold for Promoting Peripheral Nerve Regeneration and Functional Recovery
Authors: Sun Mouyuan , You Dongqi , Zhan Ning , Liu Chao , Zhang Xiaoting , Lin Lining , Zhang Jingyu , Lou Yiting , Chen Yuewei , Liu Chundi , Wang Huiming , He Yong , Yu Mengfei
Published: September 2023

Neurological function recovery after peripheral nerve injury (PNI) is exceptionally challenging, chiefly because neurons cannot efficiently proliferate, differentiate, and form regenerated axons to pass through the defect region expeditiously and transmit neurological signals. In this study, a four‐dimensional (4D) oriented dynamic scaffold is constructed based on shape memory polymer (SMP), which can regulate spatiotemporally controllable neuronal early adequate proliferation, subsequently effective differentiation and axon formation by synergizing the on‐demand microtopography and deformation force‐based mechanical stimuli (DFMS). This dynamic scaffold can accelerate the restoration of large segmental nerve defects, elevate the neural signaling efficiency by 60% compared with static scaffold, and finally form the functionalized robust regenerating nerve fascicles with comparable therapeutic effects on autologous nerve transplantation. Furthermore, the crucial role of Piezo1/Camk2b modulated neuronal differentiation and axon extension is also revealed through deep transcriptomic analysis. In summary, the 4D oriented dynamic scaffold can precisely and remotely regulate neuronal behavior and fate in a non‐invasive way, which has excellent potential for clinical application in peripheral nerve restoration.
Self‐Smoothing Deposition Behavior Enabled by Beneficial Potential Compensating for Highly Reversible Zn‐Metal Anodes
Authors: Li Jianwen , Zhou Shuang , Chen Yining , Meng Xinyu , Azizi Alireza , He Qiong , Li Hang , Chen Liang , Han Chao , Pan Anqiang
Published: September 2023

Realizing compact dendrite‐free zinc (Zn) plating is crucial to avoiding premature battery failure caused by internal short‐circuits, which is highly determined by the interface electric field (ψi) distribution. Herein, a concept of “potential compensating” is shown on Zn anodes to stimulate its self‐smoothing deposition behavior for durable batteries. A homogeneous ψi with elevated potential intensity is successfully built at the Zn/electrolyte interface via the selective adsorption of highly polarized propylene glycol (PG) molecules, which facilitate the formation of dense and uniform Zn electroplating patterns. Moreover, the PG additive can simultaneously reshape the structure of Zn2+‐solvation sheath and immobilize the H‐bonding networks in bulk electrolyte, enabling Zn anodes with exceptional electrochemical reversibility (99.6%) and ultralong calendar life (3500 h), as revealed by joint spectroscopic and electrochemical analyses. More importantly, full cells with PG safeguard can deliver desirable cycling stability even at an elevated temperature (50 °C) and low N/P ratios (cathode mass loading up to 14.38 mg cm−2). This study presents new insight into the rational design of stable practical electrolytes and interfacial chemistry regulation for sustainable zinc batteries.
Tailoring Lignin‐Derived Porous Carbon Toward High‐Energy Lithium‐Ion Capacitor Through Varying Sp2‐ and Sp3‐Hybridized Bonding
Authors: Peng Qifan , Wang Kai , Gong Yue , Zhang Xudong , Xu Yanan , Ma Yibo , Zhang Xiong , Sun Xianzhong , Ma Yanwei
Published: September 2023

Lignin‐derived porous carbon (LPC) shows great potential as electrode material for supercapacitors. However, precise control over the pore structure during the conventional carbonization–activation process remains challenging. Here, a molecular‐level strategy to tailor the pore structure through tuning inter‐/intra‐molecular bonding of lignin in a pre‐carbonization process is shown. Based on operando pyrolysis analysis, a molecular evolution model is proposed to elucidate the relationship between pre‐carbonization and the resulting porosity of LPC. Lignin undergoes a condensation process with an increase of sp2‐hybridized carbon bonding during pre‐carbonization, causing the extension of polycyclic aromatic structure and leading to an increased mesopore volume in the final porous carbon. The variation in the content ratio of sp2‐ and sp3‐hybridized carbon bonding provides insights into the spatial structure evolution of pre‐carbonized lignin, which correlates well with changes in the porous structure of LPC. The LPCs show ultrahigh specific surface area up to 3219 m2 g−1 and tailored meso‐/micropore distribution. The lithium‐ion capacitor full‐cell tests demonstrate the great potential of LPCs in energy storage applications with superior energy density and power density. This work provides a feasible strategy to precisely design the microstructure of LPC, offering promising prospects for energy storage technologies.
Self‐Assembled Virus‐Like Particle Vaccines via Fluorophilic Interactions Enable Infection Mimicry and Immune Protection
Authors: Xia Yinhe , Liu Kai , Wang Fei , Xu Zhou , Wang Yuesheng , Zong Rongling , Xu Yemin , Li Ping , Deng Bin , Xu Maolei , Chen Gang
Published: September 2023

