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Ru(II)-Catalyzed ortho C-h Allylation of N-Aryl-7-azaindoles with 2-Methylidene Cyclic Carbonate

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Chinese Journal of Chemistry 2024年第9期42卷 985-989页

作者： Jing Zhang Quan-Jian Luo han-Chi Wang Jin-heng Li Bo Sun State Key Laboratory Base of Eco-Chemical Engineering College of Chemical EngineeringQingdao University of Science and Technology QingdaoShandong266042China State key Laboratory of Applied Organic Chemistry Lanzhou University LanzhouGansu 7300ooChina School of Chemistry and Chemical Engineering Henan Normal UniversityXinxiangHenan 453007China

A Ru(II)-catalyzed ortho allylation reaction of N-aryl-7-azaindole with readily available 2-methylidene cyclic carbonate has been *** reaction is an effective pathway for synthesizing 7-azaindole derivatives with a wide scope of substrates and high *** addition,the method can be extended to the allylation of other heterocyclic compounds and several cyclic carbonates,highlighting the practicality of this strategy for synthesis.

关键词： Ru(II) Allylation N-Aryl-7-azaindoles Cyclic carbonates heterocyclic compounds C-h activation

Understanding the dehydrogenation properties of Mg(0001)/Mgh_(2)(110)interface from first principles

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Materials Reports(Energy) 2024年第1期4卷 89-94页

作者： Jianchuan Wang Bo han Zhiquan Zeng Shiyi Wen Fen Xu Yong Du State Key Laboratory of Powder Metallurgy Central South UniversityChangsha410083PR China Powder Metallurgy Research Institute Central South UniversityChangsha410083PR China Guangxi Key Laboratory of Information Materials Guilin University of Electronic TechnologyGuilin541004PR China

Magnesium hydride is one of the most promising solid-state hydrogen storage materials for on-board *** desorption from Mgh_(2) is accompanied by the formation of the Mg/Mgh_(2) interfaces,which may play a key role in the further dehydrogenation *** this work,first-principles calculations have been used to understand the dehydrogenation properties of the Mg(0001)/Mgh_(2)(110) *** is found that the Mg(0001)/Mgh_(2)(110) interface can weaken the Mg-h *** removal energies for hydrogen atoms in the interface zone are significantly lower compared to those of bulk Mgh_(2).In terms of h mobility,hydrogen diffusion within the interface as well as into the Mg matrix is *** calculated energy barriers reveal that the migration of hydrogen atoms in the interface zone is easier than that in the bulk Mgh_(2).Based on the hydrogen removal energies and diffusion barriers,we conclude that the formation of the Mg(0001)/Mgh_(2)(110) interface facilitates the dehydrogenation process of magnesium hydride.

关键词： Magnesium hydrides First-principles calculation hydrogen storage materials Interface hydrogen desorption

Parallelogram 3d-4f-5d heterometallic clusters based on trilacunary tungstoantimonates with excellent proton conductivity

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Chinese Chemical Letters 2024年第3期35卷 528-531页

作者： haiying Wang han Xu Chaolong Chen Yingjie Zhu Yikang Zhang Dongdi Zhang Jingyang Niu henan Key Laboratory of Polyoxometalate Chemistry College of Chemistry and Molecular SciencesHenan UniversityKaifeng 475004China School of Pharmaceutical Science&Yunnan Key Laboratory of Pharmacology for Natural Products Kunming Medical UniversityKunming 650500China Collaborative Innovation Center of Chemistry for Energy Materials State Key Laboratory of Physical Chemistry of Solid Surface and Department of ChemistryCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China

Two 3d-4f-5d heterometallic cluster-containing polyoxometalates,formulated as Na_(22){(SbW_(9)O_(33))_(4)[La_(3)W_(6)MO_(18)(h_(2)O)_(8)(Ch_(3)COO)_(4)]_(2)}·nh_(2)O(abbreviated as La_(6)M_(2),M=Co/Mn)were synthesized and structurally ***-crystal X-ray diffraction analyses reveal that the polyanions of La_(6)Co_(2)and La_(6)Mn_(2)consist of the uncommon 3d-4f-5d clusters{La_(6)W_(12)Co_(2)}and{La_(6)W_(12)Mn_(2)},which are encapsulated by four trilacunary Keggin tungstoantimonates to form the parallelogram-shaped title ***,the polyanions can be extended into a two-dimensional(2D)frame by the linkage of peripheral Na+*** inner space of the 2D layer was filled with water molecules and thus an h-bonded network was formed,which is expected to exhibit a fascinating proton *** study of water-assisted proton conduction demonstrated that La_(6)Co_(2)and La_(6)Mn_(2)were temperature-and humiditydependent proton conductors,respectively,and the proton conductivities could reach 1.3×10^(-2)and 2.3×10^(-2)S/cm at 65℃and 90%Rh conditions.

