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Spin effect on redox acceleration and regioselectivity in Fe-catalyzed alkyne hydrosilylation

National Science Review 2024年第2期11卷 155-167页

作者： peng He Meng-Yang Hu Jin-Hong Li tian-Zhang qiao Yi-Lin Lu Shou-Fei Zhu Frontiers Science Center for New Organic Matter State Key Laboratory and Institute of Elemento-Organic Chemistry Nankai University

Iron catalysts are ideal transition metal catalysts because of the Earths abundant, cheap, biocompatible features of iron salts. Iron catalysts often have unique open-shell structures that easily undergo spin crossover in chemical transformations, a feature rarely found in noble metal catalysts. Unfortunately, little is known currently about how the open-shell structure and spin crossover affect the reactivity and selectivity of iron catalysts, which makes the development of iron catalysts a low efficient trial-and-error program. In this paper, a combination of experiments and theoretical calculations revealed that the iron-catalyzed hydrosilylation of alkynes is typical spin-crossover catalysis. Deep insight into the electronic structures of a set of well-defined open-shell active formal Fe(0) catalysts revealed that the spin-delocalization between the iron center and the 1,10-phenanthroline ligand effectively regulates the iron center's spin and oxidation state to meet the opposite electrostatic requirements of oxidative addition and reductive elimination, respectively,and the spin crossover is essential for this electron transfer process. The triplet transition state was essential for achieving high regioselectivity through tuning the nonbonding interactions. These findings provide an important reference for understanding the effect of catalyst spin state on reaction. It is inspiring for the development of iron catalysts and other Earth-abundant metal catalysts, especially from the point of view of ligand development.

关键词： spin effect spin-delocalization spin crossover iron-catalysis alkyne hydrosilylation

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Characterization and identification towards dynamic-based electrical modeling of lithium-ion batteries

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Journal of Energy Chemistry 2024年第5期92卷 738-758页

作者： Chuanxin Fan Kailong Liu Yaxing Ren qiao peng School of Automation Nanjing Institute of TechnologyNanjing 211167JiangsuChina School of Control Science and Engineering Shandong UniversityJinan 250100ShandongChina School of Engineering University of LincolnLincoln LN67TSUK Information Technology Analytics&Operations GroupQueen’s University BelfastBelfast BT95EEUK

Lithium-ion batteries are widely recognized as a crucial enabling technology for the advancement of electric vehicles and energy storage systems in the *** design of battery state estimation and control algorithms in battery management systems is usually based on battery models,which interpret crucial battery dynamics through the utilization of mathematical ***,the investigation of battery dynamics with the purpose of battery system identification has garnered considerable attention in the realm of battery *** methods in terms of linear and nonlinear response of lithium-ion batteries have emerged as a prominent area of study in this *** review has undertaken an analysis and discussion of characterization methods,with a particular focus on the motivation of battery system ***,this work encompasses the incorporation of frequency domain nonlinear characterization methods and dynamics-based battery electrical *** aim of this study is to establish a connection between the characterization and identification of battery systems for researchers and engineers specialized in the field of batteries,with the intention of promoting the advancement of efficient battery technology for real-world applications.

关键词： Lithium-ion battery Battery dynamics Nonlinear characterization Nonlinear battery model

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Strong Linearizability Checking and Determination for Concurrent Objects

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Ruan Jian Xue Bao/Journal of Software 2024年第9期35卷

作者： Wang, Chao Jia, qiao-Wen Lü, Yi Wu, peng Centre for Research and Innovation in Software Engineering College of Computer and Information Science Southwest University Chongqing 400715 China State Key Laboratory of Computer Science Institute of Software Chinese Academy of Sciences Beijing 100190 China University of Chinese Academy of Sciences Beijing 100049 China

Linearizability is universally accepted as a correctness criterion for concurrent objects. However, it has been shown that linearizability cannot be adopted as a correctness criterion for concurrent objects with random sentences. Thus, Golab et al. proposed the concept of strong linearizability, which adds prefix preservation properties based on the linearizability definition and has more constraints for concurrent objects. The research on strong linearizability focuses on the feasibility of generating strongly linearizable objects with certain basic objects, while only a few studies are about checking and verification of strong linearizability. This study investigates strong linearizability from two aspects including the verification algorithm and approach for proving non-strong linearizability of concurrent objects. First, it divides strong linearizability into fixed effective points and pure help and proves that the notion of fixed effective points is an extension of that of fixed linearizability points. Then, two verification algorithms for strong linearizability are put forward. One algorithm is based on checking the fixed linearizability points, and the other is based on the fixed effective points. Finally, an approach is provided for proving that the concurrent objects violate strong linearizability, and it helps verify that the Herlihy&Wing queue, a single-reader single-write register, and a snapshot object violate strong linearizability. © 2024 Chinese Academy of Sciences. All rights reserved.

