bluuebunny/crossref_metadata_2025_split huggingface dataset:
Chirality‐Induced Spin Selectivity Enables New Breakthrough in Electrochemical and Photoelectrochemical Reactions
Authors: Ma Sunihl , Lee Hyungsoo , Moon Jooho 
Published: July 2024

AbstractTo facilitate the transition from a carbon‐energy‐dependent society to a sustainable society, conventional engineering strategies, which encounter limitations associated with intrinsic material properties, should undergo the paradigm shift. From a theoretical viewpoint, the spin‐dependent feature of oxygen evolution reaction (OER) reveals the potential of a spin‐polarization strategy in enhancing the performance of electrochemical (EC) reactions. The chirality‐induced spin selectivity (CISS) phenomenon attracts unprecedented attention owing to its potential utility in achieving novel breakthroughs. This paper starts with the experimental results aimed at enhancing the efficiency of the spin‐dependent OER focusing on the EC system based on the CISS phenomenon. The applicability of spin‐polarization to EC system is verified through various analytical methodologies to clarify the theoretical groundwork and mechanisms underlying the spin‐dependent reaction pathway. The discussion is then extended to effective spin‐control strategies in photoelectrochemical system based on the CISS effect. Exploring the influence of spin‐state control on the kinetic and thermodynamic aspects, this perspective also discusses the effect of spin polarization induced by the CISS phenomenon on spin‐dependent OER. Lastly, future directions for enhancing the performance of spin‐dependent redox systems are discussed, including expansion to various chemical reactions and the development of materials with spin‐control capabilities.
Antibacterial Activity of Visible Light Responsive‐Silver‐Nanoparticle/Titania Composite Thin Films with Unprecedently Higher Amounts of Silver
Authors: Daniel Likius S. , Joseph Moses T. , Uahengo Veikko , Hedimbi Marius 
Published: July 2024

AbstractTo study the antibacterial efficacy of metallic Ag nanoparticle/titania (Ag‐NP)/TiO2 composite thin films against Escherichia coli (ATCC 25922), COMP‐Agn with various amounts of Ag (10 mol% ≤ n ≤ 80 mol%) are fabricated on a quartz glass substrate at 600 °C using the molecular precursor method. The films are characterized by X‐ray diffraction, X‐ray photoelectron, scanning electron microscopy, transmission electron microscopy, photoluminescence, and UVvis techniques. The analysis reveals that the films are composed of metallic Ag‐NPs embedded in a mixture of anatase and rutile matrix, with a volumetric fraction of Ag ranging from 0.18 to 0.68. The antibacterial activity of the TiO2 thin film and COMP‐Agn are determined by disk diffusion and viable cell count methods. Neither pure TiO2 nor pure Ag films exhibit any discernible antibacterial under dark and visible light. The antibacterial of Ag content in composite films is observed to persist for a maximum increase of 70%. The model is proposed on the basis of photoexcited electron transfer from Ag NPs to the TiO2 conduction band of COMP‐Agn, which clarifies the main factors affecting the photoresponse and the excellent response to visible light via surface plasmon resonance.
Strategies to Realize AC Electrokinetic Enhanced Mass‐Transfer in Silicon Based Photonic Biosensors.
Authors: Henriksson Anders , Neubauer Peter , Birkholz Mario 
Published: July 2024

AbstractSilicon‐on‐insulator (SOI) based photonic sensors, particularly those utilizing Photonic Integrated Circuit (PIC) technology, have emerged as promising candidates for miniaturized bioanalytical devices. These sensors offer real‐time responses, occupy minimal space, possess high sensitivity, and facilitate label‐free detection. However, like many biosensors, they face challenges when detecting analytes at exceedingly low concentrations due to limitations in mass transport. An intriguing method to enhance mass transfer in microfluidic biosensors is AC electrokinetics. Proof‐of‐concept experiments have demonstrated significant enhancements in limit of detection (LOD) and response times. AC electrokinetics, compatible with silicon photonic sensors, offers techniques such as electroosmosis, electrothermal effects, and dielectrophoresis to modify fluid flow and manipulate particle trajections. This article delves into various approaches for integrating AC electrokinetics into silicon photonic biosensors, shedding light on both its advantages and limitations.
Functionalized α‐Fluorinated Amines from Imines and Enol Ethers
Authors: Kyrko Dimitra , Saraç Murat , Hao Jing , Retailleau Pascal , Ongeri Sandrine , Crousse Benoît 
Published: July 2024