关键词： Polyoxometalate Parallelogram heterometallic 3d-4f-5d cluster Proton conductivity

high-performance magnesium/sodium hybrid ion battery based on sodium vanadate oxide for reversible storage of Na^(+)and Mg^(2+)

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Journal of Energy Chemistry 2024年第9期96卷 79-88页

作者： Xiaoke Wang Titi Li Xixi Zhang Yaxin Wang hongfei Li hai-Feng Li Gang Zhao Cuiping han Institute of Applied Physics and Materials Engineering University of MacaoAvenida da UniversidadeTaipaMacao 999078China School of Physics and Technology University of JinanJinan 250022ShandongChina Songshan Lake Materials Laboratory Dongguan 523808GuangdongChina Faculty of Materials Science and Energy Engineering Shenzhen University of Advanced TechnologyShenzhen 518055GuangdongChina Institute of Technology for Carbon Neutrality Shenzhen Institute of Advanced TechnologyChinese Academy of SciencesShenzhen 518055GuangdongChina

Magnesium ion batteries(MIBs)are a potential field for the energy storage of the future but are restricted by insufficient rate capability and rapid capacity ***-sodium hybrid ion batteries(MShBs)are an effective way to address these ***,we report a new type of MShBs that use layered sodium vanadate((Na,Mn)V_(8)O_(20)·5h_(2)O,Mn-NVO)cathodes coupled with an organic 3,4,9,10-perylenetetracarboxylic diimide(PTCDI)anode in Mg^(2+)/Na^(+)hybrid *** electrochemical cycling,Mg^(2+)and Na^(+)co-participate in the cathode reactions,and the introduction of Na^(+)promotes the structural stability of the Mn-NVO cathode,as cleared by several ex-situ ***,the Mn-NVO cathode presents great specific capacity(249.9 mA h g^(−1)at 300 mA g^(−1))and cycling(1500 cycles at 1500 mA g^(−1))in the Mg^(2+)/Na^(+)hybrid ***,full battery displays long lifespan with 10,000 cycles at 1000 mA g^(−1).The rate performance and cycling stability of MShBs have been improved by an economical and scalable method,and the mechanism for these improvements is discussed.

关键词： Aqueous battery hybrid ion battery Mg^(2+)/Na^(+)co-intercalation high-rate performance Organic-water hybrid electrolyte

Experimental Investigation on heat Transfer and Combustion of a Stirling Engine Combustor Fueled by Reformed Gas and Diesel Fuel

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Journal of Thermal Science 2024年第5期33卷 1907-1919页

作者： LAN Jian ZhAO Yanchun LIN Guangtao LI Yelin REN Zhe LYU Tian ShEN Mengmeng GU Genxiang han Dong Key Laboratory for Power Machinery and Engineering Ministry of EducationShanghai Jiao Tong UniversityShanghai200240China Shanghai Marine Diesel Engine Research Institute Shanghai 201108China

Thermochemical recuperation heat recovery is an advanced waste heat utilization technology that can effectively recover exhaust waste heat from oxy-fuel Stirling *** novel combustor of a Stirling engine with thermochemical recuperation heat recovery system is expected to utilize both reformed gas and diesel fuels as sources of *** this research,the effects of various factors,including the h_(2)O addition,fuel distribution ratio(FDR),excess oxygen coefficient,and cyclone structure on the temperature distribution in the combustor,combustion emissions,and external combustion system efficiency of the Stirling engine were experimentally *** the increase of steam-to-carbon ratio(S/C),the temperature difference between the upper and lower heating tubes reduces and the circumferential temperature fluctuation decreases,and the combustion of diesel and reformed gas remains close to complete *** S/C=2,the external combustion efficiency is 80.6%,indicating a 1.6%decrease compared to conventional *** the increase of FDR,the temperature uniformity of the heater tube is improved,and the CO and hC emissions ***,the impact of the FDR on the maximum temperature difference and temperature fluctuation across the heater is *** the FDR rises from 21%to 38%,the external combustion efficiency increases from 87.4%to92.3%.The excess oxygen coefficient plays a secondary role in influencing temperature uniformity and temperature difference,and the reformed gas and diesel fuel can be burned efficiently at a low excess oxygen coefficient of *** an increase in the cyclone angle,the heater tube temperature increases,while the maximum temperature difference at the lower part decreases,and the temperature fluctuation ***,the CO and hC emissions increase,and the external combustion efficiency experiences a decrease.A cyclone angle of 30°is found to be an appropriate value for achieving optimal

