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ccS chemistry 2021年第7期3卷 1921-1928页

作者： Qunchao Zhao Patrick G.Isenegger thomas c.wilson Jeroen BISap Florian Guibbal Long Lu Véronique Gouverneur Qilong Shen Key Laboratory of Organofluorine chemistry center for Excellence in Molecular Synthesis Shanghai Institute of Organic ChemistryUniversity of Chinese Academy of SciencesChinese Academy of SciencesShanghai 200032 chemistry Research Laboratory University of OxfordOxford OX13TA Shanghai Institute of Organic chemistry Chinese Academy of SciencesShanghai 200032

Herein,we report a mild and practical protocol for the copper-catalyzed chlorofluoromethylthiolation of(hetero)aryl boronic acids with the novel reagent *** resulting products are amenable to halogen-exchange^(18)F-fluorination with cyclotronproduced[^(18)F]fluoride affording[^(18)F]*** process highlights the combined value of reagent development and(hetero)aryl boron precursors for radiochemistry by adding the[^(18)F]ScF2H group to the list of^(18)F-motifs within reach for positron emission tomography studies.

关键词： chlorofluoromethylthiolation boron reagent PET fluorine radiolabeling

α-cumyl bromodifluoromethanesulfenate: Application to the Radiosynthesis of [18F]arylScF3

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α-Cumyl bromodifluoromethanesulfenate: Application to the R...

Theory and classification of mass extinction causation

中国化学会第十五届全国氟化学会议

作者： Qunchao Zhao Jiang Wu thomas c.wilson Stefan Verhoog Long Lu Véronique Gouverneur Qilong Shen Key Laboratory of Organofluorine chemistry Shanghai Institute of Organic Chemistry University of Oxford OxfordChemistry Research Laboratory Shanghai Institute of Organic chemistry Chinese Academy of Sciences

Positron Emission Tomography(PET) is a leading noninvasive imaging modality enabling the study of physiological processes in vivo. The trifluoromethylthiol group(-ScF) has gained much attention in the context of medicinal chemistry due to its beneficial effects on pharmacokinetic and physicochemical properties including metabolic stability and lipophilicity.

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National Science Review 2024年第1期11卷 16-36页

作者： thomas J.Algeo Jun Shen State Key Laboratory of Biogeology and Environmental Geology China University of Geosciences—Wuhan State Key Laboratory of Geological Processes and Mineral Resources China University of Geosciences—Wuhan Department of Geosciences University of Cincinnati

Theory regarding the causation of mass extinctions is in need of systematization, which is the focus of this contribution. Every mass extinction has both an ultimate cause, i.e. the trigger that leads to various climato-environmental changes, and one or more proximate cause(s), i.e. the specific climato-environmental changes that result in elevated biotic mortality. With regard to ultimate causes, strong cases can be made that bolide(i.e. meteor) impacts, large igneous province(LIP) eruptions and bioevolutionary events have each triggered one or more of the Phanerozoic Big Five mass extinctions, and that tectono-oceanic changes have triggered some second-order extinction events. Apart from bolide impacts, other astronomical triggers(*** flares, gamma bursts and supernova explosions) remain entirely in the realm of speculation. With regard to proximate mechanisms, most extinctions are related to either carbon-release or carbon-burial processes, the former being associated with climatic warming, ocean acidification, reduced marine productivity and lower carbonate δ13c values, and the latter with climatic cooling, increased marine productivity and higher carbonate δ13c values. Environmental parameters such as marine redox conditions and terrestrial weathering intensity do not show consistent relationships with carbon-cycle *** this context, mass extinction causation can be usefully classified using a matrix of ultimate and proximate factors. Among the Big Five mass extinctions, the end-cretaceous biocrisis is an example of a bolide-triggered carbon-release event, the end-Permian and end-Triassic biocrises are examples of LIP-triggered carbon-release events, and the Late Ordovician and Late Devonian biocrises are examples of bioevolution-triggered carbon-burial events. Whereas the bolide-impact and LIP-eruption mechanisms appear to invariably cause carbon release, bioevolutionary triggers can result in variable carbon-cycle changes, e.g. carbon burial durin

