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中国化学会第九届全国无机化学学术会议

作者： Xiu-Juan Shang Wen-Hua Zhang Jian-Ping Lang College of Chemistry Chemical Engineering and Materials ScienceSoochow University

Diblock copolymer of poly（ε-caprolactone）-block-poly（methyl methacrylate）（PCL-b-PMMA）was conventionally synthesized by a sequential two-step strategy,which involves ring-opening polymerization（ROP）followed by atom transfer radical polymerization（ATRP）.[1-2]Such process is however time-consuming,complicated and *** our previous work,Fe（Ⅲ）-based compound Fe（bpp H2）Cl3（1）（bppy H2,2,6-di（1H-pyrazol-3-yl）pyridine）was used to initiate ring-opening polymerization ofε-caprolactone（CL）with exquisite control.[3]1 could further reduce to Fe（bpp H2）Cl2（2）by Cp2Co to terminate the polymerization and convert back to 1 via[Cp2Fe]-PF6 to restart the polymerization *** this presentation,MMA polymerization in tandem with CL polymerization provides PCL-b-PMMA in one-pot,taking advantage of the convenient switch of the oxidation states of *** polymerization sequence can be freely executed with needed catalyst Fe（bpp H2）Cl2 or Fe（bpp H2）Cl3.

关键词： Ring-opening Polymerization(ROP) Atom Transfer Radical Polymerization(ATRP) Block Copolymer Redox Active Catalyst iron complexes

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Monoribbed-Functionalized Macrobicyclic iron(Ⅱ) complexes Decorated with Terminal Reactive and Vector Groups: Synthetic Strategy, Chemical Transformations and Structural Characterization

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Chinese Journal of Chemistry 2022年第17期40卷 2089-2105页

作者： Ilya P.Limarev Genrikh E.Zelinskii Svetlana A.Belova Pavel V.Dorovatovskii Anna V.Vologzhanina Ekaterina G.Lebed Yan Z.Voloshin Nesmeyanov Institute of Organoelement Compounds of the Russian Academy of Sciences 28 Vavilova stMoscow119991 Russia Kurnakov Institute of General and Inorganic Chemistry of the Russian Academy of Sciences 31 Leninsky prMoscow119991 Russia National Research Center Kurchatov Institute 1 Kurchatova plMoscow123098 Russia

General and straightforward synthetic strategy towards the iron(Ⅱ)clathrochelates with functionalizing substituents in their apical capping and one of the three chelate ribbed fragments was *** hexachloroclathrochelate precursors were prepared by the direct template condensation of dichloroglyoxime with a suitable boronic acid on the Fe^(2+) ion as a matrix and underwent a stepwise nucleophilic substitution with S_(2)-,N_(2)- or O_(2)-bis-nucleophiles,forming the alicyclic or aromatic N_(2)-,S_(2)-or O_(2)-six-membered *** on the reaction conditions and precursor-to-dinucleophile molar ratios,iron(Ⅱ)clathrochelates with one(S,O and N),two(S,O and N)or three(S and O)X_(2)-six-membered ribbed substituent(s)were *** reactivity substantially decreases in a row:Cl_(6)-Cage>Cl_(4)X_(2)-Cage(where X=S,O or,especially,N)>Cl_(2)X_(4)-Cage(where X=S or O).The reactive monoribbed-functionalized clathrochelates underwent further chemical transformations giving the target macrobicyclic complexes with terminal vector *** follows from the single crystal XRD data,their FeN_(6)-coordination polyhedra possess the geometry intermediate between a trigonal prism and a trigonal antiprism(φ=21.3°—25.20°).Fe-N distances vary from 1.887(6)to 1.933(8)Å.Their 3D-molecules,the hydrophobic–hydrophilic balance in which can be tuned using a ribbed functionalization,form in the crystals the intermolecular specific halogen bonds and/or hydrophobic interactions.