关键词： Stirling engine fuel reforming synthetic gas oxy-combustion external combustion efficiency

Lignin-reinforced PVDF electrolyte for dendrite-free quasi-solid-state Li metal battery

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Rare Metals 2024年第3期43卷 1006-1016页

作者： Xin-Yang Chen Xue-Jie Gao han-Yan Wu Yu-Long Liu Xiao-Fei Yang Run-Cang Sun Center for Lignocellulosic Chemistry and Biomaterials College of Light Industry and Chemical EngineeringDalian Polytechnic UniversityDalian116034China Division of Energy Storage Dalian National Laboratory for Clean EnergyDalian Institute of Chemical PhysicsChinese Academy of SciencesDalian116023China School of Chemistry Northeast Normal UniversityChangchun130024China

Quasi-solid-state lithium metal batteries(QSSLMBs)assembled with polyvinylidene fluoride(PVDF)are a promising class of next-generation rechargeable batteries due to their safety,high energy density,and superior interfacial ***,PVDF has a series of inherent drawbacks such as low ionic conductivity,ease of crystallization,and hydrophobic character that leading to poor cell *** tackle these issues,a lignin-reinforced PVDF electrolyte is proposed in this work to solve these drawbacks of PVDF and enhance the comprehensive performance of *** lithophilic polar groups of lignin can promote uniform deposition of Li on the *** with the improved mechanical properties can efficiently prevent Li dendrites penetration through the *** addition,more active sites provided by lignin can also enhance Li^(+)transport and lead to a faster electrochemical reaction *** from the ingenious design,Li symmetric cells with 5%lignin-PVDF quasi-solid-state electrolyte can operate for 900 h at a high current density/capacity of 5 mA·cm^(-2)/5 mAh·cm^(-2),while shortcircuiting occurs after 56 h for the counterpart(pure PVDF).Moreover,a full cell of Li/5%lignin-PVDF/LFP cell demonstrates a high capacity of 96.2 mAh·g^(-1)after 2000 cycles at 10 *** work is expected to open up promising opportunities to develop other high-energy/power-density QSSLMBs.

关键词： Quasi-solid-state electrolyte Lignin PVDF Dendrite-free Li metal battery

Construction of MnS/MoS_(2) heterostructure on two-dimensional MoS_(2) surface to regulate the reaction pathways for high-performance Li-O_(2) batteries

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Journal of Energy Chemistry 2024年第6期93卷 443-452,I0012页

作者： Guoliang Zhang han Yu Xia Li Xiuqi Zhang Chuanxin hou Shuhui Sun Yong Du Zhanhu Guo Feng Dang Key Laboratory for Liquid-Solid Structure Evolution and.Processing of Materials(Ministry of Education) Shandong UniversityJinan 250061ShandongChina School of Environmental and Material Engineering Yantai UniversityYantai 264005ShandongChina Institute National de la Recherche Scientifique CentreÉnergie Matériaux et TélécommunicationsVarennesQuébec J31S2Canada State Key Laboratory of Powder Metallurgy Central South UniversityChangsha 410083HunanChina Integrated Composites Lab Department of Mechanical and Construction EngineeringNorthumbria UniversityNewcastle Upon TyneNE18STUK

The inherent catalytic anisotropy of two-dimensional(2D) materials has limited the enhancement of LiO_(2) batteries(LOBs) performance due to the significantly different adsorption energies on 2D and edge *** the adsorption strength in 2D materials to the reaction intermediates is essential for achieving high-performance ***,a MnS/MoS_(2) heterostructure is designed as a cathode catalyst by adjusting the adsorption behavior at the *** from the toroidal-like discharge products on the MoS_(2) cathode,the MnS/MoS_(2) surface displays an improved adsorption energy to reaction species,thereby promoting the growth of the film-like discharge *** can disturb the layer growth of MoS_(2),in which the stack edge plane features a strong interaction with the intermediates and limits the growth of the discharge *** and theoretical results confirm that the MnS/MoS_(2) heterostructure possesses improved electron transfer kinetics at the interface and plays an important role in the adsorption process for reaction species,which finally affects the morphology of Li_2O_(2),In consequence,the MnS/MoS_(2) heterostructure exhibits a high specific capacity of 11696.0 mA h g^(-1) and good cycle stability over 1800 h with a fixed specific capacity of 600 mA h g^(-1) at current density of100 mA g^(-1) This work provides a novel interfacial engineering strategy to enhance the performance of LOBs by tuning the adsorption properties of 2D materials.

