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Integration of Electrical Properties and Polarization Loss Modulation on Atomic Fe–N‑RGO for Boosting Electromagnetic Wave Absorption

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Nano-Micro Letters 2025年第2期17卷 517-532页

作者： Kaili Zhang Yuefeng Yan Zhen Wang Guansheng Ma Dechang Jia Xiaoxiao Huang Yu Zhou State key laboratory of Precision Welding&Joining of materials and Structures Harbin Institute of TechnologyHarbin 150001People’s Republic of China School of materials Science and Engineering Harbin Institute of TechnologyHarbin 150001People’s Republic of China MIIT key laboratory of advanced Structural‑Functional Integration materials&Green Manufacturing Technology Harbin Institute of TechnologyHarbin 150001People’s Republic of China

Developing effective strategies to regulate graphene’s conduction loss and polarization has become a key to expanding its application in the electromagnetic wave absorption(EMWA)*** on the unique energy band structure of graphene,regulating its bandgap and electrical properties by introducing heteroatoms is considered a feasible ***,metal-nitrogen doping reduced graphene oxide(M–N-RGO)was prepared by embedding a series of single metal atoms M–N_(4) sites(M=Mn,Fe,Co,Ni,Cu,Zn,Nb,Cd,and Sn)in RGO using an N-coordination atom-assisted *** composites had adjustable conductivity and polarization to optimize dielectric loss and impedance matching for efficient EMWA *** results showed that the minimum reflection loss(RL_(min))of Fe–N-RGO reaches−74.05 dB(2.0 mm)and the maximum effective absorption bandwidth(EAB_(max))is 7.05 GHz(1.89 mm)even with a low filler loading of only 1 wt%.Combined with X-ray absorption spectra(XAFS),atomic force microscopy,and density functional theory calculation analysis,the Fe–N_(4) can be used as the polarization center to increase dipole polarization,interface polarization and defect-induced polarization due to d-p orbital hybridization and structural ***,electron migration within the Fe further leads to conduction loss,thereby synergistically promoting energy *** study demonstrates the effectiveness of metal-nitrogen doping in regulating the graphene′s dielectric properties,which provides an important basis for further investigation of the loss mechanism.

关键词： Electromagnetic wave absorption Fe-N-RGO Dipole polarization Conduction loss Impedance matching

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Synthesis,Crystal Structure and Thermal Decomposition of a New Energetic Dipotassium 3,3'-Dinitro-5,5'-bis-1,2,4-triazole-1,1'-diolate

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Chinese Journal of Structural chemistry 2017年第2期36卷 211-216页

作者：罗义芬毕福强翟连杰王锡杰廉鹏王伯周 State key laboratory of fluorine & nitrogen Chemicals Xi'an Modern Chemistry Research Institute

A new energetic dipotassium 3,3-dinitro-5,5-bis-1,2,4-triazole-1,1-diolate [K2（DNOBT）] was synthesized, and structurally characterized by elemental analysis, IR spectra, 13 C NMR and single-crystal X-ray diffraction. K2（DNOBT）·2H2O crystallizes in monoclinic system, space group P21/n with a=6.0446（10）, b=15.999（3）, c=6.4169（11） , β=99.421（2）°, V=612.21（18） 3, Z=4, Dc=2.009 g·cm（-3）, F（000）=372, μ=0.838 mm（-1）, S=1.012, the final R=0.0248 and w R（I 〉 2σ（I））=0.0604. Thermal decomposition of the title compound was studied by using DSC and TG-DTG, and there is primarily one exothermic decomposition process at 371.5 ℃.

