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中文摘要：
上海有机化学研究所在有机合成方法学研究方面有长期积累, '十五'期间曾建成了一个麻生明院士领衔的"导向有机合成的金属有机化学"基金委创新群体， 形成了在国际上有影响力的联烯化学和不对称催化的研究团队。同时，根据有机化学及相关前沿领域的国际发展趋势，引进了一批年轻的学术骨干，探索金属化合物等对有机分子中化学键的活化机制，认识反应选择性控制的本质与规律。正在形成一个以化学键的选择性活化和可控性重组为手段发展化学键活化新方法和新策略并关注国家需求的基础研究群体。群体拟利用金属配合物1）对C=X键与其它化学键的特性差异进行选择性活化、断裂和重组；2）对烯烃，COx等的活化，实现一些新型的聚合反应；3）建立惰性化学键的选择性活化与重组的新模式，研究其对C-H和C-C键的选择性断裂与可控性重组的一些基本规律。争取在未来3-6年形成一支在国际上有影响力的研究有机合成反应中选择性控制的团队之一。
英文摘要：
Chemical bond；activation；reorganization；organometallic；catalysis
结论摘要：
项目执行3年来，对金属配合物促进下化学键的活化与可控性重组的规律有了初步的认识，发展了一些新的有机合成反应和催化剂体系1）针对惰性C-H键选择性活化中存在的问题，发展了系列过渡金属催化的碳氢键直接官能团化反应，揭示了在相关反应过程中的金属-碳(氢)键形成、断裂和转化的基本规律；2）针对张力环分子，发展了多种策略以实现碳碳键的选择性断裂与转化，并阐明了相关化合物碳碳键活化的规律；3）通过金属促进的C=C双键的活化和多样性转化，结合国家需求，发展了芳烃化合物的不对称去芳构化反应、烯烃的氟化-官能团化反应、高效硼氢化和硅氢化反应等，提出了“不饱和烃的氟钯化”策略，实现了烯烃的选择性转化反应的新模式，为物质的高效转化和创造新的功能物质提供了有效的方法； 4）运用边臂策略设计了系列金属配合物，系统研究了边臂和中心金属对乙烯聚合链转移方式与速度影响规律，实现了分子量从数千到数百万，非极性支链到极性支链、从无支化到高支化、甚至树枝状聚乙烯的可控性合成，为实现聚乙烯高性能化、系列化和专用化提供了科学基础和技术支撑。主要成果如下 1. 共发表论文270篇，其中包括J. Am. Chem. Soc. 24篇，Angew. Chem. Int. Ed. 33篇；出版学术著作（含章节）12部；申请专利47项，获得授权专利34项。部分成果获得国家自然科学二等奖2项，上海自然科学一等奖2项；22个所发展的新配体与催化剂被Sigma-Aldrich和Strem Chemicals商品化，全球销售供国际同行使用；利用上述成果所发展的高性能超高分子量聚乙烯催化剂技术和环氧氯丙烷的动力学拆分技术实现技术转让，已工业化生产。 2. 团队成员有130人次在国际学术会议做大会、主题和邀请报告；30余人次担任国际期刊的编委或顾问编委，包括Org. Lett.、Beilstein J. Org. Chem.、Organometallics副主编及Synthsis地区编辑; 3. 团队成员有1位当选中国科学院院士，2位获国家 “杰出青年科学基金”资助，2位研究员获国家委“优秀青年科学基金”资助，1位研究员入选“青年千人计划”；研究生培养方面，有48名学生获得博士学位、10名学生获得硕士学位。
成果综合统计
期刊论文
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期刊论文
Synthesis, structure, and ethylene polymerization behavior of nickel complexes based on benzoylmethy
Construction of Axial Chirality via Rhodium-Catalyzed Asymmetric Dehydrogenative Heck Coupling of Bi
Construction of Erythrinane Skeleton via Pd(0)-Catalyzed Intramolecular Dearomatization of para-Amin
Nitrogen- and Phosphorus-Containing Lewis Base Catalyzed [4+2] and [3+2] Annulation Reactions of Isa
A Family of Donor-Acceptor Photovoltaic Polymers with Fused 4,7-Dithienyl-2,1,3-benzothiadiazole Uni
From N-benzoylpyridinium imides to pyrazolo[1,5-a]pyridines: a mechanistic discussion on a stoichiom
Synthesis of Chiral 1,3-Bis(1-(diarylphosphoryl)ethyl)-benzenes via Ir-Catalyzed Double Asymmetric h
Selective Synthesis of Secondary Benzylic (Z)-allylboronates by Fe-catalyzed 1,4-hydroboration of 1-
Synthesis and catalytic activity of heterogeneous rare-earth metal catalysts coordinated with multit
Preparation of Chiral Multifunctional Thiourea-Phosphanes and Synthesis of Chiral Allylic Phosphites
LDA-Mediated Cascade Carbolithiation Reactions of Vinylidenecyclopropanes with Enones and N-Sulfonat
Copper-Catalyzed Trifluoromethylation and Cyclization of Aromatic-Sulfonyl-Group-Tethered Alkenes fo
Reversible addition of the Si-H bond of phenylsilane to the Sc=N bond of a scandium terminal imido c
Iridium-Catalyzed Allylic Alkylation Reaction with N-Aryl Phosphoramidite Ligands: Scope and Mechani
Asymmetric [3+2] annulation of N-protected isatins with but-3-yn-2-one catalyzed by DIOP: facile cre
An Efficient Method for the Synthesis of Alkylidenecyclobutanones by Gold-Catalyzed Oxidative Ring E
Rhodium(I)-Catalyzed Pauson-Khand-type [3+2+1] Cycloaddition Reaction of Ene-Vinylidenecyclopropanes
Gold(I)-Catalyzed Cycloisomerization of Nitrogen- and Oxygen-Tethered Alkylidenecyclopropanes to Tri
DABCO-Mediated [4+2] Annulation of But-3-yn-2-one and Activated Ketones: Facile Preparation of 2,3-D
Asymmetric catalytic Mannich-type reaction of hydrazones with difluoroenoxysilanes using imidazoline
Reactions of Vinylidenecyclopropanes with Diphenyl Diselenide in the Presence of AIBN and Thermally-
Gold(I)-catalyzed intramolecular hydroamination and ring-opening of sulfonamide-substituted 2-(arylm
Transition metal-catalyzed carbocyclization of nitrogen and oxygen-tethered 1,n-enynes and diynes: s
AgF-Mediated Dialkylation of Activate Alkenes: An Efficient Access to Nitrile-Containing Spirooxindo
Stereospecific Synthesis of Highly Functionalized Benzo[3.1.0]bicycloalkanes via Multistep Cascade R