关键词： concurrent object correctness criterion linearizability strong linearizability

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Study of Pyrolysis Characteristics and Kinetic Analysis of Shenmu Coal at a High Heating Rate Using TG-FTIR

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China Petroleum Processing & Petrochemical Technology 2024年第1期26卷 47-55页

作者： An Xiaoxi Zhang Yanpeng Shang Yanchao tian Yuanyu qiao Yingyun Shandong University of Science and Technology Qingdao 266510ShandongChina China University of Petroleum(Huadong) Qingdao 266555ShandongChina

Coal pyrolysis is a fundamental reaction in the thermal processing and utilization of *** the behavior and kinetics of coal pyrolysis is crucial for optimizing,designing,and developing a composite riser for the staged pyrolysis gasification process of pulverized *** this study,the non-isothermal pyrolysis behavior and kinetics of coal were examined at different heating rates(30,50,100,300,500,700,and 900℃/min)using thermogravimetry(TG)coupled with Fourier-transform infrared *** of the TG/derivative TG(TG/DTG)curves indicated that coal pyrolysis mainly occurred between 300℃ and 700℃.Higher heating rates led to more volatiles being released from the coal,and a higher temperature was required to achieve rapid *** analysis showed that both the model-free methods(Friedman,Flynn-Wall-Ozawa,and Kissinger-Akahira-Sunose)and the model-based method(Coats-Redfern)effectively describe the coal pyrolysis *** change in the Ea values between the two kinetic models was consistent throughout the pyrolysis process,and the most probable mechanism was the F2 model(secondary chemical reaction).In addition,the heating rate did not change the overall reaction order of the pyrolysis process;however,a higher heating rate resulted in a decrease in the Ea value during the initial pyrolysis stage.

关键词： coal pyrolysis TG-FTIR characteristic parameters dynamics

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The evolution and functional divergence of 10 Apolipoprotein D-like genes in Nilaparvata lugens

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Insect Science 2024年第1期31卷 91-105页

作者： Jia-Bao Lu peng-peng Ren qiao Li Fang He Zhong-tian Xu Sai-Nan Wang Jian-Ping Chen Jun-Min Li Chuan-Xi Zhang Citrus Research Institute Southwest University/Chinese Academy of Agricultural SciencesNational Engineering Research Center for CitrusChongqingChina Technology Center of Wuhan Customs District HubeiChina Institute of Insect Science Zhejiang UniversityHangzhouChina

Apolipoprotein D(ApoD),a member of the lipocalin superfamily of proteins,is involved in lipid transport and stress *** only a single copy of the ApoD gene is found in humans and some other vertebrates,there are typically several ApoD-like genes in *** date,there have been relatively few studies that have examined the evolution and functional differentiation of ApoD-like genes in insects,particularly hemi-metabolous *** this study,we identified 10 ApoD-like genes(NlApoD1−10)with distinct spatiotemporal expression patterns in Nilaparvata lugens(BPH),which is an important pest of ***1−10 were found to be distributed on 3 chromosomes in a tandem array of NlApoD1/2,NlApoD3−5,and NlApoD7/8,and show sequence and gene structural divergence in the coding regions,indicating that multiple gene duplication events occurred during *** analysis revealed that NlApoD1−10 can be clustered into 5 clades,with NlApoD3−5 and NlApoD7/8 potentially evolving exclusively in the Delphacidae *** screening using an RNA interference approach revealed that only NlApoD2 was essential for BPH development and survival,whereas NlApoD4/5 are highly expressed in testes,and might play roles in ***,stress response analysis revealed that NlApoD3−5/9,NlApoD3−5,and NlApoD9 were up-regulated after treatment with lipopolysaccharide,H2O2,and ultraviolet-C,respectively,indicating their potential roles in stress resistance.

关键词： Apolipoprotein D BPH evolution functional divergence gene duplication NIApoD

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Simulation of Underground Reservoir Stability of Pumped Storage Power Station Based on Fluid-Structure Coupling

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Computer Modeling in Engineering & Sciences 2024年第5期139卷 1381-1399页

作者： peng qiao Shuangshuang Lan Hongbiao Gu Zhengtan Mao Faculty of Architecture Civil and Transportation EngineeringBeijing University of TechnologyBeijing100020China College of Transportation Engineering Nanjing Tech UniversityNanjing210000China