AbstractWe report the addition reaction of lithium enol ethers to fluoroalkyl imines. A range of different fluoroalkyls and lithiated reagents are well tolerated. Diastereoselective addition of lithium vinyl ethers to fluoroalkyl N‐tert‐butylsulfinylimines is disclosed, providing enantiomerically enriched α‐fluorinated amines in up to 98% yield. This general approach led to the diastereoselective formation of various amino alcohols and amino ethers, which are difficult to obtain by other methods.
Electrochemically Induced Desulfurization of Thioureas for the Synthesis of Substituted 5‐Aminotetrazoles
Authors: Yu Xiao , Hao Liqiang , Liu Xian , Jin Shengkui , Liu Yiping , Ji Yafei 
Published: July 2024

AbstractA one‐pot method has been developed for synthesizing diverse substituted 5‐aminotetrazoles via the electrochemically induced desulfurizative addition–cyclization of thioureas with azidotrimethylsilane. This methodology enables the construction of C−N and N−N bonds under mild reaction conditions without transition metal catalysts or external oxidizing agents. The applicability of this approach is demonstrated by its broad substrate scope, compatibility with various functional groups, scalability to gram‐scale synthesis, and practicality evidenced by the synthesis of an antibacterial agent.
1‐Oxa‐2,6‐Diazaspiro[3.3]heptane as a New Potential Piperazine Bioisostere – Flow‐Assisted Preparation and Derivatisation by Strain‐Release of Azabicyclo[1.1.0]butanes
Authors: Graziano Elena , Natho Philipp , Andresini Michael , Mastrolorito Fabrizio , Mahdi Iktedar , Mesto Ernesto , Colella Marco , Degennaro Leonardo , Nicolotti Orazio , Luisi Renzo 
Published: July 2024

AbstractThe development of novel strained spiro heterocycles (SSHs) as bioisosteres for aromatic or non‐strained aliphatic rings is highly sought after for improving drug design. Their high molecular rigidity and predictable vectorization can enhance drug‐likeness, target selectivity and clinical success. Towards this goal, 1‐oxa‐2,6‐diazaspiro[3.3]heptane (ODASE) is reported as a novel potential SSH‐bioisostere. We demonstrate through theoretical studies the potential of this strained spiro heterocycle to act as a bioisostere for piperazine. We have developed its synthesis from the highly strained azabicyclo[1.1.0]butyl intermediate through a robust and mild flow technology‐assisted two‐step protocol. Its tolerance and stability towards medicinally relevant N‐functionalisation protocols are studied, as well as its mild reduction to the C3‐aminoalkylazetidinol motif found in the anti‐cancer drug cobimetinib.
Dendritic Cell‐Hitchhiking In Vivo for Vaccine Delivery to Lymph Nodes
Authors: Zhou Lei , Zhao Ling , Wang Mengyao , Qi Xu , Zhang Xin , Song Qingying , Xue Dayu , Mao Meihua , Zhang Zhenzhong , Shi Jinjin , Si Pilei , Liu Junjie 
Published: July 2024