1/asymmetric Pictet-Spengler cascade via sequential catalysis of ruthenium alkylidene and chiral pho
Rare-earth half-sandwich dialkyl and homoleptic trialkyl complexes for rapid and stereoselective pol
Versatile reactivity of a four-coordinate scandium phosphinidene complex: Reduction, addition, and C
Phosphine-catalyzed asymmetric [4+1] annulation of activated alpha,beta-unsaturated ketones with Mor
Silver(I)-Mediated Dual Cleavage of C-C and C-O Bonds in the Reaction of Diarylmethylenecyclopropane
Insertion of Nitriles into Zirconocene-1-aza-1,3-diene Complexes: Chemoselective Synthesis of N-H an
Rhodium-catalyzed Carbonylative Skeleton Rearrangement of 1,4-Enynes Tethered by a Cyclopropane Grou
Phosphine-Catalyzed Annulations of 4,4-Dicyano-2-Methylenebut-3-Enoates with Maleimides and Maleic A
Mechanistic Insights into the Pd-Catalyzed Intermolecular Asymmetric Allylic Dearomatization of Mult
Iron-mediated C-H bond amination by organic azides on a tripodalbis(anilido)iminophosphorane platfor
(DHQ)(2)AQN-Catalyzed Asymmetric Substitution of Isatin-Derived Hydrazones with O-Boc-Protected Mori
Gold-Catalyzed Cyclization of 1-(Indol-3-yl)-3-alkyn-1-ols: Facile Synthesis of Diversified Carbazol
Gold-catalyzed intramolecular regio- and enantioselective cycloisomerization of 1,1-bis(indolyl)-5-a
Highly enantioselective asymmetric hydrogenation of (E)-beta,beta-disubstituted alpha,beta-unsaturat
Ring-Closing Metathesis/Isomerization/Pictet-Spengler Cascade via Ruthenium/Chiral Phosphoric Acid S
Chiral multifunctional thiourea-phosphine catalyzed asymmetric [3+2] annulation of Morita-Baylis-Hil
Rhodium(I)-catalyzed [3+2] intramolecular cycloaddition of alkylidenecyclopropane-propargylic esters
Dearomatization of tryptophols via a vanadium-catalyzed asymmetric epoxidation and ring-opening casc
Palladium-catalyzed intermolecular asymmetric allylic dearomatization reaction of naphthol derivativ
DPEN-derived Triazolium Salts Catalyzed Annulation Reactions ofa,β-Unsaturated Aldehydes with 1,3-Di
Organocatalyzed arylalkylation of activated alkenes via decarboxylation of PhI(O2CR)(2): efficient s
Yb(NTf2)(3)-catalyzed [3+3] cycloaddition between isatin ketonitrones and cyclopropanes to construct
Double gamma-alkylation of allylic phosphorus ylides: a unique access to oxa-bicyclic[3.3.0] diene s
Access to 2′,3′-dihydro-1′H-spiro[indoline-3,4′-pyridin]-2-ones via amino acid derived phosphine-cat
Pd-Catalyzed Intramolecular Aminohydroxylation of Alkenes with Hydrogen Peroxide as Oxidant and Wate
SpinPhox/Iridium(I)-Catalyzed Asymmetric Hydrogenation of Cyclic alpha-Alkylidene Carbonyl Compounds
LDA-mediated domino carbolithiation reactions of vinylidenecyclopropanes with but-3-yn-2-one and 1-p
Access to Both Enantiomers of alpha-Chloro-beta-keto Esters with a Single Chiral Ligand: Highly Effi
Phosphorus-containing Lewis base catalyzed highly regioselective cyclization of isatin derived elect
Gold-Catalyzed Cyclizations of (o-Alkynyl)phenoxyacrylates with External Nucleophiles: Regio- and St
Transition metal-catalyzed fluorination of multi carbon-carbon bonds: new strategies for fluorinated
Gold-Catalyzed Cascade Cyclizations of 1,6-Diynyl Carbonates to Benzo[b]fluorenes Involving Arylatio
Silver-catalyzed cascade cyclization-stannylation of o-alkynylaniline derivatives with 2-tributylsta
Iron(II) Complexes Featuring Bidentate N-Heterocyclic Carbene-Silyl Ligands: Synthesis and Character
Rhodium(I)-catalyzed enantioselective hydrogenation of substituted acrylic acids with sterically sim
Synthesis and catalytic activity of amido-boratabenzene complexes of rare-earth metals and zirconium
Anchoring of Silyl Donors on a N-Heterocyclic Carbene through the Cobalt-Mediated Silylation of Benz
Gold-Catalyzed Cascade Reactions of Furan-ynes with External Nucleophiles Consisting of a 1,2-Rearra
Catalytic asymmetric hydrogenation of α-CF3- or β-CF3-Substituted acrylic acids using Rhodium(I) com
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