关键词： biocrisis ultimate cause proximate cause bolide large igneous province bioevolutionary event

Dynamic convergent shock compression initiated by return current in high-intensity laser-solid interactions

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Matter and Radiation at Extremes 2024年第4期9卷 40-53页

作者： Long Yang Martin Rehwald thomas Kluge Alejandro LasoGarcia Toma Toncian Karl Zeil Ulrich Schramm thomas E.cowan Lingen Huang Helmholtz-Zentrum Dresden-Rossendorf 01328 DresdenGermany Technische Universitat Dresden 01062 DresdenGermany

We investigate the dynamics of convergent shock compression in solid cylindrical targets irradiated by an ultrafast relativistic laser *** particle-in-cell simulations and coupled hydrodynamic simulations reveal that the compression process is initiated by both magnetic pressure and surface ablation associated with a strong transient surface return current with density of the order of 10^(17) A/m^(2) and lifetime of 100 *** results show that the dominant compression mechanism is governed by the plasma β,i.e.,the ratio of thermal pressure to magnetic *** targets with small radius and low atomic number Z,the magnetic pressure is the dominant shock compression *** to a scaling law,as the target radius and Z increase,the surface ablation pressure becomes the main mechanism generating convergent ***,an indirect experimental indication of shocked hydrogen compression is provided by optical shadowgraphy measurements of the evolution of the plasma expansion *** results presented here provide a novel basis for the generation of extremely high pressures exceeding Gbar(100 TPa)to enable the investigation of high-pressure physics using femtosecond J-level laser pulses,offering an alternative to nanosecond kJ-laser pulse-driven and pulsed power Z-pinch compression methods.

关键词： shock convergent return

Blood metal concentrations and cardiac structure and function in total joint arthroplasty patients

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World Journal of Orthopedics 2024年第8期15卷 773-782页

作者： Peter c Brennan Stephanie M Peterson thomas J O'Byrne Mariana L Laporta cody c Wyles Paul J Jannetto Garvan c Kane Maria Vassilaki Hilal Maradit Kremers Department of Orthopedic Surgery Mayo ClinicRochesterMN 55905United States Department of Quantitative Health Sciences Mayo ClinicRochesterMN 55905United States Department of Anesthesiology and Perioperative Medicine Mayo ClinicRochesterMN 55905United States Department of Laboratory Medicine and Pathology Mayo ClinicRochesterMN 55905United States Department of cardiovascular Diseases Mayo ClinicRochesterMN 55905United States

BAcKGROUND There is concern regarding potential long-term cardiotoxicity with systemic distribution of metals in total joint arthroplasty(TJA)*** To determine the association of commonly used implant metals with echocardiographic measures in TJA *** The study comprised 110 TJA patients who had a recent history of high chromium,cobalt or titanium *** underwent two-dimensional,three-dimensional,Doppler and speckle-strain transthoracic echocardiography and a blood draw to measure metal *** and sex-adjusted linear and logistic regression models were used to examine the association of metal concentrations(exposure)with echocardiographic measures(outcome).RESULTS Higher cobalt concentrations were associated with increased left ventricular end-diastolic volume(estimate 5.09;95%cI:0.02-10.17)as well as left atrial and right ventricular dilation,particularly in men but no changes in cardiac *** titanium concentrations were associated with a reduction in left ventricle global longitudinal strain(estimate 0.38;95%cI:0.70 to 0.06)and cardiac index(estimate 0.08;95%cI,-0.15 to-0.01).cONcLUSION Elevated cobalt and titanium concentrations may be associated with structural and functional cardiac changes in some *** studies are warranted to better understand the systemic effects of metals in TJA patients.