AbstractTherapeutic cancer vaccines are among the first FDA‐approved cancer immunotherapies. Among them, it remains a major challenge to achieve robust lymph‐node (LN) accumulation. However, delivering cargo into LN is difficult owing to the unique structure of the lymphatics, and clinical responses have been largely disappointing. Herein, inspired by the Migrated‐DCs homing from the periphery to the LNs, an injectable hydrogel‐based polypeptide vaccine system is described for enhancing immunostimulatory efficacy, which could form a local niche of vaccine “hitchhiking” on DCs. The OVA peptide modified by lipophilic DSPE domains in the hydrogel is spontaneously inserted into the cell membrane to achieve “antigen anchoring” on DCs in vivo. Overall, OVA peptide achieves active access LNs through recruiting and “hitchhiking” subcutaneous Migrated‐DCs. Remarkably, it is demonstrated that the composite hydrogel enhances LNs targeting efficacy by approximately six‐fold compared to free OVA peptide. Then, OVA peptide can be removed from the cell surface under a typical acidic microenvironment within the LNs, further share them with LN‐resident APCs via the “One‐to‐Many” strategy (One Migrated‐DC corresponding to Many LN‐resident APCs), thereby activating powerful immune stimulation. Moreover, the hydrogel vaccine exhibits significant tumor growth inhibition in melanoma and inhibits pulmonary metastatic nodule formation.
In Situ Construction of Hollow Coral‐Like Porous S‐Doped g‐C3N4/ZnIn2S4 S‐Scheme Heterojunction for Efficient Photocatalytic Hydrogen Evolution
Authors: Wang Tianyu , Pan Xuanlin , He Minyi , Kang Lei , Ma Wangjing 
Published: July 2024

AbstractThe rational design of visible‐light‐responsive catalysts is crucial for converting solar energy into hydrogen energy to promote sustainable energy development. In this work, a C─S─C bond is introduced into g‐C3N4 (CN) through S doping. With the help of the flexible C─S─C bond under specific stimuli, a hollow coral‐like porous structure of S‐doped g‐C3N4 (S‐CN) is synthesized for the first time. And an S‐doped g‐C3N4/ZnIn2S4 (S‐CN/ZIS) heterojunction catalyst is in situ synthesized based on S‐CN. S0.5‐CN/ZIS exhibits excellent photocatalytic hydrogen evolution (PHE) efficiency (19.25 mmol g−1 h−1), which is 2.7 times higher than that of the g‐C3N4/ZnIn2S4 (CN/ZIS) catalyst (8.46 mmol g−1 h−1), with a high surface quantum efficiency (AQE) of 34.43% at 420 nm. Experiments and theoretical calculations demonstrate that the excellent photocatalytic performance is attributed to the larger specific surface area and porosity, enhanced interfacial electric field (IEF) effect, and appropriate hydrogen adsorption Gibbs free energy (ΔGH*). The synergistic effect of S doping and S‐scheme heterojunction contributes to the above advancement. This study provides new insights and theoretical basis for the design of CN‐based photocatalysts.
Zinc Promoted Cross‐Electrophile Sulfonylation to Access Alkyl–Alkyl Sulfones
Authors: Wang Zhuochen , Ma Rui , Gu Chang , He Xiaoqian , Shi Haiwei , Bai Ruopeng , Shi Renyi 
Published: July 2024

AbstractThe transition metal‐catalyzed multi‐component cross‐electrophile sulfonylation, which incorporates SO2 as a linker within organic frameworks, has proven to be a powerful, efficient, and cost‐effective means of synthesizing challenging alkyl–alkyl sulfones. Transition metal catalysts play a crucial role in this method by transferring electrons from reductants to electrophilic organohalides, thereby causing undesirable side reactions such as homocoupling, protodehalogenation, β‐hydride elimination, etc. It is worth noting that tertiary alkyl halides have rarely been demonstrated to be compatible with current methods owing to various undesired side reactions. In this work, a zinc‐promoted cross‐electrophile sulfonylation is developed through a radical‐polar crossover pathway. This approach enables the synthesis of various alkyl–alkyl sulfones, including 1°‐1°, 2°‐1°, 3°‐1°, 2°‐2°, and 3°‐2° types, from inexpensive and readily available alkyl halides. Various functional groups are well tolerated in the work, resulting in yields of up to 93%. Additionally, this protocol has been successfully applied to intramolecular sulfonylation and homo‐sulfonylation reactions. The insights gained from this work shall be useful for the further development of cross‐electrophile sulfonylation to access alkyl–alkyl sulfones.
Surface Lattice Modulation Stabilizes K2Mn[Fe(CN)6] Cathode for High‐Energy K‐Ion Batteries
Authors: Wang Xunan , Gao Chongwei , Zhang Shuhua , Wang Jiali , Lou Yikai , Kang Feiyu , Zhai Dengyun 
Published: July 2024

