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Carbon-hydrogen activation in China

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Science China Chemistry 2015年第8期58卷 1245-1248页

作者： zhang-jie shi Guo-Qiang Lin College of Chemistry and Molecular Engineering Peking University Shanghai Institute of Organic Chemistry Chinese Academy of Sciences

Transition metal catalyzed C-H Functionalization is one of the most important and challenging research fields in or- ganic chemistry and has rapidly evolved in recent decades. Some recent achievements in the field include i） minimizing the pre-activation procedures of substrates, ii） reducing waste production, and iii） shortening synthetic steps by de- veloping direct activations and straightforward transfor- mations of C-H bonds. With the rapid developments in chemistry and the continuous support of the Chinese gov- ernment, Chinese chemists have played important roles in this emerging field in the past two decades. To stimulate the continued success of Chinese chemists, this work provides an intensive account of the current status of this important field in China's Mainland.

关键词： Activation analysis Transition metals

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Privileged strategies for direct transformations of inert aliphatic C–H bonds

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National Science Review 2014年第2期1卷 172-175页

作者： Guihua Chen zhang-jie shi College of Chemistry and Green Chemistry Center Peking University

Functional group transformations are central to organic ***,the functionalities used in such transformations are highly active organic groups such as halogens,ester groups and hydroxyl ***–hydrogen bonds are ubiquitous structural motifs in organic compounds,but they are not considered to be functionalgroups because(1)in general,the bond dissociation energy of a C–H bond is high,and therefore,such bonds

关键词： H bonds Privileged strategies for direct transformations of inert aliphatic C

骨桥蛋白和p38MAPK信号通路在多房棘球蚴原头节发育中的作用

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动物医学进展 2025年第1期46卷 9-15页

作者：徐刚毛艺胡帅葛宇飞徐志张玉梦谢士伟张宏伟张示杰石河子大学第一附属医院新疆石河子832000 石河子大学医学院新疆石河子832000

为明确骨桥蛋白(OPN)和多房棘球蚴(Echinococcus multilocularis,Em)p38丝裂原活化蛋白激酶(p38MAPK)信号通路在Em发育过程的作用,剖检感染Em 4~6月的长爪沙鼠,提取Em原头节后,分别用不同浓度的p38MAPK抑制剂(SB202190)处理Em原头节,选... 详细信息

为明确骨桥蛋白(OPN)和多房棘球蚴(Echinococcus multilocularis,Em)p38丝裂原活化蛋白激酶(p38MAPK)信号通路在Em发育过程的作用,剖检感染Em 4~6月的长爪沙鼠,提取Em原头节后,分别用不同浓度的p38MAPK抑制剂(SB202190)处理Em原头节,选取合适的SB202190浓度后在体外将原头节分为DMSO组、anti-p38MAPK组、PBS组、OPN组、OPN+anti-p38MAPK组,采用伊红染色、caspase-3试剂盒检测caspase-3、EDU和Hoechst染色、活性氧(ROS)检测探针检测原头节的活性、凋亡和增殖情况。结果显示,抑制Em的SB202190适宜浓度为20μmol/L,SB202190增加Em的伊红染色率、caspase-3水平,减少EDU阳性、ROS水平,OPN可减少Em伊红染色率、caspase-3水平,增加EDU阳性率、ROS水平,且SB202190可逆转OPN对Em的结果,这些结果表明SB202190可抑制Em的活性和增殖、促进凋亡并与浓度正相关,而OPN可促进Em的活性和增殖、抑制凋亡,且SB202190可逆转OPN对Em的作用。研究结果为OPN和p38MAPK信号通路可能成为治疗多房棘球蚴病的新分子靶点提供证据。

关键词：多房棘球蚴多房棘球蚴病骨桥蛋白 p38丝裂原活化蛋白激酶

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Regio-Divergent C—H Alkynylation with Janus Directing Strategy via Ir(Ⅲ)Catalysis

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Chinese Journal of Chemistry 2020年第9期38卷 929-934页

