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Pd-catalyzed intermolecular Si–O formation via Si–C activation

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Science China chemistry 2024年第8期67卷 2661-2669页

作者： Shuang Liu Yu-Shu Chen Yichen Wu Peng Wang State Key laboratory of Organometallic chemistry Shanghai Institute of Organic ChemistryUniversity of Chinese Academy of SciencesShanghai 200032China School of chemistry and Materials Science Hangzhou Institute for Advanced StudyUniversity of Chinese Academy of SciencesHangzhou 310024China College of Material chemistry and Chemical Engineering Key Laboratory of Organosilicon Chemistryand Material Technology of Ministry of EducationHangzhou Normal UniversityHangzhou 311121China

The development of efficient Si–O bond formation reaction with 100% atom-economy, excellent functional group tolerance, and broad scope under mild conditions is highly desired due to the prevalence of silanol, silyl ether, and their derivatives in synthetic chemistry and materials science. Here, we have realized the Pd-catalyzed Si–O formation reaction via a Si–C activation approach with 100% atom-economy by employing silacyclobutanes(SCBs) and various hydroxy-containing substrates, including water,alcohols, phenols, and silanols. This protocol features a broad substrate scope, remarkable functional compatibility and mild conditions, providing a series of silanols, silyl ethers in high efficiency. Notably, this protocol could also be used for selective protection of hydroxy functionalities, and for the access of a class of novel polymers containing Si–O main chain. Preliminary mechanistic studies unveiled that this reaction underwent a Pd-catalyzed concerted ring-opening mechanism.

关键词： Si–O formation Si–C activation palladium silacyclobutane silanol silyl ether

Transition-metal free trifluoromethylimination of alkenes enabled by direct activation of N-unprotected ketimines

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Chinese Chemical Letters 2024年第9期35卷 155-159页

作者： Boqiang Wang Yongzhuo Xu Jiajia Wang Muyang Yang Guo-Jun Deng Wen Shao Key laboratory for Green organic Synthesis and Application of Hunan Province Key Laboratory of Environmentally Friendly Chemistry and Application of Ministry of EducationCollege of ChemistryXiangtan UniversityXiangtan 411105China Department School of chemistry and Chemical Engineering Henan Normal UniversityXinxiang 453007China

A highly site-selective intermolecular trifluoromethylimination of activated and unactivated olefins was reported under transition-metal-and photosensitizer-free *** newly developed strategy provides straightforward and efficient access to diverse value-added vicinal trifluoromethyl amines without resorting to the pre-functionalized *** experiments demonstrate that the approach proceeded through CF_(3)and iminyl two-radicals process,which were generated directly from commercially available benzophenone imine in a novel electron-donor mode via a SET process activated by the bifunctional hypervalent iodine *** synthetic potential of the protocols was further showcased via the condensation/amination sequential cascade,and transformations to accessβ-CF_(3)primary amines.

关键词： Transition-metal free Alkenes difunctionalization Amination Trifluoromethylation Single-electron transfer

Illuminating spin-crossover octanuclear metal-organic cages

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Science China chemistry 2024年第4期67卷 1208-1215页

作者： Zhi-Kun Liu Alyona A.Starikova Yu-Xia Li Ke Sun Meng Yu Zi-Shuo Yao Jun Tao Key laboratory of Cluster Science of Ministry of Education School of Chemistry and Chemical EngineeringLiangxiang CampusBeijing Institute of TechnologyBeijing 102488China Institute of Physical and organic chemistry Southern Federal UniversityRostov-on-Don 344090Russia

Spin-crossover(SCO)materials that reversibly switch between high-and low-spin states have potential for the storage of spin state-relative information,and have gained much attention incorporating secondary physical properties,such as fluorescence and magneto-optical *** this study,we synthesized three octanuclear metal-organic cages(MOCs)using tetraphenylethylene-based luminophores,aldehydes,and Fe^(Ⅱ)salts,by subcomponent self-assembly approach,namely[Fe1]-[Fe3].By controlling the ligand-field strength and guest encapsulation,we finely tuned their SCO *** them,MOC[Fe2]displayed nearly complete SCO behavior in the solid state,which is rare for high-nuclearity *** also demonstrated the coupling of SCO with fluorescence emission in these MOCs by using isostructural Zn^(Ⅱ)complexes([Zn1]-[Zn3])as control experiments,for the first *** calculations revealed the energy-transfer mechanism between fluorophores and SCOactive centers,which emphasizes the significant contribution of d-d transitions in the interplay between the occurrence of SCO and fluorescence emission.