关键词： Total joint arthroplasty Metal-on-metal cardiotoxicity Heart failure Echocardiography cobalt

SMXL5 attenuates strigolactone signaling in Arabidopsis thaliana by inhibiting SMXL7 degradation

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Molecular Plant 2024年第4期17卷 631-647页

作者： Qingtian Li Haiyang Yu Wenwen chang Sunhyun chang Michael Guzman Lionel Faure Eva-Sophie Wallner Heqin Yan thomas Greb Lei Wang Ruifeng Yao David c.Nelson Department of Botany and Plant Sciences University of CaliforniaRiversideRiversideCA 2521USA Yazhouwan National Laboratory Sanya 572025China Hainan Seed Industry Laboratory Sanya 57205China State Key Laboratory of chemo/Biosensing and chemometrics Hunan Provincial Key Laboratory of Plant Functional Genomics and Developmental RegulationCollege of BiologyHunan UniversityChangsha 410082China Key Laboratory of Seed Innovation Center for Agricultural Resources ResearchInstitute of Genetics and Developmental BiologyChinese Academy of SciencesShijiazhuangHebei 050021China University of chinese Academy of Sciences Beijing 10004China School of the Sciences Biology DivisionTexas Woman’s UniversityDentonTX 76204USA centre for Organismal Studies(cOS) Heidelberg University6120 HeidelbergGermany

Hormone-activated proteolysis is a recurring theme of plant hormone signaling *** strigolactone signaling,the enzyme receptor DWARF14(D14)and an F-box protein,MORE AXILLARY GROWTH2(MAX2),mark SUPPRESSOR OF MAX21-LIKE(SMXL)family proteins SMXL6,SMXL7,and SMXL8 for rapid *** of these transcriptional corepressors initiates downstream growth *** homologous proteins SMXL3,SMXL4,and SMXL5,however,are resistant to MAX2-mediated *** discovered that the smxl4 smxl5 mutant has enhanced responses to ***5 attenuates strigolactone signaling by interfering with AtD14-SMXL7 ***5 interacts with AtD14 and SMXL7,providing two possible ways to inhibit SMXL7 ***5 function is partially dependent on an ethylene-responsive-element binding-factor-associated amphiphilic repression(EAR)motif,which typically mediates interactions with the TOPLESS family of transcriptional ***,we found that loss of the EAR motif reduces SMXL5-SMXL7 interactions and the attenuation of strigolactone signaling by *** hypothesize that integration of SMXL5 into heteromeric SMXL complexes reduces the susceptibility of SMXL6/7/8 proteins to strigolactone-activated degradation and that the EAR motif promotes the formation or stability of these *** mechanism may provide a way to spatially or temporally fine-tune strigolactone signaling through the regulation of SMXL5 expression or translation.

关键词： Arabidopsis typically inhibiting

Reversed charge transfer induced by nickel in Fe-Ni/Mo_(2)c@nitrogen-doped carbon nanobox for promoted reversible oxygen electrocatalysis

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Journal of Energy chemistry 2024年第1期88卷 202-212,I0005页

作者： Zhicheng Nie Lei Zhang Qiliang Zhu Zhifan Ke Yingtang Zhou thomas Wågberg Guangzhi Hu School of Materials Science and Engineering Anhui University of Science and TechnologyHuainan 232001AnhuiChina Institute for Ecological Research and Pollution control of Plateau Lakes School of Ecology and Environmental ScienceYunnan UniversityKunming 650504YunnanChina National Engineering Research center for Marine Aquaculture Marine Science and Technology CollegeZhejiang Ocean UniversityZhoushan 316004ZhejiangChina Department of Physics UmeåUniversityUmeåS-90187Sweden