Influenza epidemics persistently threaten global health. Vaccines based on virus‐like particles (VLPs), which resemble the native conformation of viruses, have emerged as vaccine candidates. However, the production of VLPs via genetic engineering remains constrained by challenges such as low yields, high costs, and being time consuming. In this study, a novel VLP platform is developed that could mimic infection and confer influenza protection through fluorination‐driven self‐assembly. The VLPs closely mimick the key steps in viral infection including dendritic cell (DC) attachment and pH‐responsive endo‐lysosomal escape, which enhances DC maturation and antigen cross‐presentation. It is also observed that the VLPs migrate from the injection site to the draining lymph nodes efficiently. Immunization with VLPs triggers both Th1 and Th2 cellular responses, thereby inducing an improved CD8+ T cell response along with strong antigen‐specific antibody responses. In several infected mouse models, VLP vaccines ameliorate weight loss, lung virus titers, pulmonary pathologies, and confer full protection against H1N1, H6N2, H9N2, and mixed influenza viruses. Therefore, the results support the potential of VLPs as an effective influenza vaccine with improved immune potency against infection. A methodology to generate VLPs based on fluorophilic interactions, which can be a general approach for development of pathogenic VLPs, is reported.
Multifunctional Nanofibrous Scaffolds Capable of Localized Delivery of Theranostic Nanoparticles for Postoperative Cancer Management
Authors: Guo Lin , Zhao Qilong , Zheng Li‐wu , Wang Min
Published: September 2023

Postoperative recovery of cancer patients can be affected by complications, such as tissue dysfunction or disability caused by tissue resection, and also cancer recurrence resulting from residual cancer cells. Despite impressive progress made for tissue engineering scaffolds that assist tissue regeneration for postoperative cancer patients, the majority of existing tissue engineering scaffolds still lack functions for monitoring and killing residual cancer cells, if there are any, upon their detection. In this study, multifunctional scaffolds that comprise biodegradable nanofibers and core–shell structured microspheres encapsulated with theranostic nanoparticles (NPs) are developed. The multifunctional scaffolds possess an extracellular matrix‐like nanofibrous architecture and soft tissue‐like mechanical properties, making them excellent tissue engineering patch candidates for assisting in the repair and regeneration of tissues at the cancerous sites after surgery. Furthermore, they are capable of localized delivery of theranostic NPs upon quick degradation of core–shell structured microspheres that contain theranostic NPs. Leveraging on folic acid‐mediated ligand‐receptor binding, surface‐enhanced Raman scattering activity, and near‐infrared‐responsive photothermal effect of the theranostic gold NPs (AuNPs) delivered locally, the multifunctional scaffolds display excellent active targeting, diagnosis, and photothermal therapy functions for cancer cells, showing great promise for adaptive postoperative cancer management.
Scalable Electrodeposition of Liquid Metal from an Acetonitrile‐Based Electrolyte for Highly Integrated Stretchable Electronics
Authors: Monnens Wouter , Zhang Bokai , Zhou Zhenyu , Snels Laurens , Binnemans Koen , Molina‐Lopez Francisco , Fransaer Jan
Published: September 2023

The advancement of highly integrated stretchable electronics requires the development of scalable sub‐micrometer conductor patterning. Eutectic gallium indium (EGaIn) is an attractive conductor for stretchable electronics, as its liquid metallic character grants it high electrical conductivity upon deformation. However, its high surface tension makes its patterning with sub‐micrometer resolution challenging. In this work, this limitation is overcome by way of the electrodeposition of EGaIn. A non‐aqueous acetonitrile‐based electrolyte that exhibits high electrochemical stability and chemical orthogonality is used. The electrodeposited material leads to low‐resistance lines that remain stable upon (repeated) stretching to a 100% strain. Because electrodeposition benefits from the resolution of mature nanofabrication methods used to pattern the base metal, the proposed “bottom‐up” approach achieves a record‐high density integration of EGaIn regular lines of 300 nm half‐pitch on an elastomer substrate by plating on a gold seed layer prepatterned by nanoimprinting. Moreover, vertical integration is enabled by filling high‐aspect‐ratio vias. This capability is conceptualized by the fabrication of an omnidirectionally stretchable 3D electronic circuit, and demonstrates a soft‐electronic analog of the stablished damascene process used to fabricate microchip interconnects. Overall, this work proposes a simple route to address the challenge of metallization in highly integrated (3D) stretchable electronics.
Near‐Infrared Light‐Driven Photocatalysis with an Emphasis on Two‐Photon Excitation: Concepts, Materials, and Applications
Authors: Han Chuang , Kundu Bidyut Kumar , Liang Yujun , Sun Yujie
Published: September 2023