关键词： triazole structurally monoclinic energetic acetate bonds primarily anion heating shaped

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Improved Studies on the Synthesis,Characterization and Crystal Structure of 2,2-Dimethyl-5-nitro-5-nitroso-1,3-dioxane

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Chinese Journal of Structural chemistry 2017年第3期36卷 401-408页

作者：张家荣毕福强王伯周张俊林王民昌贾思媛霍欢李祥志 State key laboratory of fluorine & nitrogen Chemical Xi'an Modern chemistry Research Institute

The synthetic process for 2,2-dimethyl-5-nitro-5-nitroso-1,3-dioxane（DMNNDO） was improved by using tri（hydroxymethyl）nitromethane and acetone as starting materials through a ＂one-pot＂ method combined with alkaline hydrolysis and nitrosation reactions. The yield of DMNNDO was increased from 37% to 45%. The structure of DMNNDO was characterized by IR,^1H NMR,^13 C NMR,and elemental analysis. Also the thermal decomposition of DMNNDO was studied by using DSC and TG-DTG to find that there are primarily two exothermic decomposition processes between 90 and 300 oC. The crystal structure of DMNNDO was studied by X-ray single-crystal diffraction for the first time. The molecular structure exists as a dimeric form due to the presence of nitroso group. The crystal belongs to monoclinic system,space group C2/c with a = 14.515（3）,b = 9.955（2）,c = 11.897（2） °,β = 98.500（3）°,V = 1.6998（2） nm^3,Z = 8,D_c = 1.486 g×cm^-3,μ = 0.128 mm^-1,F（000） = 800,S = 1.055,R = 0.0358 and wR = 0.0917. In particular,DMNNDO could be easily hydrolyzed in hydrous systems and the hydrolysis mechanism in CDCl_3 was revealed by means of NMR monitoring.

关键词： 2 2-dimethyl-5-nitro-5-nitroso-1 3-dioxane synthesis crystal structure thermal

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Access to Versatile Functionalized Cu(Ⅲ) Complexes Enabled by Direct Transmetalation to Well-Defined Copper(Ⅲ) Fluoride Complex Me_(4)N^(+)[Cu(CF_(3))_(3)F]^(-)

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Chinese Journal of chemistry 2024年第10期42卷 1107-1113页

作者： Guangyu Wang Huaiyuan Li Xuebing Leng Long Lu Qilong Shen key laboratory of fluorine and nitrogen chemistry and advanced materials Shanghai Institute of Organic ChemistryUniversity of Chinese Academy of SciencesChinese Academy of Sciences345 Lingling LuShanghai 200032China

The invention of a well-defined Cu(Ⅲ)fluoride complex Me_(4)N^(+)[Cu(CF_(3))_(3)(F)]^(-)1 enabled to access a versatile of functionalized Cu(Ⅲ)complexes[Me_(4)N]^(+)[Cu(X)(CF_(3))_(3)]^(-)(X=C_(6)F_(5),C_(6)F_(5)C≡C,CN,Cl,N_(3),^(t)BuOO,SCN,OAc,SAr),many of them for the first *** availability of these complexes allowed us to evaluate the trans-influence order of ligand in Cu(Ⅲ)complexes:Bn>CF_(3)^(-)>C_(6)F_(5)^(-)>N_(3)^(-)>py~CH_(3)^(-)~C_(6)F_(5)C≡C>NO_(2)PhO^(-)~^(t)BuOO^(-)~CH_(3)COO^(-)>F^(-).

关键词： fluorine Copper Cu(Ⅲ) Cu(Ⅲ)fluoride Trifluoromethyl

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Combination of methylthio-chemistry with living crystallization-driven self-assembly toward uniformπ-conjugated nanostructures with antibacterial activity,surface tailorability,tunable morphology and dimension

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Science China chemistry 2024年第7期67卷 2341-2352页

作者： Chuyu Duan Binbin Xu Ruru Li Xiaoyu Huang Shaoliang Lin Chun Feng Shanghai key laboratory of advanced Polymeric materials School of Materials Science and EngineeringEast China University of Science and TechnologyShanghai 200237China School of chemistry and materials Science Hangzhou Institute for Advanced StudyUniversity of Chinese Academy of SciencesHangzhou 310024China key laboratory of fluorine and nitrogen chemistry and advanced materials Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032China

