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Photoinduced generation of alkyl and phthalimide nitrogen radicals from n-hydroxyphthalimide esters for the synthesis of benzophenone-type bioisosteres

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Science china chemistry 2024年第10期67卷 3389-3396页

作者： Fei Li Jianyang dong Huijuan Liao Jiayi Dang Xuechen Zhou Yuying Wang chenya Wang Qin Jiang Gang Li dong Xue Key Laboratory of Applied Surface and Colloid chemistry Ministry of Education and School of Chemistry and Chemical EngineeringShaanxi Normal University

n-Hydroxyphthalimide（nHPI） esters have emerged as powerful sources of alkyl radicals generated by single-electron transfer,but homolysis of nHPI ester to produce an alkyl radical and a phthalimide nitrogen radical is still in its infancy. In this study, we developed a light-induced method for generation of alkyl and phthalimide nitrogen radicals from nHPI esters and subsequent reactions of the radicals with [1.1.1]propellane and aryl aldehydes for rapid generation of bicycle [1.1.1]pentane ketones. This method does not require metals or photosensitizers, features a broad substrate scope（90 examples） and excellent functional group tolerance, and can be used for the functionalization of structurally complex natural products and drugs. Mechanistic investigations indicate that the reaction involves photoinduced homolytic cleavage of the Cs2CO3-nHPI ester complex to produce alkyl and phthalimide nitrogen radicals and subsequent hydrogen atom transfer between the phthalimide nitrogen radical and the aldehyde to generate an acyl radical.

关键词： phthalimide nitrogen radicals aryl aldehydes hydrogen atom transfer bicycle[1.1.1]pentane ketones bioisosteres

An intelligent active probing and trace-back scheme for IoT anomaly detection

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Digital Communications and networks 2024年第1期10卷 168-181页

作者： Luying Wang Lingyi chen neal n.Xiong Anfeng Liu Tian Wang Mianxiong dong School of Computer Science and Engineering Central South UniversityChangsha 410083China Department of Computer Science and Mathematics Sul Ross State UniversityAlpineTX 79830USA Artificial Intelligence and Future networks Beijing Normal University&UICZhuhai 519087China Department of Information and Electronic Engineering Muroran Institute of TechnologyMuroran 050-8585Japan

Due to their simple hardware,sensor nodes in IoT are vulnerable to attack,leading to data routing blockages or malicious tampering,which significantly disrupts secure data *** Intelligent Active Probing and Trace-back Scheme for IoT Anomaly Detection(APTAD)is proposed to collect integrated IoT data by recruiting Mobile Edge Users(MEUs).(a)An intelligent unsupervised learning approach is used to identify anomalous data from the collected data by MEUs and help to identify anomalous nodes.(b)Recruit MEUs to trace back and propose a series of trust calculation methods to determine the trust of nodes.(c)The last,the number of active detection packets and detection paths are designed,so as to accurately identify the trust of nodes in IoT at the minimum cost of the network.A large number of experimental results show that the recruiting cost and average anomaly detection time are reduced by 6.5 times and 34.33%respectively,while the accuracy of trust identification is improved by 20%.

关键词： Anomaly detection Internet of things Integrating data collection Mobile edge users Intelligent

Boosted Lithium-Ion Transport Kinetics in n-Type Siloxene Anodes Enabled by Selective nucleophilic Substitution of Phosphorus

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nano-Micro Letters 2024年第10期16卷 618-637页

作者： Se In Kim Woong-Ju Kim Jin Gu Kang dong-Wan Kim School of Civil Environmental and Architectural EngineeringKorea University02841 SeoulSouth Korea nanophotonics Research Center Korea Institute of Science and Technology02792 SeoulSouth Korea