关键词： Li-O_(2)batteries Two-dimensional materials MnS/MoS_(2)heterostructure Edge plane Adsorption behavior

In Situ high-performance Gel Polymer Electrolyte with Dual-reactive Cross-linking for Lithium Metal Batteries

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Energy & Environmental Materials 2024年第1期7卷 51-59页

作者： Fuhe Wang honghao Liu Yaqing Guo Qigao han Ping Lou Long Li Jianjie Jiang Shijie Cheng Yuancheng Cao School of Materials Science and Engineering huazhong University huazhong University of Science and Technology Wuhan 430074China State Key Laboratory of Advanced Electromagnetic Engineering and Technology School of Electrical and Electronic Engineering Huazhong University of Science and TechnologyWuhan 430074China State Grid huzhou Power Supply Company Huzhou 313000China huzhou Electric Power Design Institute Company Huzhou 311404China

Lithium metal batteries have been considered as one of the most promising next-generation power-support devices due to their high specific energy and output ***,the uncontrollable side-reaction and lithium dendrite growth lead to the limited serving life and hinder the practical application of lithium metal ***,a tri-monomer copolymerized gel polymer electrolyte(TGPE)with a cross-linked reticulation structure was prepared by introducing a cross-linker(polyurethane group)into the acrylate-based in situ polymerization *** soft segment of polyurethane in TGPE enables the far migration of lithium ions,and the-Nh forms hydrogen bonds in the hard segment to build a stable cross-linked *** system hinders anion migration and leads to a high Li^(+)migration number(t_(Li^(+))=0.65),which achieves uniform lithium deposition and effectively inhibits lithium dendrite *** a result,the assembled symmetric cell shows robust reversibility over 5500 h at a current density of 1 mA cm^(-2).The LFP∷TGPE∷Li cell has a capacity retention of 89.8%after cycling 800 times at a rate of *** summary,in situ polymerization of TGPE electrolytes is expected to be a candidate material for high-energy-density lithium metal batteries.

关键词： gel polymer electrolytes hydrogen bonds in situ polymerization lithium metal batteries polyurethane

Optimizing 2D-metal contact in layered Tin-selenide via native oxide modulation

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Nano Research 2024年第4期17卷 3014-3020页

作者： Yue Zheng Qi You Zhentian Yin Jian Tang Ke Jiang Zihao Xie henan Li Cheng han Yumeng Shi International Collaborative Laboratory of 2D Materials for Optoelectronics Science and Technology of Ministry of Education Institute of Microscale OptoelectronicsShenzhen UniversityShenzhen 518060China College of Electronics and Information Engineering Shenzhen UniversityShenzhen 518060China

The discovery of two-dimensional(2D)semiconductor has opened up new avenues for the development of short-channel field-effect transistors(FETs)with desired electrical *** them,orthorhombic tin-selenide(SnSe)has garnered increasing attention due to its potential applications in a variety of electronic,optoelectronic,and thermoelectric ***,the realization of high-performance SnSe FETs with low contact resistance(Rc)remains a ***,we systematically investigate the contact of few-layer SnSe FETs through the modulation of native oxide on SnSe by using different *** is found that chromium(Cr)-contacted devices possess the best FET performance,such as electron mobility up to 606 cm^(2)/(V·s)at 78 K,current on/off ratio exceeding 1010,and saturation current of~550μA/μm,where a negligible Schottky barrier(SB)of~30 meV and a low contact resistance of~425Ωμm are achieved.X-ray photoelectron spectroscopy(XPS)and cross-sectional electron dispersive X-ray spectroscopy(EDX)results further reveal that the improved contact arises from the Cr-induced reduction of native oxide(SnOx)to Sn,which thins the tunneling barrier for efficient electron *** findings provide a deep insight into the 2D-metal contact of SnSe and pave the way for its applications in future nanoelectronics.

关键词： few-layer SnSe field-effect transistors(FETs) Cr contact native oxide contact resistance(Rc) Schottky barrier(SB)