Living crystallization-driven self-assembly(CDSA)provides robust access to uniformπ-conjugated nanostructures(CNSs)from block copolymers(BCPs)containing a crystallineπ-conjugated segment with controlled dimension,morphology and composition,which show appealing applications in biomedicine,photocatalysis and *** further expand the application spectrum of these CNSs,the development of facile strategies toward diverse CNSs with varying structures/functionalities is highly ***,BCPs consisting of oligo(p-phenylene ethynylene)-b-poly(polypropyl-3-methanethiol acrylate)(OPE_(9)-bPMTPA35and OPE_(9)-b-PMTPA_(58);the subscript represents the number of repeat unit of each block)consisting of a crystallineπ-conjugated core-forming OPE_(9)segment and a corona-forming PMTPA block are *** efficient“click-type”alkylation of methylthio groups,OPE_(9)-b-PMTPA with varying contents of sulfonium unit is *** ribbon-like micelles with different widths and lengths can then be generated in a controlled manner via the self-seeding approach of living ***,negatively charged polymeric and Ag nanoparticles can be immobilized on sulfonium/methylthio-containing shells by taking advantage of electrostatic attraction and coordination interaction,***,the ribbon-like micelles with positively charged shells exhibit antibacterial activity against *** the ease of modification of PMTPA-based shell and attractive opto-electronic/photocatalytic properties ofπ-conjugated units,the combination of methylthio-chemistry and living CDSA opens a new avenue to generate multi-functional CNSs for widespread applications from biomedicine to photocatalysis.

关键词： crystallization-driven self-assembly block copolymer π-conjugated nanostructure methylthio-chemistry

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Synthesis and Crystal Structure of One Mixed-ligand Coordination Polymer Based on the Novel Terphenyl-2,5,2',5'-tetracarboxylic Acid Ligand

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Chinese Journal of Structural chemistry 2012年第10期31卷 1518-1523页

作者：张修堂张炉青张梁栋范黎明魏培海张书香 advanced Material Institute of Research Department of ChemistryQilu Normal University Shandong Provincial key laboratory of fluorine chemistry and Chemical materials University of Jinan 250022 Shandong Provincial key laboratory of fluorine chemistry and Chemical materials University of Jinan

Solvothermal reaction of aromatic terphenyl-2,5,2＇,5＇-tetracarboxylic acid （Hnqptc） ligand and the transitional metal cation of Mn11 in the presence of 3-（2-pyridyl）pyrazole （pp） affords one new coordination polymer, [Mn（qptc）0.5（pp）2]n·n（H2O）（1）. The structure has been determined by single-crystal X-ray diffraction analyses and further characterized by elemental analyses, IR, TGA, and magnetism. The carboxyl groups of qptc4 exhibit a μ1-η1：η0 coordination mode, and the qptc4- acts as a H-shaped ligand linking the Mn11 centers together to form a 2D polymeric [Mn（qptc）0.5]n layer. The crystal of 1 crystallizes in orthorhombic, space group Pbca with a = 9.3119（12）, b = 20.848（3）, c = 26.134（3） A, V= 5073.4（11） A3, Z= 8, C27HIgMnN6O5,Mr=562.42, Dc = 1.473 g/cm3, F（000） = 2304 and μ（MoKa） = 0.571 mm-1. The final R = 0.0468 and wR = 0.1196 for 4429 observed reflections with I 〉 2σ（I） and R = 0.0797 and wR = 0.1383 for all data.