The interaction between metal and support is critical in oxygen catalysis as it governs the charge transfer between these two entities,influences the electronic structures of the supported metal,affects the adsorption energies of reaction intermediates,and ultimately impacts the catalytic *** this study,we discovered a unique charge transfer reversal phenomenon in a metal/carbon nanohybrid ***,electrons were transferred from the metal-based species to N-doped carbon,while the carbon support reciprocally donated electrons to the metal domain upon the introduction of *** led to the exceptional electrocatalytic performances of the resulting Ni-Fe/Mo_(2)c@nitrogen-doped carbon catalyst,with a half-wave potential of 0.91 V towards oxygen reduction reaction(ORR)and a low overpotential of 290 m V at 10 mA cm^(-2)towards oxygen evolution reaction(OER)under alkaline ***,the Fe-Ni/Mo_(2)c@carbon heterojunction catalyst demonstrated high specific capacity(794 mA h g_(Zn)~(-1))and excellent cycling stability(200 h)in a Zn-air *** calculations revealed that Mo_(2)c effectively inhibited charge transfer from Fe to the support,while secondary doping of Ni induced a charge transfer reversal,resulting in electron accumulation in the Fe-Ni alloy *** local electronic structure modulation significantly reduced energy barriers in the oxygen catalysis process,enhancing the catalytic efficiency of both ORR and ***,our findings underscore the potential of manipulating charge transfer reversal between the metal and support as a promising strategy for developing highly-active and durable bi-functional oxygen electrodes.

关键词： Metal-support interaction charge transfer reversal Oxygen reduction reaction Oxygen evolution reaction Zinc-air battery

Numerical study of novel OME_(1-6) combustion mechanism and spray combustion at changed ambient environments

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Frontiers in Energy 2024年第4期18卷 483-505页

作者： Frederik WIESMANN Zeyan QIU Dong HAN Lukas STRAUβ Sebastian RIEβ Michael WENSING thomas LAUER Institute of Powertrains and Automotive Technology TU Wien1060 ViennaAustria Key Laboratory for Power Machinery and Engineering of Ministry of Education Shanghai Jiao Tong UniversityShanghai 200240China Professorship for Fluid Systems Technology Friedrich-AlexanderUniversität Erlangen-Nürnberg91058 ErlangenGermany

For a climate-neutral future mobility,the socalled e-fuels can play an essential ***,oxygenated e-fuels containing oxygen in their chemical formula have the additional potential to burn with significantly lower soot *** particular,polyoxymethylene dimethyl ethers or oxymethylene ethers(PODEs or OMEs)do not contain carbon-carbon bonds,prohibiting the production of soot precursors like acetylene(c_(2)H_(2)).These properties make OMEs a highly interesting candidate for future climate-neutral compression-ignition ***,to fully leverage their potential,the auto-ignition process,flame propagation,and mixing regimes of the combustion need to be *** achieve this,efficient oxidation mechanisms suitable for computational fluid dynamics(cFD)calculations must be developed and *** present work aims to highlight the improvements made by developing an adapted oxidation mechanism for OME1-6 and introducing it into a validated spray combustion cFD model for *** simulations were conducted for single-and multi-injection patterns,changing ambient temperatures,and oxygen *** results were validated against high-pressure and high-temperature constantpressure chamber ****-chemiluminescence measurements accomplished the characterization of the auto-ignition *** experiments and simulations were conducted for two different *** improvements concerning the prediction of the ignition delay time were accomplished while also retaining an excellent agreement for the flame lift-off *** spatial zones of high-temperature reaction activity were also affected by the adaption of the reaction *** showed a greater tendency to form OH^(*) radicals within the center of the spray in accordance with the experiments.

