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Catalytically generated noncovalent ammonium dienolate:a versatile platform for the development of organocatalytic asymmetric cascade reactions

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Science China Chemistry 2024年第8期67卷 2524-2546页

作者： Jun-Bing Lin Dong-sheng Ji Peng-Fei Xu State Key Laboratory of Applied Organic Chemistry College of Chemistry and Chemical EngineeringLanzhou UniversityLanzhou 730000China Shaanxi Key Laboratory of Chemical Reaction Engineering College of Chemistry and Chemical EngineeringYan’an UniversityYan’an 716000China

Organocatalytic cascade reactions represent a powerful strategy for the rapid construction of complex chiral molecules with multiple stereocenters from simple substrates under mild conditions. The intriguing structural feature and diverse reactivity of catalytically generated dienolate species render them competent and versatile intermediates for the development of practical and valuable cascade reactions. Over the past years, a plethora of innovative and pioneering noncovalent ammonium dienolatemediated cascade reactions have been designed and implemented under the catalysis of chiral organocatalysts, making dienolate activation a general, robust, and complementary method for the functionalization of unsaturated carbonyl compounds and related substances. This review illustrates the recent advances in organocatalytic noncovalent ammonium dienolate-mediated cascade reactions(mainly from 2010 to 2023), including the cascade transformations of ammonium dienolates directly generated from unsaturated ketone/aldehyde, ester/lactone/azlactone, amide/lactam/pyrazolone/oxindole, and alkylidene nitrile compounds. The contents are arranged based on the reaction types of the ammonium dienolates, with an emphasis on cascade 2,5-, 3,5-, and 4,5-difunctionalizations of these intermediates. Furthermore, other cascade reactions involving the 1,3-, 2,3-, and even more complex 3,4,5-reactivities of ammonium dienolates were also discussed. The reaction pathway, reaction stereoinduction, and synthetic applications of the ammonium dienolate-mediated cascade reactions were highlighted throughout the article. As a stimulating and ever-growing research area, the organocatalytic noncovalent ammonium dienolate-mediated cascade reactions are expected to continue demonstrating their magic power for constructing chiral targets in the future and further expanding the boundaries of asymmetric catalysis.

关键词： organocatalysis asymmetric catalysis ammonium dienolate cascade reaction difunctionalization

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Exoskeleton active assistance strategy for human muscle activation reduction during linear and circular walking

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Advances in Manufacturing 2024年第3期12卷 484-496页

作者： Wen-Tao sheng Ke-Yao Liang Hai-Bin Tang School of Intelligent Manufacturing Nanjing University of Science and TechnologyNanjing210094People’s Republic of China School of Mechatronics Engineering Harbin Institute of TechnologyHarbin150001People’s Republic of China

The exoskeleton is employed to assist humans in various domains including military missions,rehabilitation,industrial operation,and activities of daily living(ADLs).Walking is a fundamental ADL,and exoskeletons are capable of reducing the activation and metabolism of lower extremity muscles through active assistance during *** improve the performance of active assistance strategy,this article proposes a framework using an active hip ***,it correlates to an already established Bayesian-based human gait recognition algorithm,with a particular focus on linear and circular walking within industrial and ADL *** theorizing this strategy for exoskeletons,this study further reveals,in part,the activation characteristics of human hip muscles for the instruction and regulation of active assistance duration and onset *** proposed active assistance strategy provides new insights for enhancing the performance of assistive robots and facilitating human robot interaction within the context of ADLs.

关键词： Human-robot interaction Hip exoskeleton Muscle activation Walking assistance

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Upper-rim-modified thioether thiacalix[4]arene used for liquid-liquid extraction of Au(Ⅲ)and Pd(Ⅱ)in hydrochloric acid medium

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Chinese Journal of Chemical Engineering 2024年第2期66卷 110-118页

作者： sheng Wan Rong Xie Jianhong Fan Kewen Tang Department of Chemistry and Chemical Engineering Hunan Institute of Science and TechnologyYueyang 414006China