关键词： Macrocyclic compounds Clathrochelates iron complexes Ligand reactivity Targetdelivery

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An inverted triplesalen ligand by a convergent synthesis and its influence on trinuclear Fe_3~Ⅲ complexes

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Science China Chemistry 2012年第6期55卷 951-966页

作者： FELDSCHER Bastian KRICKEMEYER Erich MOSELAGE Marc THEIL Hubert HOEKE Veronika KAISER Yvonne STAMMLER Anja BGGE Hartmut GLASER Thorsten Lehrstuhl für Anorganische Chemie I Fakultt für Chemie Universitt Bielefeld Universittsstr. 25 D-33615 Bielefeld Germany

The inverted triplesalen ligand H6feldMe has been synthesized from 2,4,6-triformyl-phloroglucinol and a ketimine salen half-unit in a convergent synthesis. NMR, IR, and UV-vis spectroscopy reveal that this ligand is not in the O-protonated tau- tomer but in the N-protonated tautomer with substantial heteroradialene contribution. This ligand and the conventional triple- salen ligand H6talent-au2 have been used to synthesize the trinuclear Fem complexes [（feldMe）（FeCl）3] and [（talent-Bu2）（FeC1）3], respectively. The molecular structures of these complexes were obtained by single-crystal X-ray diffraction. Two trinuclear Fem complexes of [（feldMe）（FeCl）3] dimerize via two Fe-phenolate bonds, whereas due to steric hindrance no dimerization is observed for [（talent-Bu2）（FeC1）3]. The structural data also reveal some heteroradialene contribution in the trinuclear complexes. Whereas UV-vis and MOlSbauer spectroscopy are not suitable to distinguish between the two complexes, FT-IR spectra show characteristic features due to the different substitution patterns of the conventional and the inverted triplesalen ligands. Another handle is provided by electrochemistry. Whereas both complexes exhibit an irreversible oxidation wave （0.94 V vs. Fc＋/Fc for [（feldMe）（FeC1）3] and 0.84 V vs. Fc~/Fc for [（talent-Bu2）（FeC1）3]）, which is assigned to the oxidation of the central backbone, higher potential oxidations are reversible for [（talent-Bu2）（FeC1）3]） but irreversible for [（feldMe）（FeC1）3]. This is attributed to the reversible oxidation of the terminal phenolates in the di-tert-butyl substituted [（talentBu2）（FeCl）3] in contrast to the mono-methyl-substituted phenolates in [（feld^ae）（FeC1）3]. The magnetic properties of [（talen^-Bu2）（FeC1）3] reveal a very small ferromagnetic coupling with significant zero-field splitting of the Feul S = 5/2 ions. In contrast, the dimerization of two trinu- clear complexes in [（feldMe）（FeCl）3] results in antiferromagnetic interactions between the two pheno

关键词： magnetic properties iron complexes spin-polarization triplesalen

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Study on the Reaction Behavior of Some Trinuclear complexes of Transition Metals: [Fe_2M(μ_3-O) (μ-O_2CCH_3)_6(H_2O)_3]·xH_2O by the Method of Probe Reaction of Acetic Acid

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Chinese Journal of Structural Chemistry 1998年第5期17卷 365-371页

作者： HE Ling-Jie CHEN Bo CAI Su-Hua WANG Yan-Ming ZHOU Wen-Bo ZHANG Lin-Na (Fujnin Institute of Research on the Structure of Matter,the Chinese Academy of Sciences, Fuzhou, Fujian 350002, China)XIE Qing-Shan (Present address:Shishi Organizing Committee ,Sh Fu Jian Inst. Res. Struct. of Matter Chinese Academy of Sciences Fuzhou Fu jian 350002 China Shishi Organizing Committee Shishi Fujian 362000 China