Efficient utilization of sunlight in photocatalysis is widely recognized as a promising solution for addressing the growing energy demand and environmental issues resulting from fossil fuel consumption. Recently, there have been significant developments in various near‐infrared (NIR) light‐harvesting systems for artificial photosynthesis and photocatalytic environmental remediation. This review provides an overview of the most recent advancements in the utilization of NIR light through the creation of novel nanostructured materials and molecular photosensitizers, as well as modulating strategies to enhance the photocatalytic processes. A special focus is given to the emerging two‐photon excitation NIR photocatalysis. The unique features and limitations of different systems are critically evaluated. In particular, it highlights the advantages of utilizing NIR light and two‐photon excitation compared to UV–visible irradiation and one‐photon excitation. Ongoing challenges and potential solutions for the future exploration of NIR light‐responsive materials are also discussed.
When JV Curves Conceal Material Improvements: The Relevance of Photoluminescence Measurements in the Optimization of Perovskite Solar Cells
Authors: Dreessen Chris , Zanoni Kassio P. S. , Gil‐Escrig Lidón , Rodkey Nathan , Khan Jafar I. , Laquai Frédéric , Sessolo Michele , Roldán‐Carmona Cristina , Bolink Henk J.
Published: September 2023

Lead halide perovskites have prompted great interest, offering impressive photovoltaic performances. Most fundamental investigations and cell optimizations focus on solution‐based solar cells, which are not easily extended to larger scales. Commonly in these cells, losses in the open‐circuit voltage are attributed to arise primarily from interface recombination, and therefore the most studies have focused on optimization of the surface to eliminate defects states. In contrast, thermal evaporation is an alternative, solvent‐free, and scalable method to deposit lead halide perovskites that is gaining attention. However, the number of reports showing high‐efficiency solar cells (> 20%) prepared using thermal evaporation is still small. Here, the origins of non‐radiative charge carrier recombination are investigated in perovskite cells that are deposited via thermal co‐evaporation. This is done through a combination of photoluminescence spectroscopy, current‐voltage characterization, and simulations. It is found that the non‐radiative recombination in these cells is caused equally by bulk and interface defects. In general, it is advocated to perform a dual analysis of the photoluminescence spectroscopy of both the film and the photovoltaic device, in conjunction with current‐voltage measurements. It is emphasized that such a dual analysis is needed to enable the identification of improvements and to unlock further advancements in this technology.
High‐Efficient Blue Emission and Bandgap Engineering from Jahn–Teller Distorted Halide Double Perovskites
Authors: Liu Yan , Dai Xing , Zeng Xuelian , Yuan Xianrong , Wang Yanan , Song Yuhang , Chen Haoyu , Zhang Chao , Wang Yong , Wan Li , Zou Yatao , Ning Weihua , Sun Baoquan
Published: September 2023

Decreasing the power consumption of light‐emitting diodes (LEDs) and increasing the energy generation of solar cells are crucial tasks toward the mitigation of greenhouse gas emissions and Paris Agreement goals. Lead (Pb)‐free halide double perovskites, identified as environmentally friendly alternatives to Pb‐based perovskites, are not deemed useful thus far due to the absence of high photoluminescence quantum yield (PLQY) examples and large bandgaps. Herein, penta‐cationic antimony (Sb5+)‐doping strategy is demonstrated for the benchmark material of Cs2NaInCl6, achieving blue emission with near‐unity PLQY and the lowest bandgap of 1.24 eV. The excellent PLQY observed in the material is attributed to Sb5+ doping‐induced Jahn–Teller distortion in Cs2NaInCl6 and a newly emerged band structure, which has remained undisclosed in all previous reports. This groundbreaking discovery represents the first instance in the field of perovskite materials where the incorporation of a single dopant has resulted in a zero‐to‐one enhancement in their emission profile. This breakthrough is expected to have profound implications for advancing research in the utilization of similar dopants, such as manganese cations (Mn6+ and Mn7+), not only in halide perovskite structures but also in oxide‐based perovskites and other semiconductor systems.
Alkylidene Meldrum′s Acid as Acceptor‐Donor‐Acceptor with Azomethine Ylide for Organocatalytic Asymmetric (3+2) Cycloaddition/Annulation: Synthesis of Chromeno[4,3‐b]pyrrolidine
Authors: Liou Yan‐Cheng , Chen Yi‐Ru , Hsu Ching‐Wen , Huang Xuan‐Rui , Wang Heng‐Wei , Lin Wenwei
Published: September 2023