Gold(Au)and palladium(Pd)play an increasing role in the production and human life;Therefore,it is of great significance to study their recovery.A 5,11,17,23-tetra-ethylthio-25,26,27,28-tetra-hydroxyl thiacalix[4]arene(TCAET)was synthesized specifically for the capture of Au(Ⅲ)and Pd(Ⅱ)from HCl medium by liquid-liquid *** a 0.1 mol·L^(-1)HCl medium,the transfer of Au(Ⅲ)and Pd(Ⅱ)from the aqueous phase to the organic phase was highly efficient,with a transfer ratio of 100%for Au(Ⅲ)and 98%for Pd(Ⅱ).Furthermore,the extraction equilibrium time for Au(Ⅲ)was just 5 ***'s method data demonstrated that TCAET formed complexes with Au(Ⅲ)and Pd(Ⅱ)in a ratio of 2:3 and 1:1,respectively,during the extraction *** showed high selectivity toward Pd(Ⅱ)and Au(Ⅲ)over other competing metal ***,both Au(Ⅲ)and Pd(Ⅱ)could be successfully stripped from the loaded organic phases with a 1.0 mol·L^(-1)thiourea in 0.5 mol·L^(-1)HCl and 0.5 mol·L^(-1)thiourea in 0.5 mol·L^(-1)HCl,*** obtained from five consecutive extraction-stripping cycles showed good reusability of TCAET toward Au(Ⅲ)and Pd(Ⅱ)*** conclusion can provide a certain reference for thiacalixarene in the recovery of precious metal species.

关键词： Thiacalixarene Upper-rim modification Liquid-liquid extraction Precious metal Thioether

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Radical involved reactive wetting and retarding mechanism of alumina refractory ceramic by molten slags under weak static magnetic field

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Journal of Iron and Steel Research International 2024年第6期31卷 1355-1366页

作者： sheng-hao Li Ao Huang Fan-bo Zeng Hui Peng Hao-ran Wei Xue-chun Huang sheng-qiang Song Hua-zhi Gu The State Key Laboratory of Refractories and Metallurgy Wuhan University of Science and TechnologyWuhan 430081HubeiChina

High alumina slag will cause severe corrosion at the interface of alumina refractory,and the wetting behavior of slag is a key factor influencing the corrosion resistance of refractory *** static magnetic field is a promising solution for improvement in the slag resistance of *** wetting of alumina refractory ceramics with different basicities of high alumina slags under a weak static magnetic field was analyzed,given that a weak static magnetic field can affect the corrosion behavior of refractory *** slag S_(3) as an example,when there was an external static magnetic field of 1.0 mT at 1600 ℃,the thickness of calcium aluminate reaction layer at the interface decreased by 36.7%,the denting depth of interface decreased by 35.6%,and the apparent wetting angle increased by 20%.The living radicals and their formation path in oxide melts were verified by first-principles calculation combined with electron paramagnetic resonance spectroscopy *** influence of the flux density of a weak static magnetic field on the wetting behavior of slags was also *** contact angle of the slags increased owing to the inhibitory effect of magnetic field on the radicalinvolved reaction at the interface of the slag and the alumina refractory *** relationships between the magnetic flux density,diffusion coefficient,slag microstructure(hyperfine coupling constant),and contact angle were *** provides a theoretical basis for the field control of radical involved reactive wetting between inorganic oxide slags and solid oxide ceramics.

关键词： Alumina refractory ceramic Molten slag Weak magnetic field effect Reactive wetting Free radical

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Interregional compensation for farmland protection:From the perspective of farmland allocation optimization

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Journal of Geographical Sciences 2024年第7期34卷 1437-1454页

作者： YANG Bohan sheng Siyu SHANGGUAN Ziheng KE Xinli School of Public Administration Central China Normal UniversityWuhan430079China School of Business Hubei UniversityWuhan430000China College of Public Administration Huazhong Agricultural UniversityWuhan430070China

Interregional compensation for farmland protection(IRCFP)is a policy instrument for encouraging farmland protection through interregional fiscal transfer *** practices and studies on IRCFP have generally determined the payers and recipients of compensation based on the present distribution of farmland,and the compensation standards did not combine farmland development right value with farmland deficit and surplus,resulting in insignificant effects on farmland protection and even policy ***,in this study,we proposed an interregional compensation mechanism for farmland protection based on farmland allocation optimization by considering 31 provincial-level regions in *** results showed that(1)the determination of farmland surplus or deficit areas based on farmland allocation optimization met the regional construction land demand from the perspective of achieving food security.(2)The combination of the compensation value standard and cropland deficit and surplus had a positive effect on farmland protection.(3)Interregional compensation for farmland protection based on farmland allocation optimization can coordinate economic development,farmland protection,and ecological ***,we discussed the rationality of interregional compensation for farmland protection based on farmland allocation optimization and designed the operation mechanism of IRCFP.