关键词： oxygenated fuels reaction kinetics oxidation mechanisms computational fluid dynamics(cFD) oxymethylene ethers(OME) e-fuels multiinjection spray-combustion

Unsynchronized butyrophilin molecules dictate cancer cell evasion of Vγ9Vδ2 T-cell killing

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cellular & Molecular Immunology 2024年第4期21卷 362-373页

作者： Zeguang Wu Qiezhong Lamao Meichao Gu Xuanxuan Jin Ying Liu Feng Tian Ying Yu Pengfei Yuan Shuaixin Gao thomas S.Fulford Adam P.Uldrich catherine c.L Wong Wensheng Wei Biomedical Pioneering Innovation center Peking-Tsinghua Center for Life SciencesPeking University Genome Editing Research CenterState Key Laboratory of Protein and Plant Gene ResearchSchool of Life SciencesPeking University100871BeijingChina EdiGene Inc. Life Science ParkChangping District102206BeijingChina center for Precision Medicine Multi-Omics Research Peking University Health Science CenterPeking University100191BeijingChina Department of Microbiology and Immunology at the Peter Doherty Institute for Infection and Immunity The University of MelbourneParkvilleVIC3010Australia cancer Immunology Program Peter MacCallum Cancer CentreMelbourneVICAustralia State Key Laboratory for complex Severe and Rare DiseasesClinical Research InstitutePeking Union Medical College HospitalChinese Academy of Medical Science&Peking Union Medical CollegePeking-Tsinghua Center for Life Sciences100871BeijingChina

Vγ9Vδ2 T cells are specialized effector cells that have gained prominence as immunotherapy agents due to their ability to target and kill cells with altered pyrophosphate *** our effort to understand how cancer cells evade the cell-killing activity of Vγ9Vδ2 T cells,we performed a comprehensive genome-scale cRISPR screening of cancer *** found that four molecules belonging to the butyrophilin(BTN)family,specifically BTN2A1,BTN3A1,BTN3A2,and BTN3A3,are critically important and play unique,nonoverlapping roles in facilitating the destruction of cancer cells by primary Vγ9Vδ2 T *** coordinated function of these BTN molecules was driven by synchronized gene expression,which was regulated by IFN-γsignaling and the RFX ***,an enzyme called QPcTL was shown to play a key role in modifying the N-terminal glutamine of these BTN proteins and was found to be a crucial factor in Vγ9Vδ2 T cell killing of cancer *** our research,we offer a detailed overview of the functional genomic mechanisms that underlie how cancer cells escape Vγ9Vδ2 T ***,our findings shed light on the importance of the harmonized expression and function of gene family members in modulating T-cell activity.

关键词： Butyrophilin Vγ9Vδ2 T-cell cancer-specific immune evasion Glutaminyl-peptide cyclotransferase-like Pyrophosphate metabolite Immunotherapy

Entangled photon pair generation in an integrated Sic platform

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Light(Science & Applications) 2024年第6期13卷 1041-1046页

作者： Anouar Rahmouni Ruixuan Wang Jingwei Li Xiao Tang thomas Gerrits Oliver Slattery Qing Li Lijun Ma National Institute of Standards and Technology 100 Bureau DrGaithersburgMD20899USA Department of Electrical and computer Engineering Carnegie Mellon UniversityPittsburghPA15213USA

Entanglement plays a vital role in quantum information *** to its unique material properties,silicon carbide recently emerged as a promising candidate for the scalable implementation of advanced quantum information processing *** date,however,only entanglement of nuclear spins has been reported in silicon carbide,while an entangled photon source,whether it is based on bulk or chip-scale technologies,has remained ***,we report the demonstration of an entangled photon source in an integrated silicon carbide platform for the first ***,strongly correlated photon pairs are efficiently generated at the telecom c-band wavelength through implementing spontaneous four-wave mixing in a compact microring resonator in the 4H-silicon-carbide-on-insulator *** maximum coincidence-to-accidental ratio exceeds 600 at a pump power of 0.17 mW,corresponding to a pair generation rate of(9±1)×10^(3) pairs/***-time entanglement is created and verified for such signal-idler photon pairs,with the two-photon interference fringes exhibiting a visibility larger than 99%.The heralded single-photon properties are also measured,with the heralded g^((2))(0)on the order of 10^(−3),demonstrating the Sic platform as a prospective fully integrated,complementary metal-oxide-semiconductor compatible single-photon source for quantum applications.

关键词： quantum coincidence mixing