AbstractPotassium‐ion batteries (PIBs) are considered as competitive candidates for energy storage applications due to their abundant resources and low cost. K2Mn[Fe(CN)6] (KMnF) is an ideal cathode for PIBs because of its high theoretical specific energy (≈600 Wh kg−1). However, it suffers from severe Mn dissolution and complex phase transitions caused by Jahn–Teller distortion, resulting in rapid capacity decay. Here, a simple, controllable and universal “transition metal (TM2+) ion exchange” strategy is proposed to modulate the surface lattice of KMnF, not only stabilizing the structure but also maintaining its inherent high capacity. The surface Mn2+ is substituted by TM2+, including Fe2+, Ni2+, Cu2+, or Co2+, forming heterogeneous protection layer. Especially when the surface Mn2+ is modified by redox‐active Fe2+, it exhibits a capacity as high as 144 mAh g−1 and considerable energy density of 560 Wh kg−1 and a remarkable capacity retention (86% after 1,000 cycles at 50 mA g−1, and 71% after 5,000 cycles at 1,000 mA g−1, respectively). The surface‐modified KMnF cathode proved to be effective in stabilizing the structure by preventing the Mn dissolution and formation of tetragonal phase caused by Jahn–Teller distortion. This work provides a simple and universal strategy for stabilizing high‐energy Mn‐based cathode.
Impact of an automated patient outcome feedback system on emergency medicine resident patient follow‐up: An interrupted time series analysis
Authors: Rudolf Frances , Oyama Leslie C. , El‐Kareh Robert 
Published: July 2024

AbstractObjectivesEmergency medicine (EM) residents desire, but often lack, reliable feedback of patient outcomes following handoffs to other providers. This gap is a substantial barrier to calibrating their diagnostic decision making and learning. To address this educational priority, we developed and evaluated the Post‐Handoff Reports of Outcomes (PHAROS) system—an automated system within our electronic health record (EHR) to deliver provider‐specific patient outcome feedback.MethodsPHAROS includes: (1) individualized lists of patients seen and brief summaries of each case, (2) flags for important posthandoff events, and (3) links to charts to facilitate review. Starting June 2020, we coupled PHAROS with a resident educational session and individualized emails every 2 weeks outlining patients seen, number of posthandoff events, and instructions on how to access the PHAROS system.ResultsFrom July 2017 through April 2022, we measured the proportion of handoffs followed by reaccessing patients’ charts between 2 and 14 days posthandoff—a proxy for following up on the patient's outcomes. We performed an interrupted time series analysis on this outcome to determine if PHAROS was associated with a significant change in the trend of our outcome over time. Our secondary outcome was the number of times PHAROS was viewed each month. Our primary outcome had a significant increase in the slope over time (+0.13%/month, p = 0.03) after the introduction of the personalized reports and a nonsignificant change (−1.6%, p = 0.07) at the time of the intervention. The median (IQR) number of views of PHAROS per month was 33.2 (23.75–38.75).ConclusionsThe PHAROS system was associated with a significant increase in the rate of posthandoff chart reaccess among EM residents over time. The PHAROS project demonstrated the feasibility of harnessing the capabilities of the EHR to create an automated system to support EM trainee feedback of patient outcomes—a key component of diagnostic calibration and learning.
Dynamic response and discrimination of gaseous sarin using a boron‐difluoride complex film‐based fluorescence sensor
Authors: Zhou Zhijie , Zhang Lei , Peng Lingya , Li Yingjie , Zhu Xiaolin , Wu Yidi , Qiu Zebiao , He Gang , Qin Molin , Peng Haonan , Fang Yu 
Published: July 2024