关键词： interregional compensation farmland allocation optimization farmland protection land development rights China

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Snowpack variations and their hazardous effects under climate warming in the central Tianshan Mountains

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Advances in Climate Change Research 2024年第3期15卷 442-451页

作者： Jian-sheng HAO Yan WANG Lan-Hai LI Key Laboratory of Land Surface Pattern and Simulation Institute of Geographic Sciences and Natural Resources ResearchChinese Academy of Sciences(CAS)Beijing 100101China Xinjiang Key Laboratory of Water Cycle and Utilization in Arid Zone Urumqi 830011China State Key Laboratory of Desert and Oasis Ecology Xinjiang Institute of Ecology and GeographyChinese Academy of SciencesUrumqi 830011China Tianshan Snowcover and Avalanche Observation and Research Station of Xinjiang Xinyuan 835800China CAS Research Center for Ecology and Environment of Central Asia Urumqi 830011China

Climate change alters snowpack evolution,which in turn influences the likelihood of snow avalanches and flood *** lack of systemic observational data on key snow characteristics in high mountains remains a scientific challenge in terms of systematically elucidating the dynamic chain of variations in climate-snowpack-snow *** restricts our understanding and poses challenges in the prediction of snow-related disaster *** such,this study analysed the variations of temperature and snowfall and the physical characteristics of snowpacks based on ground-based observations from the Kunse River Valley situated in the Tianshan Mountains from 1967 to *** results reveal that the temperature increased significantly by 0.32°C per decade(p<0.01)during the snow season,along with more extreme snowfall *** snow-cover duration was observed to have been shortened by 4.77 d per decade(p<0.01)from 1967 to 2021,which is characterised by later snow-cover onset and earlier ***,average and maximum snow depths increased along with an increase in peak snow water equivalent,thus indicating a higher frequency of extremely scarce or abundant snow *** low snowpack temperature gradient and earlier snowmelt dates in spring lead to earlier occurrences of snowmelt floods and wet *** the risks of these events increase,they pose greater threats to farmlands,road transportation,water-electricity infrastructure and several other human ***,these insights are critical for providing vital information that can deepen our understanding of the impact of climate change on snowpack characteristics and improve management strategies for snow-related disaster prevention and mitigation.

关键词： Climate change Snowpack variations Snow-related disaster Tianshan Mountains

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靶向BRD4的ATTECs设计、合成与降解活性研究

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药学实践与服务 2023年第1期41卷 18-25页

作者：周洛竹盛春泉海军军医大学药学系药物化学教研室上海200433

目的基于自噬小体绑定化合物(ATTEC)策略,设计并合成靶向BRD4的自噬降解剂,验证其降解活性。方法以化合物伊斯平斯(ispinesib)为LC3配体,通过不同长度的linker与化合物JQ1相连,产物结构经1H NMR、13C NMR与ESI-MS确证,并使用蛋白印迹法(... 详细信息

目的基于自噬小体绑定化合物(ATTEC)策略,设计并合成靶向BRD4的自噬降解剂,验证其降解活性。方法以化合物伊斯平斯(ispinesib)为LC3配体,通过不同长度的linker与化合物JQ1相连,产物结构经1H NMR、13C NMR与ESI-MS确证,并使用蛋白印迹法(Western Blot)技术测试其在不同细胞系中诱导BRD4的降解活性。结果获得5个首次报道的BRD4-ATTEC分子,化合物4在不同细胞系中显示出一定的BRD4降解活性。结论本研究发现了新型BRD4自噬降解剂,拓展了靶向自噬降解的适用范围。

关键词：自噬小体绑定化合物 BRD4 LC3蛋白伊斯平斯

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Electrochemical Mono-Deuterodefluorination of Trifluoromethyl Aromatic Compounds with Deuterium Oxide

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CCS Chemistry 2024年第1期6卷 230-240页

作者： Jie sheng Xu Cheng Institute of Chemistry and Biomedical Sciences Jiangsu Key Laboratory of Advanced Organic MaterialsSchool of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210023 State Key Laboratory of Elemento-Organic Chemistry Nankai UniversityTianjin 30071

The deuterodifluoromethyl group CF_(2)D combines the structural features of CF_(3) and CD_(3) groups,finding wide applications in diverse pharmaceutical *** this work,the electrochemical monodeuterodefluorination of Ar-CF_(3) to Ar-CF_(2)D is achieved with an unreported deuterium atom transfer-coupled electron transfer pathway using D_(2)O as the only D source for the first time.A series of Ar-CF_(3) substances,including commercial pharmaceuticals,were converted to corresponding CF_(2)D products in up to 91% yield and 97% D-incorporation.A variety of functional groups,including pyridine,pyrrole,furan,thiophene,borate,thio ether,amine,amide,sulfonamide,and halide,are well tolerated in this protocol.t-BuOLi was an essential reagent to achieve chemoselective mono-defluorination.