A quinine‐derived thiourea‐catalyzed enantioselective double annulation strategy using alkylidene Meldrum′s acid as an acceptor‐donor‐acceptor with salicylaldehyde‐derived azomethine ylide is reported. The methodology is realized via a (3+2) cycloaddition/transesterification/decarboxylation sequence, giving chromeno[4,3‐b]pyrrolidines within 15–420 minutes at room temperature in 51–97% yields with 92–99% ee under 1–10 mol% catalyst loading. A plausible activation model is proposed for the excellent stereoinduction by H‐bond interaction between the catalyst and the Meldrum′s acid motif according to control experiments.
Nonaqueous Liquid Electrolytes for Sodium‐Ion Batteries: Fundamentals, Progress and Perspectives
Authors: Li Chuanchuan , Xu Hongyue , Ni Ling , Qin Bingsheng , Ma Yinglei , Jiang Hongzhu , Xu Gaojie , Zhao Jingwen , Cui Guanglei
Published: September 2023

Sodium‐ion batteries (SIBs), driven by sustainability and cost advantage, have been recognized as one of the most promising electrochemical energy storage devices. Electrolytes, as the most unique component that not only ionically connect while insulating electronically electrodes but also determine the eventual improvements in performance mainly regarding cycle life, Coulombic efficiency, energy density, and safety, hold the key to the practical implementation of SIBs. In this review, the fundamental design principles of Na+‐ion electrolytes and the chemical properties of the Na+ cation over the Li+ cation in terms of ion transport, salt dissolution, and solvation structure are first discussed. Then, a sequence of crucial experimental discoveries and strategical achievements in the field of electrolytes for SIBs are presented, with focuses on the ether‐based electrolytes for co‐intercalation into graphite, diluted and highly concentrated electrolytes, wide temperature range electrolytes, nonflammable electrolytes, indispensable electrolyte components (functional additives and new sodium salts). Finally, a detailed analysis of research trends of practically feasible Na+‐ion electrolytes is presented to aid in the ongoing quest for better SIBs of the future.
Kontrolle der Reduzierbarkeit von Metalloxiden zur effizienten Aktivierung von C−H‐Bindungen in Kohlenwasserstoffen
Authors: Yang Guo‐Qing , Niu Yiming , Kondratenko Vita A. , Yi Xianfeng , Liu Chang , Zhang Bingsen , Kondratenko Evgenii V. , Liu Zhong‐Wen
Published: September 2023

Die Kenntnis der Struktur katalytisch aktiver Spezies/Phasen und die Bereitstellung von Methoden zu ihrer gezielten Herstellung sind zwei Voraussetzungen für die Entwicklung von Katalysatoren mit der gewünschten Performance. Hierin stellen wir eine einfache Methode zur präzisen Herstellung von Träger‐/Vollkatalysatoren vor. Diese Methode nutzt die Eigenschaft von Metalloxiden, bei Behandlung in wässrigen Ammoniaklösungen lösbar zu sein und gleichzeitig ausgefällt werden zu können. Bei Anwendung dieser Methode auf einen herkömmlichen VOx−Al2O3‐Katalysator wurde die Konzentration koordinativ ungesättigter Al‐Zentren einfach durch Änderung des pH‐Werts der Lösung eingestellt. Diese Stellen beeinflussen die Stärke der V−O−Al‐Bindungen isolierter VOx‐Spezies und damit deren Reduzierbarkeit. Diese Methode ist auch zur Steuerung der Reduzierbarkeit von Vollkatalysatoren anwendbar, wie am Beispiel eines CeO2−ZrO2−Al2O3‐Systems gezeigt wurde. Die Einsetzbarkeit der entwickelten Katalysatoren wurde in der oxidativen Dehydrierung von Ethylbenzol zu Styrol mit CO2und in der nichtoxidativen Propandehydrierung zu Propen bestätigt. Unser Ansatz lässt sich auf die Herstellung beliebiger Metalloxidkatalysatoren, die in einer Ammoniaklösung löslich sind, ausweiten.
Stereoselective Photoredox Catalyzed (3+3) Dipolar Cycloaddition of Nitrone with Aryl Cyclopropane
Authors: Xu Yao , Gao Hai‐Xiang , Pan Chengkai , Shi Yue , Zhang Chi , Huang Genping , Feng Chao
Published: September 2023