关键词： terphenyl-2,5,2',5'-tetracarboxylic acid 3-(2-pyridyl)pyrazole manganese(II)

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A Novel Energetic Ionic Salt: Hydroxylammonium Potassium 3,3’-Dinitro-5,5’-bis-1,2,4-triazole-1,1’-diolate Dihydrate

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Chinese Journal of Structural chemistry 2020年第1期39卷 96-103,3页

作者： LUO Yi-Fen ZHAI Lian-Jie BI Fu-Qiang HUO Huan LI Xiang-Zhi WANG Bo-Zhou State key laboratory of fluorine&nitrogen Chemicals Xi’an Modern Chemistry Research InstituteXi’an 710065China

A novel energetic ionic salt,hydroxylammonium potassium 3,3?-dinitro-5,5?-bis-1,2,4-triazole-1,1?-diolate dihydrate[(NH3OH)2K(DNOBT)1.5?2H2O],was synthesized and structurally characterized by elemental analysis,IR spectra,13C NMR and single-crystal X-ray diffraction.(NH3OH)2K(DNOBT)1.5?2H2O crystallizes in triclinic system,space group P with a=7.9212(6),b=9.1924(7),c=14.2549(15)?,a=103.917(2)°,β=99.736(2)°,g=104.8110(10)°,V=944.16(14)?^3,Z=2,Dc=1.855 g/cm^3,F(000)=538,μ=0.386 mm^-1,S=1.070,the final R=0.0525 and wR(I>2s(I))=*** decomposition of(NH3OH)2K(DNOBT)1.5?2H2O and its intermediate potassium 1?-hydroxy-3,3?-dinitro-5,5?-bis-1,2,4-triazole-1-olate monohydrate[K(HDNOBT)?H2O]was studied by using DSC and *** was found that(NH3OH)2K(DNOBT)1.5?2H2O,which has primarily one exothermic decomposition process at 248.2℃,has better thermal stability than K(HDNOBT)?H2O which is decomposed at 210.9℃.

关键词： hydroxylammonium potassium 3,3’-dinitro-5,5’-bis-1,2,4-triazole-1,1’-diolatedihydrate synthesis crystal structure thermal decomposition

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In situ construction of Cu(Ⅰ)-Cu(Ⅱ) pairs for efficient electrocatalytic nitrate reduction reaction to ammonia

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Journal of Energy chemistry 2025年第1期 106-113页

作者： Muyun Zheng Yuchi Wan Leping Yang Shen Ao Wangyang Fu Zhengjun Zhang Zheng-Hong Huang Tao Ling Feiyu Kang Ruitao Lv State key laboratory of New Ceramics and Fine Processing School of Materials Science and Engineering Tsinghua University Institute of New Energy materials and Engineering School of Materials Science and Engineering Fuzhou University key laboratory of advanced materials (MOE) School of Materials Science and Engineering Tsinghua University key laboratory for advanced Ceramics and Machining Technology of Ministry of Education Tianjin Key Laboratory of Composite and Functional Materials School of Materials Science and Engineering Tianjin University

Electrocatalytic nitrate reduction reaction （NO3-RR） to ammonia under ambient conditions is expected to be a green process for ammonia synthesis and alleviate water pollution *** report a CuO nanoparticles incorporated on nitrogen-doped porous carbon （CuO@NC） catalyst for *** of Cu（Ⅱ） is reduced to Cu（Ⅰ） during the NO3-RR process to construct Cu（Ⅰ）-Cu（Ⅱ） pairs,confirmed by in situ X-ray photoelectron spectroscopy （XPS） and Raman *** functional theory （DFT） calculations indicated that the formation of Cu（Ⅰ） could provide a reaction path with smaller energy barrier for NO3-RR,while Cu（Ⅱ） effectively suppressed the competition of hydrogen evolution reaction （HER）.As a result,CuO@NC catalyst achieved a Faradaic efficiency of 84.2% at -0.49 V versus reversible hydrogen electrode （RHE）,and a NH3yield rate of 17.2 mg *** -0.79 V ***,higher than the HaberBosch process (<3.4 g h-1g-1cat.).This work may open a new avenue for effective NO3-RR by modulating oxidation states.