关键词： electrochemistry C-F activation fluorinecontaining drugs deuterated drugs deuterium oxide

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A CSMA/CA based MAC protocol for hybrid Power-line/Visible-light communication networks:Design and analysis

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Digital Communications and Networks 2024年第2期10卷 481-497页

作者： sheng Hao Huyin Zhang Fei Yang Chenghao Li Jing Wang School of Computer Science Central China Normal UniversityWuhan430079PR China Hubei Key Laboratory of intelligent Robot(Wuhan Institute of Technology) Wuhan430079PR China School of Computer Science Wuhan UniversityWuhan430079China School of Information Science and Engineering Shandong Normal UniversityJinan250000China School of Computer Science Hubei University of TechnologyWuhan430079China

Hybrid Power-line/Visible-light Communication(HPVC)network has been one of the most promising Cooperative Communication(CC)technologies for constructing Smart Home due to its superior communication reliability and hardware *** research on HPVC networks focuses on the performance analysis and optimization of the Physical(PHY)layer,where the Power Line Communication(PLC)component only serves as the backbone to provide power to light Emitting Diode(LED)*** designing a Media Access Control(MAC)protocol remains a great challenge because it allows both PLC and Visible Light Communication(VLC)components to operate data transmission,i.e.,to achieve a true HPVC network *** solve this problem,we propose a new HPC network MAC protocol(HPVC MAC)based on Carrier Sense Multiple Access/Collision Avoidance(CSMA/CA)by combining IEEE 802.15.7 and IEEE 1901 ***,we add an Additional Assistance(AA)layer to provide the channel selection strategies for sensor stations,so that they can complete data transmission on the selected channel via the specified CSMA/CA mechanism,*** on this,we give a detailed working principle of the HPVC MAC,followed by the construction of a joint analytical model for mathematicalmathematical validation of the HPVC *** the modeling process,the impacts of PHY layer settings(including channel fading types and additive noise feature),CSMA/CA mechanisms of 802.15.7 and 1901,and practical configurations(such as traffic rate,transit buffer size)are comprehensively taken into ***,we prove the proposed analytical model has the ***,through extensive simulations,we characterize the HPVC MAC performance under different system parameters and verify the correctness of the corresponding analytical model with an average error rate of 4.62%between the simulation and analytical results.

关键词： Hybrid power-line/Visible light communication (HPVC)networks MAC protocol CSMA/CA IEEE 802.15.7 IEEE 1901 Performance analysis

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Solvent-free carbon sphere nanofluids towards intelligent lubrication regulation

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Friction 2024年第1期12卷 95-109页

作者： sheng ZHANG Wen LI Xiaoliang MA Xiaoqiang FAN Minhao ZHU Tribology Research Institute School of Mechanical EngineeringSouthwest Jiaotong UniversityChengdu 610031China Key Laboratory of Advanced Technologies of Materials Ministry of EducationSchool of Materials Science and EngineeringSouthwest Jiaotong UniversityChengdu 610031China

By simply switching the electrical circuit installed on steel/steel contact,the tribological behaviors of nanofluids(NFs)can be regulated in real time,thereby achieving the desired performance of friction reduction and wear ***,solvent-free carbon spherical nanofluids(C-NFs)were successfully prepared for intelligent lubrication regulation.C-NFs with excellent lubrication performance can immediately reduce the coefficient of friction(COF)despite applying a weak electric potential(1.5 V).Moreover,polyethylene glycol 400(PEG400)containing 5.0 wt%C-NFs remained responsive to electrical stimulation under the intermittent voltage application with an average coefficient of friction(ACOF)reduction of 20.8%over *** intelligent lubrication regulation of C-NFs under an external electric field(EEF)mainly depends on the orderly arranged double-electric adsorption film of ion canopy-adsorbed carbon spheres(CSs).The intermittent electrical application can continuously reinforce the adsorption film and its durability for real-time controlling the sliding ***-stimulation-responsive intelligent lubricants provide a new technical support for realizing intelligent stepless control of devices.

关键词： solvent-free carbon spherical nanofluids(C-NFs) intelligent lubrication regulation lubrication performance adsorption film

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