AbstractThis study presents a novel boron‐difluoride complex‐based fluorescent nanofilm sensor capable of detecting sarin vapors in the environment by reporting an output fluorescence signal. The sensor's evaluation demonstrated an exceptionally low detection limit for sarin vapor, even in the presence of various interfering gases, with theoretical and practical limits of detection of 0.7 and 1 ppb, respectively. The sensor featured a rapid response time (less than 2 s), a broad linear detection range (1 ppb–1000 ppm), and superior selectivity for sarin vapor over a group of interfering analytes, outperforming existing sarin sensors. Mechanistic study indicates that the sensor's heightened sensitivity to sarin vapor is due to the robust affinity of nitrogen atoms within the core BODIQ unit for sarin. Additionally, the tetraphenylethylene structure with steric hindrance effectively inhibits the tight packing of BODIQ derivatives, and forms numerous microporous structures in the self‐assembled nanofilm, which are beneficial for the mass transfer, enhancing the sensor efficiency in detecting vapors. Furthermore, we have achieved the differentiation of sarin, diethyl chlorophosphate, and HCl vapor through the analysis of sensing kinetic. This fluorescent sensor opens new avenues for sustainable, low‐cost, and environment‐friendly portable devices, as well as for environmental monitoring and tracking applications.
Coming to the Caribbean: Eighty‐five years of rhesus macaques (Macaca mulatta) at Cayo Santiago—A rare nonhuman primate model for the studies of adaptation, diseases, genetics, natural disasters, and resilience
Authors: Wang Qian , Francis George 
Published: July 2024

AbstractThe Cayo Santiago rhesus macaque colony represents one of the most important nonhuman primate resources since their introduction to the Caribbean area in 1938. The 85 years of continuing existence along with the comprehensive database of the rhesus colony and the derived skeletal collections have provided and will continue to provide a powerful tool to test hypotheses about adaptive and evolutionary mechanisms in both biology and medicine.
Florbetaben amyloid PET acquisition time: Influence on Centiloids and interpretation
Authors: Johns Emily , Vossler Hillary A. , Young Christina B. , Carlson Mackenzie L. , Winer Joseph R. , Younes Kyan , Park Jennifer , Rathmann‐Bloch Julia , Smith Viktorija , Harrison Theresa M. , Landau Susan , Henderson Victor , Wagner Anthony , Sha Sharon J. , Zeineh Michael , Zaharchuk Greg , Poston Kathleen L. , Davidzon Guido A. , Mormino Elizabeth C. 
Published: July 2024

AbstractINTRODUCTIONAmyloid positron emission tomography (PET) acquisition timing impacts quantification.METHODSIn florbetaben (FBB) PET scans of 245 adults with and without cognitive impairment, we investigated the impact of post‐injection acquisition time on Centiloids (CLs) across five reference regions. CL equations for FBB were derived using standard methods, using FBB data collected between 90 and 110 min with paired Pittsburgh compound B data. Linear mixed models and t‐tests evaluated the impact of acquisition time on CL increases.RESULTSCL values increased significantly over the scan using the whole cerebellum, cerebellar gray matter, and brainstem as reference regions, particularly in amyloid‐positive individuals. In contrast, CLs based on white matter–containing reference regions decreased across the scan.DISCUSSIONThe quantification of CLs in FBB PET imaging is influenced by both the overall scan acquisition time and the choice of reference region. Standardized acquisition protocols or the application of acquisition time–specific CL equations should be implemented in clinical protocols.Highlights
Acquisition timing affects florbetaben positron emission tomography (PET) scan quantification, especially in amyloid‐positive participants.
The impact of acquisition timing on quantification varies across common reference regions.
Consistent acquisitions and/or appropriate post‐injection adjustments are needed to ensure comparability of PET data.
Perivascular spaces, plasma GFAP, and speeded executive function in neurodegenerative diseases
Authors: Andriuta Daniela , Ottoy Julie , Ruthirakuhan Myuri , Feliciano Ginelle , Dilliott Allison A. , Hegele Robert A. , Gao Fuqiang , McLaughlin Paula M. , Rabin Jennifer S. , Wood Alexander Madeline , Scott Christopher J. M. , Yhap Vanessa , Berezuk Courtney , Ozzoude Miracle , Swardfager Walter , Zebarth Julia , Tartaglia M. Carmela , Rogaeva Ekaterina , Tang‐Wai David F. , Casaubon Leanne , Kumar Sanjeev , Dowlatshahi Dar , Mandzia Jennifer , Sahlas Demetrios , Saposnik Gustavo , Fischer Corinne E. , Borrie Michael , Hassan Ayman , Binns Malcolm A. , Freedman Morris , Chertkow Howard , Finger Elizabeth , Frank Andrew , Bartha Robert , Symons Sean , Zetterberg Henrik , Swartz Richard H. , Masellis Mario , Black Sandra E. , Ramirez Joel ,   ONDRI Investigators
Published: July 2024