关键词： metal-organic cages spin crossover fluorescence switching materials DFT calculation

TCP-1,a novel peptide to diagnose early colon cancer

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Chinese Chemical Letters 2024年第3期35卷 226-233页

作者： Hang Yu Baoying Wen Min Huang Ru Feng Libin Pan Manyi Xu Hao Lin Lin Cong Sen Zhang Yan Li Chi-Hin Cho Chongjing Zhang Xiaoguang Chen Yan Wang State Key laboratory of Bioactive substances and Functions of natural Medicines Institute of Materia MedicaChinese Academy of Medical SciencesBeijing 100050China School of Biomedical Sciences Faculty of MedicineThe Chinese University of Hong KongHong KongChina

A nine cyclic peptide(TCP-1)showed excellent specificity for colon ***-1 binds with human tumor tissues at early stages and mice tumor with diameters of 1-4 mm,suggesting that TCP-1 may be used for early diagnosis of colon *** mechanism of the targeted binding of TCP-1 to colon cancer was also studied using immunoprecipitation,LC-MS and *** screening and identifying of the possible binding target proteins of TCP-1,keratin,typeⅡcytoskeletal 5 was speculated to be the specific binding target protein of TCP-1 in human tumor *** studies were conducted to investigate the target-mediated drug disposition of the new tumor-specific peptide by LC-MS/*** tissue distribution study showed that TCP-1 was found only in colon tumors(the target site)in tumor mice did not bind to any other *** TCP-1 to tumor markedly increased its removal rate from blood circulation but mildly extended its staying time in *** tumor mice,a lower AUC of TCP-1(reduced by almost 35%)and 2-fold higher clearance were found compared to that of normal *** proposed metabolic pathway of TCP-1 in the kidney was also determined using LC-MS^(n)-*** high specificity and low toxicity of the peptide may be caused by its extremely tight binding to the *** applications for future clinical use,including MRI and PET/CT were also explored,and this research may promote the development of colon cancer diagnostic technology research and provide new ideas and technical routes for tumor diagnostic technology.

关键词： Colon cancer TCP-1 Peptide Cytokeratin 5 Pharmacokinetics/pharmacodynamics(PK/PD)

Designing Tough,Printable,and Adaptable Eutectogels with Multinetworks via Synergy of Rapid Orthogonal Photopolymerizations and Solvent Effect in Seconds

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CCS chemistry 2024年第2期6卷 390-402页

作者： Jupen Liu Lijun Zhou Ping Zhang Yanxia Zhao Hongqiu Wei You Yu Key laboratory of Synthetic and natural Functional Molecule chemistry of the Ministry of Education College of Chemistry and Materials ScienceNorthwest UniversityXi’an 710069

Achieving a straightforward design of tough,printable,and adaptable polymeric eutectogels is still challenging in related fields due to the uncontrollable polymerization and solvent-exchanging processes,and inherent contrasting multiple ***,we report a one-step synergistic strategy based on ruthenium chemistry-catalyzed photopolymerization and solvent effect for preparing high-performance *** orthogonal ruthenium photochemistry helps multinetworks formation via phenol-coupling of gelatin and copolymerization of acrylamide(AAm)and[2-(methacryloyloxy)ethyl]trimethylammonium tetrafluoroborate(META)monomers in *** obvious difference in the supramolecular interactions of free AAm monomers and polymerized units in P(AAm-co-META)with deep eutectic solvents(DESs)significantly promotes the microphase-separation behavior in ***,the in situ polymerization and microphase-separation behavior enable the as-prepared eutectogel materials to have excellent mechanical properties(stress of∼1.2 MPa),toughness(∼4.0 MJ m^(−3)),elasticity,adaptivity,and conductivity(∼0.5 S m^(−1)at room temperature).Also,the critical strength of the resultant eutectogels can be modulated by varying the DES *** rapid and well-controlled synergistic approach is compatible with extrusion printing techniques to make flexible sensors with high sensitivities and response times to detect pressure in a range of 0–500 *** a general and simple strategy has application potential in biological,engineering,and material sciences.