The reaction behaviors of the title complexes have been studied in thesystem of dinitrogen gas by means of in situ IR. It has been found that some activefragments created at some stage of the thermal decomposition process of the *** acetic acid both obtained from the ligand of the complexes and introducedfrom outside to convert to acetone by decarboxylation. Their optimum reaction temperatures are of 240~270℃ for [Fe2MnO(O2CCH3),(H2O)3], 290~320 C for [Fe3Q(O2CCH3)6(H2O)3], 300~330℃ for [Fe2CoO(O2CCH3),(H2O)3] and 320~ 350℃for [Fe2NiO(O2CCH3)6(H2O)3], indicating the lowering sequence of the activity of active species. At the same time it has been shown that this activity may come from thejoined contributions of both the coordinating capability of the hetero-metals in the complexes and their structural factors. On the basis of the TGA, DTA and EI-MS data,the composition of the active fragments has been tentatively inferred as [Fe2MnO(O2CCH3)3-2].

关键词： in situ IR carboxylato complexes iron complexes manganese complexes cobalt complexes nickel complexes

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Dangling Ligand Enables an iron Hexa-Coordinated Molecular Catalyst for Water Oxidation by Photocatalysis

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CCS Chemistry 2024年第3期6卷 623-630页

作者： Bing Yang Qi Liu Xiang-Zhu Wei Tao Lei Qing-Qing Yang Xu-Zhe Wang Jing-Xin Jian Xin Jiang Chen-Ho Tung Li-Zhu Wu Key Laboratory of Photochemical Conversion and Optoelectronic Materials New Cornerstone Science LaboratoryTechnical Institute of Physics and ChemistryChinese Academy of SciencesBeijing 100190 School of Future Technology University of Chinese Academy of SciencesBeijing 100049

Photocatalytic water oxidation reaction by transition metal complexes remains a challenge because of their poor stability under irradiation,especially for earth-abundant metal *** this regard,ironbased water oxidation catalysts are prone to hydrolysis and/or dissociate the ligands to form nanoparticles under a real catalytic ***,we describe a unique hexa-coordinated catalyst 1[Fe^(II)(Py_(3)tacn)Cl_(2)]and its reference 2[Fe^(II)(PhPy_(2)tacn)Cl_(2)]with a dangling pyridyl ligand and a phenyl group,*** anticipated that the dynamically open and close coordination behaviors of the pyridyl ligand enabled balance of the reactivity and stability of catalyst *** our delight,the“open form”of catalyst 1 provided a free coordination site,and the“close form”guaranteed its molecular integrity,resulting in a water oxidation reaction with high efficiency and *** turnover number and turnover frequency values of 2332 and 60 s^(−1)are the highest known to date among iron-based homogeneous water oxidation systems under visible light irradiation.

关键词： water oxidation photocatalysis homogeneous catalysis iron complexes dangling ligand intermediates characterization

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Oligomerization of Ethylene by Fe(salphen)/EAO and Fe(salen)/EAO Catalysts

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Chinese Journal of Catalysis 2000年第2期21卷 99-100页

作者： QIAN Mingxing, WANG Mei, HE RenOpen Laboratory of Comprehensive Utilization for Carbon Resources, Dalian University of Technology, Dalian 116012, China) 大连理工大学碳资源综合利用开放实验室辽宁大连 116012

The oligomerization was studied of ethylene catalyzed by Fe(salphen) (A, salphen = N,N'-o-phenylenebis (salicylideneaminato)) and Fe(salen) (B, salen = N,N'-ethylenebis (salicylideneaminato)) which were prepared according to earlier description. The catalytic activity and selectivity of the two complexes with EAO (ethylaluminoxane) as cocatalyst for ethylene oligomerization were studied at various reaction temperatures, Al/Fe ratios, and reaction time. Both A and B showed higher catalytic activity and selectivity for low-carbon olefins. The catalytic activity of A/EAO and B/EAO catalysts for ethylene oligomerization were strongly affected by the reaction temperatures. When temperature was raised from 90°to 200°C, the activity increased by 25 times for A/EAO and by 26 times for B/EAO. Both catalysts displayed decreased selectivity for low-carbon linear α-olefins as the temperature was raised. The effect of n(Al)/n(Fe) ratio on ethylene oligomerization was also studied.

关键词： ethylene oligomerization iron complexes ethylaluminoxane

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