Doped two-dimensional(2D)materials hold significant promise for advancing many technologies,such as microelectronics,optoelectronics,and energy ***,n-type 2D oxidized Si nanosheets,namely n-type siloxene(n-SX),are employed as Li-ion battery *** thermal evaporation of sodium hypophosphite at 275℃,P atoms are effectively incorporated into siloxene(SX)without compromising its 2D layered morphology and unique Kautsky-type crystal ***,selective nucleophilic substitution occurs,with only Si atoms being replaced by P atoms in the O_(3)≡Si-H *** resulting n-SX possesses two delocalized electrons arising from the presence of two electron donor types:(i)P atoms residing in Si sites and(ii)H *** doping concentrations are varied by controlling the amount of precursors or their mean free *** at 2000 mA g^(-1),the n-SX electrode with the optimized doping concentration(6.7×10^(19) atoms cm^(-3))delivers a capacity of 594 mAh g^(-1) with a 73%capacity retention after 500 *** improvements originate from the enhanced kinetics of charge transport processes,including electronic conduction,charge transfer,and solid-state *** approach proposed herein offers an unprecedented route for engineering SX anodes to boost Li-ion storage.

关键词： Li-ion battery Two-dimensional n-type siloxene Doping mechanism Kinetics

Geochemistry and mineral chemistry of the armoor granitoids,eastern dharwar craton: implications for the redox conditions and tectono-magmatic environment

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Acta Geochimica 2024年第1期43卷 110-133页

作者： A.Ajay Kumar ch.Ashok Department of Geology Osmania UniversityHyderabad 500007India CSIR-national Geophysical Research Institute UppalHyderabad 500007India

The mineralogical and geochemical characteristics of the K-rich granites from the Armoor granitic rocks in the northeastern portion of the Eastern Dharwar Craton(EDC) are *** order to understand its physicochemical conditions,the petrogenesis of the granitoid was explained from biotite chemistry and geochemical *** of mineral chemistry expose that compositionally,K-feldspar and plagioclase in Armoor granite rocks range from An0,Ab_(3-5.9),Or_(94-96.9) and An_(5-29,-Ab71.9-94.9),Or_(0-1.5),*** mineral chemistry of biotite crystals exhibits composition that varies from primary to re-equilibrated primary *** biotites from the Armoor granites generally exhibit an I-type trend,with calc-alkaline parental magma in a subduction *** chemistry of granites displays magnetite(oxidized)series nature,which has oxygen fugacity(fO_(2))=-15.1 to-16.7(log_(10) bar),under high oxidizing *** and pressure estimates for the crystallization of Armoor granites based on biotite composition are T=612-716 ℃ and 1.0-0.4 kbar,***,these rocks are metaluminous to slightly peraluminous and magnesian,with calc-alkaline potassiumrich *** the chondrite normalized REE diagram,the granites have positive europium anomalies;rich Sr/Y,(Dy/Yb)_(n) ratios and reduced Mg#,Rb/Sr,Rb,Sr indicate that the melting of earlier rocks,crystal accumulation and residual garnet source formed at high *** examined granites show that they are produced from the melting of crustal ***,the extensive analyses of the described Armoor granite suggest that they were produced by crust sources and developed under oxidizing conditions in subduction setting.

关键词： Armoor granites Oxygen fugacity Crystal accumulation Remelting Subduction

Prediction and interpretation of photocatalytic nO removal on g-C_(3)n_(4)-based catalysts using machine learning

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chinese chemical Letters 2024年第2期35卷 477-483页

作者： Jing Li Xinyan Liu Hong Wang Yanjuan Sun Fan dong School of Resources and Environment University of Electronic Science and Technology of ChinaChengdu 611731China Research Center for Carbon-neutral Environmental & Energy Technology Institute of Fundamental and Frontier SciencesUniversity of Electronic Science and Technology of ChinaChengdu 611731China

Predictive modeling of photocatalytic nO removal is highly desirable for efficient air pollution ***,great challenges remain in precisely predicting photocatalytic performance and understanding interactions of diverse features in the catalytic ***,a dataset of g-C_(3) n_(4)-based catalysts with 255 data points was collected from peer-reviewed publications and machine learning(ML)model was proposed to predict the nO removal *** result shows that the Gradient Boosting Decision Tree(GBDT)demonstrated the greatest prediction accuracy with R 2 of 0.999 and 0.907 on the training and test data,*** SHAP value and feature importance analysis revealed that the empirical categories for nO removal rate,in the order of importance,were catalyst characteristics>reaction process>preparation ***,the partial dependence plots broke the ML black box to further quantify the marginal contributions of the input features(e.g.,doping ratio,flow rate,and pore volume)to the model output *** ML approach presents a pure data-driven,interpretable framework,which provides new insights into the influence of catalyst characteristics,reaction process,and preparation conditions on nO removal.