By resorting to the principle of remote activation, we herein demonstrate the first photoredox catalyzed (3+3) dipolar cycloaddition of nitrones with aryl cyclopropanes. Key to the fidelity of the reaction resides in a facile manner of substrate activation by single‐electron transfer (SET) oxidation with photoredox catalysis, and the reaction takes place through a stepwise cascade encompassing a three‐electron‐type nucleophilic substitution triggered cyclopropane ring‐opening and a diastereoselective 6‐endo‐trig radical cyclization manifold. The reaction proceeds under mild conditions with excellent regio‐ and stereoselectivity, nicely complementing the well‐developed Lewis acid catalyzed cycloaddition of donor‐acceptor cyclopropanes. Other merits of the protocol include wide scope of aryl cyclopropanes with diversified substitution patterns and good functional‐group compatibility. A mechanism involving an aryl radical cation promoted remote activation mode was also proposed and supported by mechanistic experiments.
Modular and Practical 1,2‐Aryl(Alkenyl) Heteroatom Functionalization of Alkenes through Iron/Photoredox Dual Catalysis**
Authors: Zhang Weigang , Liu Tao , Ang Hwee Ting , Luo Penghao , Lei Zhexuan , Luo Xiaohua , Koh Ming Joo , Wu Jie
Published: September 2023

Efficient methods for synthesizing 1,2‐aryl(alkenyl) heteroatomic cores, encompassing heteroatoms such as nitrogen, oxygen, sulfur, and halogens, are of significant importance in medicinal chemistry and pharmaceutical research. In this study, we present a mild, versatile and practical photoredox/iron dual catalytic system that enables access to highly privileged 1,2‐aryl(alkenyl) heteroatomic pharmacophores with exceptional efficiency and site selectivity. Our approach exhibits an extensive scope, allowing for the direct utilization of a wide range of commodity or commercially available (hetero)arenes as well as activated and unactivated alkenes with diverse functional groups, drug scaffolds, and natural product motifs as substrates. By merging iron catalysis with the photoredox cycle, a vast array of alkene 1,2‐aryl(alkenyl) functionalization products that incorporate a neighboring azido, amino, halo, thiocyano and nitrooxy group were secured. The scalability and ability to rapid synthesize numerous bioactive small molecules from readily available starting materials highlight the utility of this protocol.
Evading the Illusions: Identification of False Peaks in Micro‐Raman Spectroscopy and Guidelines for Scientific Best Practice
Authors: Thyr Jakob , Edvinsson Tomas
Published: September 2023

Micro‐Raman spectroscopy is an important analytical tool in a large variety of science disciplines. The technique is suitable for both identification of chemical bonds and studying more detailed phenomena like molecular interactions, material strain, crystallinity, defects, and bond formations. Raman scattering has one major weakness however: it is a very low probability process. The weak signals require very sensitive detection systems, which leads to a high probability of picking up signals from origins other than the sample. This complicates the analysis of the results and increases the risk of misinterpreting data. This work provides an overview of the sources of spurious signals occurring in Raman spectra, including photoluminescence, cosmic rays, stray light, artefacts caused by spectrometer components, and signals from other compounds in or surrounding the sample. The origins of these false Raman peaks are explained and means to identify and counteract them are provided.
Alleviating the loss: A conical fish screen installation reduces native fish entrainment at a gravity‐fed water diversion
Authors: Bretzel Joachim B. , Boys Craig A. , Watts Robyn J. , Doyle Katherine E. , Baumgartner Lee J.
Published: September 2023

Each year, millions of fish are extracted from Australian waterways by the pumping and diversion of water into irrigation systems. Fish protection screens can help reduce these losses but are largely untested in Australian rivers.

In this study, a large, gravity‐fed irrigation offtake on Gunbower Creek, Victoria, Australia, was investigated for fish and debris entrainment. Experiments were performed under screened and unscreened conditions across various river flows.

Mark–release–recapture experiments were undertaken with fingerlings of two recreationally significant fish species, Murray cod (Maccullochella peelii) and golden perch (Macquaria ambigua), together with wild fish community assessments, to determine how effective the screen was at reducing fish entrainment into the irrigation channel.

The mean percentage of recaptured fingerlings was significantly lower when the irrigation channel offtake was screened compared with unscreened. Entrainment of released fish into the irrigation channel was reduced by >98%.

Similarly, wild fish entrainment was significantly lower when the irrigation channel was screened. When screened, fewer wild species dominated the sampled fish community, and entrained fish were generally <40 mm in length.