Based on global initiatives such as the clean energy transition and the development of renewable energy,the pumped storage power station has become a new and significant way of energy storage and regulation,and its construction environment is more complex than that of a traditional *** particular,the stability of the rock strata in the underground reservoirs is affected by the seepage pressure and rock stress,which presents some challenges in achieving engineering safety and *** the advantages of the numerical simulation method in dealing deal with nonlinear problems in engineering stability,in this study,the stability of the underground reservoir of the Shidangshan(SDS)pumped storage power station was numerically calculated and quantitatively analyzed based on fluid-structure coupling theory,providing an important reference for the safe operation and management of the underground ***,using the COMSOL software,a suitablemechanicalmodel was created in accordance with the geological structure and project characteristics of the underground ***,the characteristics of the stress field,displacement field,and seepage field after excavation of the underground reservoir were simulated in light of the seepage effect of groundwater on the nearby rock of the underground ***,based on the construction specifications and Molar-Coulomb criterion,a thorough evaluation of the stability of the underground reservoir was performed through simulation of the filling and discharge conditions and anti-seepage strengthening *** findings demonstrate that the numerical simulation results have a certain level of reliability and are in accordance with the stress measured in the project *** underground reservoir excavation resulted in a maximum displacement value of the rock mass around the caverns of 3.56 mm in a typical section,and the safety coefficient of the parts,as determined using the Molar-Coulomb criterion,was highe

关键词： Underground reservoir fluid-structure coupling numerical simulation pumped storage power station filling and discharge

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Cryptic diversity and rampant hybridization in annual gentians on the Qinghai-Tibet Plateau revealed by population genomic analysis

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Plant Diversity 2024年第2期46卷 194-205页

作者： peng-Cheng Fu qiao-qiao Guo Di Chang Qing-Bo Gao Shan-Shan Sun School of Life Science Luoyang Normal UniversityLuoyang 471934PR China Key Laboratory of Adaptation and Evolution of Plateau Biota Northwest Institute of Plateau BiologyChinese Academy of SciencesXining 810001PR China

Understanding the evolutionary and ecological processes involved in population differentiation and speciation provides critical insights into biodiversity formation. In this study, we employed 29,865 single nucleotide polymorphisms(SNPs) and complete plastomes to examine genomic divergence and hybridization in Gentiana aristata, which is endemic to the Qinghai-Tibet Plateau(QTP) region. Genetic clustering revealed that G. aristata is characterized by geographic genetic structures with five clusters(West, East, Central, South and North). The West cluster has a specific morphological character(i.e., blue corolla) and higher values of FSTcompared to the remaining clusters, likely the result of the geological barrier formed by the Yangtze River. The West cluster diverged from the other clusters in the Early Pliocene;these remaining clusters diverged from one another in the Early Quaternary. Phylogenetic reconstructions based on SNPs and plastid data revealed substantial cyto-nuclear conflicts. Genetic clustering and D-statistics demonstrated rampant hybridization between the Central and North clusters,along the Bayankala Mountains, which form the geological barrier between the Central and North clusters. Species distribution modeling demonstrated the range of G. aristata expanded since the Last Interglacial period. Our findings provide genetic and morphological evidence of cryptic diversity in G. aristata, and identified rampant hybridization between genetic clusters along a geological *** findings suggest that geological barriers and climatic fluctuations have an important role in triggering diversification as well as hybridization, indicating that cryptic diversity and hybridization are essential factors in biodiversity formation within the QTP region.

关键词： Gentiana aristata Hybrid zone Qinghai-Tibet Plateau Plastome Nuclear SNPs

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Fabrication of Molecularly Imprinted Electrospun Nanofibers with Mono-amidoxime Functional Ligand for Efficient Decontamination of Toxic Organophosphates

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Chinese Journal of Polymer Science 2024年第4期42卷 446-456页

作者： Lan Wang peng Jiang Ya-Lin Niu Jun-peng Cao tian-Ying Guo Key Laboratory of Functional Polymer Materials Ministry of EducationInstitute of Polymer ChemistryCollege of Chemistry and Frontier Science Center for the Creation of New Organic SubstancesNankai UniversityTianjin300071China

There is an urgent imperative to discover practical and efficacious artificial catalysts for the expeditious decontamination of toxic organophosphates. Herein, we propose a novel molecularly imprinted approach utilizing electrospun fiber scaffolds. Specifically, an amidoxime-based functional polymer (PMAOX) has been synthesized, which contains amidoxime groups that can act as nucleophiles and ligands for the formation of catalytic active sites. This polymer was blended with polyacrylonitrile (PAN), a well-processable material, to prepare a nanofiber mat using electrospinning techniques. Then, the amidoxime side groups on fiber surface were further cross-linked after the molecular coordination of templates to complete the molecularly imprinting process. This approach can not only enhance the content of functional molecularly imprinted polymers without affecting structural stability, but also combines surface MI technology to fully expose and leverage the advantages of active sites. The as prepared molecularly imprinted electrospun nanofibers MIF-Zn-PMAOX/PAN-6/4 catalyzes the degradation of paraoxon with a half-life of 32 min, and MIF-Ag-PMAOX/PAN catalyzes the degradation of parathion with a half-life of 18 min. The maximum catalytic rate evidence rate enhancements nearly 3700-fold of the self-hydrolysis. Thus, the mono-amidoxime based molecularly imprinted fibers demonstrate the versatility and superiority as self-detoxifying for organophosphates.