关键词： Machine learning g-C_(3)n_(4)-based catalysts nO removal Interpretability Catalytic informatics

A n-CoSe/CoSe_(2)-C@Cu hierarchical architecture as a current collector-integrated anode for potassium-ion batteries

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Rare Metals 2024年第8期43卷 3702-3712页

作者： Zi-Jie Mu Yan-Jun Gao Wen-Shuai dong Zong-You Li Qing-Yi Song Han-Jiao Huang Li-dong Xing Jian-Guo Zhang Wei Wang Qi-Yao Yu State Key Laboratory of Explosion Science and Technology School of Mechatronical EngineeringBeijing Institute of TechnologyBeijing 100081China School of Metallurgical and Ecological Engineering University of Science and Technology BeijingBeijing 100083China

The highly reversible insertion/extraction of large-radius K^+into electrode materials remains a tough goal,especially for con version-type ***,we design a current collector-integrated electrode(n-CoSe/CoSe_(2)-C@Cu) as an advanced anode for potassium-ion battery(PIBs).The conductive CoSe/CoSe_(2) heterojunction with rich Se vacancy defects,conductive sp^2 n-doped carbon layer,and the elastic copper foil matrix can greatly accelerate the electron transfer and enhance the structural ***,the well-designed n-CoSe/CoSe_(2)-C@Cu current collector-integrated electrode displays enhanced potassium storage performance with regard to a high capacity(325.1 mAh·g^(-1) at 0.1 A·g^(-1) after 200cycles),an exceptional rate capability(223.5 mAh·g^(-1) at2000 mA·g^(-1)),and an extraordinary long-term cycle stability(a capacity fading of only 0.019% per cycle over1200 cycles at 2000 mA·g^(-1)).Impressively,ex situ scanning electron microscopy(SEM) characterizations prove that the elastic structure of copper foil is merged into the cleverly designed n-CoSe/CoSe_(2)-C@Cu heterostructure,which buffers the deformation of structure and volume and greatly promotes the cycle life during the potassium/depotassium process.

关键词： Potassium-ion battery Integrated collector electrode CoSe CoSe_2 Heterojunction Copper foil matrix n-doped carbon

Irreducible Representations of GL_(n)(C)of Minimal Gelfand-Kirillov Dimension

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Acta Mathematica Sinica,English Series 2024年第3期40卷 639-657页

作者： Zhan Qiang BAI Yang Yang chEn dong Wen LIU Bin Yong SUn School of Mathematical Sciences Soochow UniversitySuzhou 215006P.R.China School of Sciences JiangnanUniversityWui214122P.R.China School of Mathematical Sciences Zhejiang UniversityHangzhou 310058P.R.China Institute for Advanced Study in Mathematics Zhejiang UniversityHangzhou 310058P.R.China

In this article,by studying the Bernstein degrees and Goldie rank polynomials,we es-tablish a comparison between the irreducible representations of G=GL_(n)(C)possessing the minimal Gelfand-Kirillov dimension and those induced from finite-dimensional representations of the maximal parabolic subgroup of G of type(n-1,1).We give the transition matrix between the two bases for the corresponding coherent families.