AbstractINTRODUCTIONWe investigated the effect of perivascular spaces (PVS) volume on speeded executive function (sEF), as mediated by white matter hyperintensities (WMH) volume and plasma glial fibrillary acidic protein (GFAP) in neurodegenerative diseases.METHODSA mediation analysis was performed to assess the relationship between neuroimaging markers and plasma biomarkers on sEF in 333 participants clinically diagnosed with Alzheimer's disease/mild cognitive impairment, frontotemporal dementia, or cerebrovascular disease from the Ontario Neurodegenerative Disease Research Initiative.RESULTSPVS was significantly associated with sEF (c = ‐0.125 ± 0.054, 95% bootstrap confidence interval [CI] [‐0.2309, ‐0.0189], p = 0.021). This effect was mediated by both GFAP and WMH.DISCUSSIONIn this unique clinical cohort of neurodegenerative diseases, we demonstrated that the effect of PVS on sEF was mediated by the presence of elevated plasma GFAP and white matter disease. These findings highlight the potential utility of imaging and plasma biomarkers in the current landscape of therapeutics targeting dementia.Highlights
Perivascular spaces (PVS) and white matter hyperintensities (WMH) are imaging markers of small vessel disease.
Plasma glial fibrillary protein acidic protein (GFAP) is a biomarker of astroglial injury.
PVS, WMH, and GFAP are relevant in executive dysfunction from neurodegeneration.
PVS's effect on executive function was mediated by GFAP and white matter disease.
Elimination of GGTA1, CMAH, β4GalNT2 and CIITA genes in pigs compromises human versus pig xenogeneic immune reactions
Authors: Xu Jing , Ren Jilong , Xu Kai , Fang Minghui , Ka Meina , Xu Fei , Wang Xin , Wang Jing , Han Zhiqiang , Feng Guihai , Zhang Ying , Hai Tang , Li Wei , Hu Zheng 
Published: July 2024

AbstractBackgroundPig organ xenotransplantation is a potential solution for the severe organ shortage in clinic, while immunogenic genes need to be eliminated to improve the immune compatibility between humans and pigs. Current knockout strategies are mainly aimed at the genes causing hyperacute immune rejection (HAR) that occurs in the first few hours while adaptive immune reactions orchestrated by CD4 T cell thereafter also cause graft failure, in which process the MHC II molecule plays critical roles.MethodsThus, we generate a 4‐gene (GGTA1, CMAH, β4GalNT2, and CIITA) knockout pig by CRISPR/Cas9 and somatic cell nuclear transfer to compromise HAR and CD4 T cell reactions simultaneously.ResultsWe successfully obtained 4KO piglets with deficiency in all alleles of genes, and at cellular and tissue levels. Additionally, the safety of our animals after gene editing was verified by using whole‐genome sequencing and karyotyping. Piglets have survived for more than one year in the barrier, and also survived for more than 3 months in the conventional environment, suggesting that the piglets without MHC II can be raised in the barrier and then gradually mated in the conventional environment.Conclusions4KO piglets have lower immunogenicity, are safe in genomic level, and are easier to breed than the model with both MHC I and II deletion.