Debris loads decreased significantly in the irrigation channel owing to the screen, indicating the economic benefits of fish screens.

Implementing screens could aid in native fish conservation efforts in riverine environments.
The clinical anatomy fellowship: A participants' perspective
Authors: Thiel Grace E. , Murtha Celeste M. , Dennis Jennifer F. , Hopper Mari
Published: September 2023

Kansas City University offers a Clinical Anatomy Fellowship which enrolls nine medical students during each academic year and provides training in research, teaching, and advanced anatomical topics. The Fellows practice as novice educators, working alongside Anatomy faculty to teach medical students in the Gross Anatomy laboratory. However, little has been reported related to Fellowship participation and success outcomes. This survey‐based study was designed to explore (1) student motivation(s) for pursuing the Fellowship, (2) benefits of participation, and (3) the perceived impact on residency applications and career success. Three unique populations were surveyed. The most important factors driving application to the Fellowship were a desire to increase competitiveness in the residency application process (Likert mean score 4.7–5.0) and a passion for Anatomy (Likert mean score 4.3–4.7). Taking a year away from the College of Osteopathic Medicine curriculum (Likert mean score 4.4) and delaying clinical exposure (Likert mean score 4.2) were the most important deterrents to application. The most reported benefits after program completion included opportunities to build a strong residency application (44% and 50% of Fellows), conduct research (44% and 45% of Fellows), and participate in teaching (11% and 50% of Fellows). 73% of past Fellows matched into their top specialty of choice. Flexibility in the program allows participants to individualize their Fellowship experience to address their personal goals related to residency applications and careers as future physicians. As the results suggest, the Clinical Anatomy Fellowship benefits Fellows, signaling other medical institutions to consider adopting a similar program.
Optimization of herbaceous feedstock delivery to a network of supply depots for a biorefinery in the Piedmont, USA
Authors: Resop Jonathan P. , Cundiff John S.
Published: September 2023

The southeastern USA has the potential to be a significant producer of bio‐based products; however, research is still needed to demonstrate the most cost‐effective feedstock delivery system for this region. A logistic system that has shown promise is one utilizing a network of supply depots. This study calculated the cost to produce a stream of size‐reduced herbaceous biomass (i.e., switchgrass) for five theoretical depots in the Piedmont province. Three depots were located in south central Virginia and two in north central North Carolina. A logistics system with a 20‐bale handling unit was used for load‐out operations at 199 theoretical satellite storage locations (SSLs) within a 48 km radius of each depot location. The distribution of potential production fields and the transportation distance from SSLs to the depots were determined with spatial and network analyses. Based on an analysis of potential land cover available for feedstock production, the annual capacity per depot ranged from 80 839 to 170 830 Mg, resulting in a total annual capacity of 555 195 Mg for all five depots. Cost to deliver feedstock for 24/7 operation, 48 weeks per year ranged from 46.03 to 62.86 USD Mg−1 annual capacity. At the low end, these costs were: SSL operation (22%), truck (29%), receiving facility (26%), and debaling‐size‐reduction (23%). The principle economy‐of‐scale factors were the receiving facility and debaling‐size‐reduction costs. To minimize per‐Mg cost, depot capacity should be chosen such that equipment can be operated as close to 80% of design capacity as possible.
Facile prepared microfluidic chip for multiplexed digital RT‐qPCR test
Authors: Hu Wenqi , Zhu Yidan , Tang Qu , Ji Xiaolei , Wang Lei , Ou Weijun , Li Guo , Wu Li , Cong Hui , Qin Yuling
Published: September 2023

The chip‐based digital polymerase chain reaction (PCR) is an indispensable technique for amplifying and quantifying nucleic acids, which has been widely employed in molecular diagnostics at both fundamental and clinical levels. However, the previous designs have yet to achieve widespread application due to limitations in complex chip fabrication, pretreatment procedures, special surface properties, and low throughput. This study presents a facile digital microfluidic chip driven by centrifugal force for digital PCR analysis. Interestingly, regardless of the hydrophilicity or hydrophobicity of the inner chip surface, an efficient digitization process can be achieved. PCR reagents introduced into the inlet can be allocated to 9600 microchambers and subsequently isolated by the immiscible phase (silicone oil). The centrifugal priming approach offers a facile means to achieve high‐throughput analysis. The design was further employed for the quantification of nucleic acids using digital PCR. The calculated result exhibited a strong correlation with the measured value at the concentrations from 1 copy/μL to 1000 copies/μL (R2 = 0.99). Additionally, the chip also allowed digital multiplexed analysis, thereby indicating its potential for multi‐target detection applications.
Production and characterization of a chimeric protein targeting synuclein epitopes for immunotherapy against synucleinopathies
Authors: Carreño‐Campos Christian , Govea‐Alonso Dania O. , Villarreal Maria Luisa , Caltempa Anabel O. , Gonzalez‐Ortega Omar , Rosales‐Mendoza Sergio
Published: September 2023