关键词： Organophosphateshydrolysis Electrospinning Molecular imprinting

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Atomistic study of inverse size effect induced by interfacial plasticity in pearlitic multi-principal element alloy

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Rare Metals 2024年第7期43卷 3341-3355页

作者： Chen Yang qiao-Sheng Xia Cun-Hong Yin Dong-peng Hua College of Mechanical Engineering Guizhou University Key Laboratory of Advanced Manufacturing Technology Ministry of EducationGuizhou University State Key Laboratory of Solidification Processing Center of Advanced Lubrication and Seal MaterialsNorthwestern Polytechnical University

Owing to the fine nano-laminated structure,the pearlitic multi-principal element alloy（PMPEA） exhibits excellent mechanical and tribological ***,the incomplete understanding of the size effect of its lamella thickness and the unclear understanding of the plasticity-interface interaction mechanism limit further optimization of *** this study,the FeCoNi/Ni3Ti interface-mediated plastic deformation behavior in PMPEA and the variation of mechanical and tribological properties with lamella thickness within the nanoscale range using molecular dynamics（MD） simulation were *** results indicate that the mechanical and tribological properties of the PMPEA with lamella thicknesses below 10 nm have a significant inverse size effect,i.e.,the smaller the lamella thickness,the weaker the *** is because the plastic carrier-interface interaction mechanism changes from a strengthening mechanism that hinders dislocations to a weakening mechanism that promotes dislocations with the decreases in the lamella thickness,and the weakening effect becomes more pronounced as the lamella thickness decreases and the number of interfaces *** particular,the deformation behavior of Ni3Ti lamellae changes from crystal-like to amorphous-like with decreasing ***,in the sample with larger lamella thickness,the occurrence of hierarchical slips in the body-centered cubic（BCC） phase due to the multiprincipal elements effect can better alleviate the stress concentration caused by the dislocation accumulation at the interface,so that the phase interface exhibits outstanding load-bearing *** the dislocation pattern in BCC phase shows a firm high-density cell,which makes the substrate exhibit a stable tribological response.

关键词： Multi-principal element alloy Nano-laminated structure Molecular dynamics simulation Nanoindentation and nanoscratch

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Emerging mechanisms and implications of c GAS-STING signaling in cancer immunotherapy strategies

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Cancer Biology & Medicine 2024年第1期21卷 45-64页

作者： Jiawen Zhang Sihui Yu qiao peng Ping Wang Lan Fang Tongji University Cancer Center Shanghai Tenth People’s HospitalSchool of MedicineTongji UniversityShanghai 200072China Reproductive Medicine Center Department of Obstetrics and GynecologyShanghai General HospitalShanghai Jiao Tong University School of MedicineShanghai 201620China Department of Obstetrics and Gynecology Zhongshan HospitalFudan UniversityShanghai 200032China

The intricate interplay between the human immune system and cancer development underscores the central role of immunotherapy in cancer *** this landscape,the innate immune system,a critical sentinel protecting against tumor incursion,is a key *** cyclic GMP-AMP synthase(c GAS)and stimulator of interferon genes(STING)pathway has been found to be a linchpin of innate immunity:activation of this signaling pathway orchestrates the production of type I interferon(IFN-α/β),thus fostering the maturation,differentiation,and mobilization of immune effectors in the tumor ***,STING activation facilitates the release and presentation of tumor antigens,and therefore is an attractive target for cancer *** strategies to activate the STING pathway,including use of pharmacological agonists,have made substantial advancements,particularly when combined with immune checkpoint *** approaches have shown promise in preclinical and clinical settings,by enhancing patient survival *** review describes the evolving understanding of the c GAS-STING pathway's involvement in tumor biology and ***,this review explores classical and non-classical STING agonists,providing insights into their mechanisms of action and potential for optimizing immunotherapy *** challenges and complexities,the c GAS-STING pathway,a promising avenue for enhancing cancer treatment efficacy,has the potential to revolutionize patient outcomes.

关键词： cGAS-STING pathway type I interferon cyclic dinucleotide STING agonist cancer immunotherapy

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