作者： Xianwei Lif Guangxin Liang zhang-jie shi School of Chemical Engineering and Light Industry Guangdong University of TechnologyGuangzhouGuangdong 510006China School of Physical Science and Technology ShanghaiTech UniversityShanghai 201210China State Key Laboratory and Institute of Elemento-Organic Chemistry Nankai UniversityTianjin 300071China Department of Chemistry Fudan UniversityShanghai 200433China College of Chemistry and Molecular Engineering Peking UniversityBeijing 100871China State Key Laboratory of Organometallic Chemistry Shanghai Institute of Organic ChemistryCASShanghai 200032China

Summary of main observation and conclusion Directing strategy has been extensively exploited to maintain activity and selectivity for the rapid access to functionalized molecules and pharmaceutical ***,‘one-to-one’activation model was usually achieved through traditional directing strat***,we achieved‘one-to-two'activation model by slight modification of simple and practical ketoxime and amide *** judicious choice of directing groups,Csp3—H and Csp2—H bond alkynylation reaction,and more significantly,dehydrogenative Csp3—H alkynylation,were realized,enabling the regio-divergent late-stage modifications of pharmaceuticals.

关键词： activation maintain conclusion

Direct transformation of dinitrogen: synthesis of N-containing organic compounds via N-C bond formation

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National Science Review 2020年第10期7卷 1564-1583页

作者： Ze-jie Lv Junnian Wei Wen-Xiong zhang Ping Chen Dehui Deng zhang-jie shi Zhenfeng Xi Beijing National Laboratory for Molecular Sciences (BNLMS) Key Laboratory of Bioorganic Chemistry and Molecular Engineering of Ministry of EducationCollege of ChemistryPeking University Dalian Institute of Chemical Physics Chinese Academy of Sciences Department of Chemistry Fudan University

N-containing organic compounds are of vital importance to lives. Practical synthesis of valuable N-containing organic compounds directly from dinitrogen(N2), not through ammonia(NH3), is a holy-grail in chemistry and chemical industry. An essential step for this transformation is the functionalization of the activated N2units/ligands to generate N-C bonds. Pioneering works of transition metal-mediated direct conversion of N2into organic compounds via N-C bond formation at metal-dinitrogen [N2-M] complexes have generated diversified coordination modes and laid the foundation of understanding for the N-C bond formation mechanism. This review summarizes those major achievements and is organized by the coordination modes of the [N2-M] complexes(end-on,side-on, end-on-side-on, etc.) that are involved in the N-C bond formation steps, and each part is arranged in terms of reaction types(N-alkylation, N-acylation, cycloaddition, insertion, etc.) between [N2-M]complexes and carbon-based substrates. Additionally, earlier works on one-pot synthesis of organic compounds from N2via ill-defined intermediates are also briefed. Although almost all of the syntheses of N-containing organic compounds via direct transformation of N2so far in the literature are realized in homogeneous stoichiometric thermochemical reaction systems and are discussed here in detail, the sporadically reported syntheses involving photochemical, electrochemical, heterogeneous thermo-catalytic reactions, if any, are also mentioned. This review aims to provide readers with an in-depth understanding of the state-of-the-art and perspectives of future research particularly in direct catalytic and efficient conversion of N2into N-containing organic compounds under mild conditions, and to stimulate more research efforts to tackle this long-standing and grand scientific challenge.

关键词： dinitrogen transformation metal-dinitrogen complex N−C bond formation N-containing organic compounds

Direct Transformation of Arenols Based on C—O Activation

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Chinese Journal of Chemistry 2020年第8期38卷 855-863页

作者： Feng Liu Hao-jun Jiang Yi Zhou zhang-jie shi School of Perfume and Aroma Technology Shanghai Institute of Technology100 Haiquan RdShanghai 201418China Department of Chemistry Fudan University2005 Honghu RdShanghai 200438China