The aggregation and spread of alpha‐synuclein (αSyn) is associated with several pathogenic pathways that lead to neurodegeneration and, ultimately, to synucleinopathies development. Hence, the establishment of a safe and effective disease‐modifying therapy that limits or prevents the spread of toxic αSyn aggregation could lead to positive clinical outcomes. A rational vaccine design can be focused on the selection of specific epitopes able to induce the immune response desired, for example, antibodies able to mediate the clearance of αSyn aggregates without the induction of inflammatory responses. To develop a rapid system for the evaluation of a vaccine candidate against synucleinopathies, rLTB‐Syn (an antigen based on three B cell epitopes from αSyn and the B subunit of the heat‐labile Escherichia coli enterotoxin [LTB] as adjuvant/carrier) was produced using recombinant E. coli (Rosetta DE3) as the expression host. The bacterial version of rLTB‐Syn was produced as soluble protein at yields up to 1.72 mg/g biomass. A method for the purification of rLTB‐Syn (~18 kDa) was developed based on ion exchange chromatography, reaching purity >93% with a final concentration of 82.6 μg/mL. Furthermore, the purified soluble rLTB‐Syn retained GM1 binding activity, suggesting proper folding and pentameric structure. The results from this study establish a fast and effective method to obtain rLTB‐Syn, making it useful in the design of novel vaccine formulations targeting synucleinopathies.
Preparation of Trimetallic‐Organic Framework Film Electrodes via Secondary Growth for Efficient Oxygen Evolution Reaction
Authors: Li Shulin , Wang Zixiong , Wang Tienan , Yang Yuting , Xiao Yang , Tian Yuyang , Zhu He , Jing Xiaofei , Zhu Guangshan
Published: September 2023

Metal–organic frameworks (MOFs) are promising electrocatalysts for clean energy conversion systems. However, developing MOF‐based electrodes with high performance toward oxygen evolution reaction (OER) is still challenging. In this work, a series of MOF film electrodes derived from Ni‐btz were prepared by employing the secondary growth strategy under solvothermal conditions. Fe and Co ions were also incorporated into the Ni‐btz framework to produce a trimetallic coupling effect to obtain enhanced OER activity. The as‐prepared FeCoNi‐btz/NF exhibited not only good stability but also excellent OER performance under alkaline conditions. Furthermore, the possible intermediates including metal oxides and metal oxyhydroxides were confirmed by X‐ray photoelectron spectroscopy (XPS) and transmission electron microscopy (TEM).
Cycloaddition–Retro‐Electrocyclization Click Reaction of Amine End‐Capped Oligoynes with Tetracyanoethylene
Authors: Pigulski Bartłomiej , Misiak Klaudia , Męcik Patrycja , Szafert Sławomir
Published: September 2023

This study shows the first example of cycloaddition–retro‐electrocyclization (CA‐RE) click reaction involving nitrogen end‐capped push‐pull oligoynes. The reported CA‐RE reaction with TCNE (tetracyanoethylene) is fully regioselective and leads exclusively to the unprecedented TCBD (tetracyanobuta‐1,3‐diene‐2,3‐diyl) end‐capped carbon rods. The molecular structure of the products was unambiguously confirmed using X‐ray single crystal diffraction and their optical and electronic properties were investigated experimentally and rationalized using DFT (density functional theory) calculations.
An investigation of drum granulation of post‐pyrolysis washed biochar
Authors: Fazzalari Anthony , Briens Cedric , Tribe Lauren
Published: September 2023