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Understanding the alkyl effect of geminal dinitropropyl ester energetic plasticizers on hydroxyl terminated polybutadiene(HTPB):Simultaneous tuning on low temperature behavior and processability

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Chinese Journal of Chemical Engineering 2023年第2期54卷 364-371页

作者： Baodong Zhao Yinglei Wang Fulei Gao Yajing Liu Weixiao Liu Feng Ding Xi'an Modern chemistry Research Institute Xi'an 710065China State key laboratory of fluorine&nitrogen Chemicals Xi'an 710065China

Geminal dinitropropyl ester plasticizers(DNPEPs) possess excellent energetic performances which provide good potentials as insensitive plasticizer. In this study, we design and synthesize DNPEPs with different alkane chain parts, and systematically investigate their structure-property *** show that DNPEPs have impact sensitivities all higher than 25.2 J, thermal decomposition temperatures all higher than 254 ℃, and glass transition temperatures(T_(g)) lower than-90 ℃.Furthermore, the effects of DNPEPs as plasticizer are studied on hydroxyl terminated polybutadiene(HTPB) in detail, including the viscosity, glass transition temperatures and others. It is noteworthy that 2,2-dinitropropyl nonanoate(DNPNc) among these DNPEPs exhibits the most expected simultaneous tuning effects on both viscosity and T_(g) of HTPB systems, providing favorable potentials to replace the conventional plastizers as dioctyl sebacate(DOS) in the HTPB based propellants and explosives.

关键词： Molecular simulation Experimental validation Preparation Energetic plasticizer Glass transition temperature Viscosity

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Tuning the interfacial reaction environment via pH-dependent and induced ions to understand C–N bonds coupling performance in NO3- integrated CO2 reduction to carbon and nitrogen compounds over dual Cu-based N-doped carbon catalyst

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Journal of Energy chemistry 2025年第1期100卷 273-285页

作者： Tianhang Zhou Chen Shen Zhenghao Wu Xingying Lan Yi Xiao College of Carbon Neutrality Future Technology State Key Laboratory of Heavy Oil Processing China University of Petroleum (Beijing) Institute of materials Science TU Darmstadt Department of chemistry Xi'an Jiaotong-Liverpool University Department of Mechanical and Mechatronics Engineering and Waterloo Institute of Nanotechnology University of Waterloo Waterloo

Dual atomic catalysts （DAC）,particularly copper （Cu2）-based nitrogen （N） doped graphene,show great potential to effectively convert CO2and nitrate （NO3-） into important industrial chemicals such as ethylene,glycol,acetamide,and urea through an efficient catalytical process that involves C–C and C–N ***,the origin of the coupling activity remained unclear,which substantially hinders the rational design of Cu-based catalysts for the N-integrated CO2reduction reaction （CO2RR）.To address this challenge,this work performed advanced density functional theory calculations incorporating explicit solvation based on a Cu2-based N-doped carbon (Cu2N6C10) catalyst for *** calculations are aimed to gain insight into the reaction mechanisms for the synthesis of ethylene,acetamide,and urea via coupling in the interfacial reaction *** to the sluggishness of CO2,the formation of a solvation electric layer by anions （F-,Cl-,Br-,and I-） and cations (Na+,Mg2+,K+,and Ca2+) leads to electron transfer towards the Cu *** process significantly accelerates the reduction of *** results reveal that*CO intermediates play a pivotal role in N-integrated ***,the Cu2-based N-doped carbon catalyst examined in this study has demonstrated the most potential for C–N coupling to *** findings reveal that through the process of a condensation reaction between*CO and NH2OH for urea synthesis,*NO3-is reduced to*NH3,and*CO2to*CCO at dual Cu atom *** dual-site reduction facilitates the synthesis of acetamide through a nucleophilic reaction between NH3and the ketene ***,we found that the I-and Mg2+ions,influenced by pH,were highly effective for acetamide and ammonia synthesis,except when F-and Ca2+were ***,the mechanisms of C–N bond formation were investigated via ab-initio molecular dynamics simulations,and we found that adjusting the micro-environment can change the dominant side reaction,shift

关键词： pH-dependent micro-environments C–N coupling Dual Cu-based nitrogen carbon catalysts Explicit solvation model Ion stabilizer AIMD

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