Contents *** 8562.C—O Activation via the in-situ Formed Intermediate 8562.1.C—C bond formation 8562.2.C—X bond formation 8573.C—O Activation via Dearomatization-Condensation-Rearomatization Process *** catalyzed C—O cleavage of phenols,dearomatization-condensation-rearomatization process in a gas phase ***-condensation-rearomatization process in a liquid phase *** *** C—O Activation of Phenol Salts *** C—O Activation of Phenol *** and Perspective *** Transition-metal-catalyzed cross-coupling reactions of aryl electrophiles with organic or organometallic reagents emerged as one of the most powerful tools for constructing aromatic compounds.[1]In the early days,the most popular electrophiles werearyl halides because of their high reactivity and availability.

关键词： catalyzed Phenol Transformation

Transition Metal Catalyzed Direct Oxidative Borylation of C--H Bonds

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Chinese Journal of Chemistry 2018年第10期36卷 950-954页

作者： Zhong-Tao Jiang Bi-qin Wang zhang-jie shi College of Chemistry and Materials Science Sichuan Normal University Chengdu Sichuan 610068 China Department of Chemistry Fudan University Shanghai 200433 China

Organoboron is well-developed and broadly utilized organometallic reagents in organic synthesis due to its extraordinary performances in transition-metal catalyzed C-C and C-X bonds construction. Catalytic C--H borylation and further transformations catalyzed by transition metal catalysts in the absence of oxidants were well studied in decades. However, as known, transition metal catalyzed oxidative C-H borylations were not reviewed up to date. In this article the oxidative borylation of C（sp2）-H and C（sp3）-H bonds were summarized and their mechanisms were also accounted.

关键词： C-H borylation oxidation organoboron transition metal catalysis

Advances in electrochemical transformation of N_(2)using molecular catalysts

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Science China Chemistry 2023年第10期66卷 2743-2753页

作者： Qiong Yuan Junnian Wei Dehui Deng zhang-jie shi Ping Chen Zhenfeng Xi Beijing National Laboratory for Molecular Sciences Key Laboratory of Bioorganic Chemistry and Molecular Engineering of Ministry of EducationCollege of ChemistryPeking UniversityBeijing 100871China Dalian Institute of Chemical Physics Chinese Academy of SciencesDalian 116023China Department of Chemistry Fudan UniversityShanghai 200433China

The conversion of N_(2)to NH_(3)holds great importance due to the essential role of NH_(3)in fertilizer production,energy storage and the synthesis of key industrial *** of novel methods for N_(2)transformation is a worthwhile goal and researchers have turned their attention to electrochemical N_(2)reduction as a potentially sustainable *** development of molecular electrocatalysts has gained considerable momentum over the last decades,and this review focuses on the advances and challenges in the field of molecular electrochemical nitrogen fixation and aims to inspire further research into the realm of nitrogen fixation chemistry from an electrochemical perspective.

关键词： dinitrogen transformation dinitrogen complexes electrochemistry dinitrogen fixation electrocatalyst

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Silylamido supported dinitrogen heterobimetallic complexes: syntheses and their catalytic ability

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National Science Review 2021年第12期8卷 29-36页

作者： Dan-dan Zhai Si-jun Xie Yi Xia Hua-yi Fang zhang-jie shi Department of Chemistry Fudan University State Key Laboratory of Organometallic Chemistry Shanghai Institute of Organic ChemistryChinese Academy of Sciences

Molybdenum dinitrogen complexes supported by monodentate arylsilylamido ligand,[Ar(MeSi)N]MoNMg(THF)[N(SiMe)Ar](5) and [Ar(MeSi)N]MoNSiMe(6)(Ar=3,5-MeCH) were synthesized and structurally characterized,and proved to be effective catalysts for the disproportionation of cyclohexadienes and isomerization of terminal ***~1 H NMR spectrum suggested that the bridging nitrogen ligand remains intact during the catalytic reaction,indicating possible catalytic ability of the Mo-N=N motif.

关键词： dinitrogen fixation dinitrogen-metal complex catalytic ability disproportionation isomerization