关键词： Bernstein degree coherent continuation Gelfand-Kirillov dimension

DMPP mitigates n_(2)O and nO productions by inhibiting ammonia-oxidizing bacteria in an intensified vegetable field under different temperature and moisture regimes

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Pedosphere 2024年第3期34卷 652-663页

作者： Xi ZHAnG Xintong XU chenyuan WAnG Qianqian ZHAnG Yubing dong Zhengqin XIOnG Jiangsu Key Laboratory of Low Carbon Agriculture and GHGs Mitigation College of Resources and Environmental SciencesNanjing Agricultural UniversityNanjing 210095(China) Department of Soil Science of Temperate Ecosystems Department of Agricultural Soil ScienceGeorg-August University of GottingenGottingen 37077(Germany) State Key Laboratory of Subtropical Silviculture Zhejiang A&F UniversityHangzhou 311300(China) Huaiyin Institute of Agricultural Sciences of Xuhuai Region in Jiangsu Jiangsu Academy of Agricultural SciencesHuai’an 223001(China)

Vegetable soils with high nitrogen input are major sources of nitrous oxide(n_(2)O)and nitric oxide(nO),and incorporation of the nitrification inhibitor 3,4-dimethylpyrazole phosphate(DMPP)into soils has been documented to effectively reduce ***,the efficiency of DMPP in terms of soil n_(2)O and nO mitigations varies greatly depending on soil temperature and moisture ***,further evaluations of DMPP efficiency in diverse environments are required to encourage widespread application.A laboratory incubation study(28 d)was established to investigate the interactive effects of DMPP,temperature(15,25,and 35?C),and soil moisture(55% and 80% of water-holding capacity(WHC))on net nitrification rate,n_(2)O and nO productions,and gene abundances of nitrifiers and denitrifiers in an intensive vegetable *** showed that incubating soil with 1%DMPP led to partial inhibition of the net nitrification rate and n_(2)O and nO productions,and the reduction percentage of n_(2)O production was higher than that of nO production(69.3%vs.38.2%)regardless of temperature and soil moisture *** increased temperatures promoted the net nitrification rate but decreased soil n_(2)O and nO *** moisture influenced nO production more than n_(2)O production,decreasing with the increased moisture level(80%).The inhibitory effect of DMPP on cumulative n_(2)O and nO productions decreased with increased temperatures at 55%***,the inhibitory effect of DMPP on cumulative n_(2)O production increased with increased temperatures at 80%*** on the correlation analyses and automatic linear modeling,the mitigation of both n_(2)O and nO productions from the soil induced by DMPP was attributed to the decreases in ammonia-oxidizing bacteria(AOB)amoA gene abundance and nO_(2)^(-)-n ***,our study indicated that DMPP reduced both n_(2)O and nO productions by regulating the associated AOB amoA gene abundance and nO_(2)^(-)-n concentra

关键词： 3,4-dimethylpyrazole phosphate environment condition gene abundance nitrification inhibitor nitrite accumulation soil water content

OSDA-free synthesis of FeZSM-22 zeolite from natural minerals for n-octane hydroisomerization

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chinese Journal of chemical Engineering 2024年第2期66卷 51-59页

作者： Tiesen Li Ting chen Yinghui Ye Peng dong TinghaiWang Qingyan Cui chan Wang Yuanyuan Yue national Engineering Research Center of chemical Fertilizer Catalyst College of Chemical EngineeringFuzhou UniversityFuzhou 350002China Qingyuan Innovation Laboratory Quanzhou 362801China

A seed-directed approach to synthesizing Fe ZSM-22 zeolite without organic structure directing agent(OSDA)was developed by using Fe-rich diatomite as all aluminum and iron *** Fe ZSM-22zeolite with optimal crystallinity and purity can be obtained by systematically adjusting feed composition and synthesis *** show that Fe ZSM-22 zeolite synthesized with OSDA-free owns high crystallinity,obvious thin needle-shaped morphology and high Bronsted/Lewis acid ***,when used for n-octane hydroisomerization reaction,its derived catalyst exhibits the best catalytic performance reflected by the highest selectivity to C_(8)isomers compared to the two reference catalysts prepared based on a Fe-containing and a Fe-free ZSM-22 synthesized through an OSDA-directed route from natural diatomite and conventional chemicals,*** work provides an alternative route to sustainably synthesizing heteroatomic zeolites with high performance.

关键词： FeZSM-22 zeolite OSDA-free synthesis natural minerals n-octane hydroisomerization