Biochar, unwashed and washed with a solution of Triton and hydrogen peroxide, was wet drum granulated using molasses binder solutions. Unwashed biochar was very hydrophobic and granulation proceeded through forming liquid marbles and layering. Washing reduced the hydrophobicity of the biochar. The effectiveness of the wash depended on the biochar source; it significantly reduced the hydrophobicity of biochar from woodchips and moderately reduced the hydrophobicity of biochar from flower digestate. Therefore, washed biochar from woodchips was granulated using a hydrophilic mechanism, while washed biochar from digestate was granulated according to a combination mechanism of liquid marbles collapsing and then coalescing. The change in granulation mechanism produced stronger and denser granules with higher yields of granules in the 1–4 mm optimal size range. Washing and then granulating biochar created a product that could be further tailored for optimal soil amendment.
Dcalycinumines A—E, Alkaloids with Cytotoxic Activities of Nasopharyngeal Carcinoma Cells from Daphniphyllum calycinum
Authors: Tang Qing , Dai Xiao‐Yong , Lin Qiang , Ling Zhi‐Peng , Hao Yi‐Kun , Zhu Tian‐Xi , Zhang Ji‐Hui , Hou Yi‐Bo , Li Yao‐Lan , Huang Lai‐Qiang , Wang Jing‐Hao , Wang Guo‐Cai , Zhang Yu‐Bo
Published: September 2023

Comprehensive Summary

Five novel Daphniphyllum alkaloids, named dcalycinumines A—E (1—4, 6), and eight previously described Daphniphyllum alkaloids (5, 7—13) were isolated from Daphniphyllum calycinum. Compound 1 is the first Daphniphyllum alkaloid possessing a highly rearranged 6/6/6/7/5/6 hexacyclic architecture with a unique 3‐methyl‐1‐azabicyclo [4,4,0] decane ring system. Compound 2 represents a rare diamino Daphniphyllum alkaloid with an unprecedented 6/5/5/6/6/5 carbon skeleton featuring a unique 1‐aza‐6‐azaspiro [4,5] decane unit, whereas 3 also represents a rare diamino Daphniphyllum alkaloid as a possible precursor of 2. Compound 4 is the second example of C‐22‐nor yuzurimine‐type alkaloids. Their structures and absolute configurations were elucidated by HRESIMS, NMR spectroscopic analyses, ECD calculations, and single‐crystal X‐ray diffraction. Moreover, compound 1 showed remarkable antitumor activities, which could inhibit the proliferation, migration and invasion of nasopharyngeal carcinoma cells, and promoted nasopharyngeal carcinoma cells apoptosis.
Is Gulf War Illness a prolonged early phase tauopathy?
Authors: Baas Peter W. , Sullivan Kimberly A. , Terry Alvin V. , Case Kendra , Yates Philip L. , Sun Xiaohuan , Raghupathi Ramesh , Huber Bertrand R. , Qiang Liang
Published: September 2023

The work of the Gulf War Illness (GWI) Consortium and that of basic and clinical researchers across the USA have resulted in a better understanding in recent years of the pathological basis of GWI, as well as of the mechanisms underlying the disorder. Among the most concerning symptoms suffered by veterans with GWI are cognitive decrements including those related to memory functioning. These decrements are not severe enough to meet dementia criteria, but there is significant concern that the mild cognitive impairment of these veterans will progress to dementia as they become older. Recent studies on GWI using human brain organoids as well as a rat model suggest that one potential cause of the cognitive problems may be elevated levels of tau in the brain, and this is supported by high levels of tau autoantibodies in the blood of veterans with GWI. There is urgency in finding treatments and preventive strategies for these veterans before they progress to dementia, with added value in doing so because their current status may represent an early phase of tauopathy common to many neurodegenerative diseases.
Conceptualizing multiplicity spectrum experiences: A systematic review and thematic synthesis
Authors: Eve Zarah , Heyes Kim , Parry Sarah
Published: September 2023

Background

Dissociative identity disorder and depersonalization–derealization have attracted research and clinical interest, facilitating greater understanding. However, little is known about the experience of multiplicity of self outside of traumagenic or illness constructs. Consequently, this systematic review explored how people identifying as having multiple selves conceptualize their experiences and identity.

Methods

A comprehensive search of qualitative studies reporting lived experiences of multiplicity was conducted through PsycINFO, PubMed and Scopus (PROSPERO ID: CRD42021258555). Thirteen relevant studies were retrieved (N = 98, 16–64 years, conducted in the United Kingdom, the United States, Hungary and Poland).

Results

Using line‐by‐line thematic synthesis, four analytical themes were developed: multiplicity: disorder versus experience; impact of understanding multiplicity; importance of supporting multiplicity; and continuum of experiences.

Discussion

This review highlights heterogeneity within multiplicity‐spectrum experiences, emphasizing the need for person‐centred, individualized understanding, separate from mental health conceptualizations. Therefore, training in person‐centred individualized care to promote self‐concept clarity is needed across health, education and social care. This systematic review is the first to synthesize voices of people with lived experience across the multiplicity spectrum, demonstrating how qualitative research can contribute to advancing our understanding of this complex phenomena with the community, acknowledging reciprocal psychosocial impacts of multiplicity and providing valuable recommendations for services.