关键词： orthogonal chemistry visible-light photopolymerization solvent effect microphase separation adaptable polymers printable eutectogels

Twisted Phosphors that Violate Kasha's Exciton Model in organic Systems

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Chinese Journal of chemistry 2024年第11期42卷 1237-1246页

作者： Boyi Fu Guangming Wang Jiuyang Li Junbo Li Xun Li Xiaoya Zhao Shuhui Ding Guoping Yan Qianqian Yan Kaka Zhang School of Materials Science and Engineering Wuhan Institute of TechnologyWuhanHubei430205 China Key laboratory of Synthetic and Self-Assembly chemistry for organic Functional Molecules Shanghai Institute of Organic ChemistryUniversity of Chinese Academy of SciencesChinese Academy of Sciences345 Lingling RoadShanghai200032 China

Kasha's exciton model proposes that T1 energy levels of organic compounds are insensitive to molecular aggregation and microenvironment change because of negligible small transition dipole moments of T1 *** model holds true in most organic systems till *** we report the fabrication of twisted organic phosphors with intramolecular charge transfer characters and flexible molecular *** doped into different organic matrices,the twisted phosphor adopts different conformation,exhibits distinct phosphorescence colors and T1 energy levels,which violates Kasha's exciton model in organic *** that the change of phosphorescence colors and maxima can be readily distinguished by human eyes and conventional instrument,the twisted phosphors would be exploited as a new type of molecular probe,which would exhibit potential application in optical sensing and stimuli-responsive systems.

关键词： Afterglow Twisted phosphor Triplet excited state Room-temperature phosphorescence Luminescence Spin-orbit coupling

Synthesis and Modulation of Low-Dimensional Transition Metal Chalcogenide Materials via Atomic Substitution

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Nano-Micro Letters 2024年第9期16卷 49-94页

作者： Xuan Wang Akang Chen XinLei Wu Jiatao Zhang Jichen Dong Leining Zhang Key laboratory of Cluster Science Ministry of Education of ChinaBeijing Key Laboratory of Photoelectronic and Electrophonic Conversion MaterialsSchool of Chemistry and Chemical EngineeringBeijing Institute of TechnologyBeijing 100081People’s Republic of China Beijing National laboratory for Molecular Sciences Key Laboratory of Organic SolidsInstitute of Chemistry Chinese Academy of SciencesBeijing 100190People’s Republic of China

In recent years,low-dimensional transition metal chalcogenide(TMC)materials have garnered growing research attention due to their superior electronic,optical,and catalytic properties compared to their bulk *** controllable synthesis and manipulation of these materials are crucial for tailoring their properties and unlocking their full potential in various *** this context,the atomic substitution method has emerged as a favorable *** involves the replacement of specific atoms within TMC structures with other elements and possesses the capability to regulate the compositions finely,crystal structures,and inherent properties of the resulting *** this review,we present a comprehensive overview on various strategies of atomic substitution employed in the synthesis of zero-dimensional,one-dimensional and two-dimensional TMC *** effects of substituting elements,substitution ratios,and substitution positions on the structures and morphologies of resulting material are *** enhanced electrocatalytic performance and photovoltaic properties of the obtained materials are also provided,emphasizing the role of atomic substitution in achieving these ***,challenges and future prospects in the field of atomic substitution for fabricating low-dimensional TMC materials are summarized.

关键词： Transition metal chalcogenides Atomic substitution Ion exchange Low-dimensional materials Controllable synthesis

A robust indium-organic framework with open tubular channels for efficient separation of acetylene

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Nano Research 2024年第4期17卷 3139-3146页

作者： Yong-Zhi Li Gang-Ding Wang Fan Xu Qing Yin Danyang Zhao Jiqiu Qi Yanwei Sui Lei Hou Yao-Yu Wang School of Materials and Physics China University of Mining and TechnologyXuzhou 221116China Key laboratory of Synthetic and natural Functional Molecule of the Ministry of Education Shaanxi Key Laboratory of Physico-Inorganic ChemistryCollege of Chemistry&Materials ScienceNorthwest UniversityXi’an 710069China

Considering the tremendous applications and purification requirement of acetylene(C_(2)H_(2)),seeking appropriate adsorbents with high capacity and selectivity is a vital task and remains an enduring ***,we designed and synthesized a robust three-dimensional(3D)indium-organic framework([(Me)_(2)NH_(2)][In(L6)_(0.5)(IPA)_(0.5)]·DMA·2H_(2)O(In-L6-IPA,DMA=dimethylammonium,IPA=isopropyl alcohol))featuring two types of one-dimensional(1D)tubular *** activated In-L6-IPA displayed high loading for C_(2)H_(2)(104.4 cm^(3)·g^(-1),the second highest value among all reported indium-based metal-organic frameworks(MOFs))and simultaneously selective adsorption for C_(2)H_(2) over CO_(2),C_(2)H_(6),and ethylene(C_(2)H_(4))at 298 K under 100 *** modelling revealed that the porous wall of In-L6-IPA provides more and stronger multiple interactions for C_(2)H_(2) than CO_(2),C_(2)H_(6),and C_(2)H_(4) containing C–H···π,C–H···O,and O···π*** experiments validated the actual separation ability for various ratios of binary C_(2)H_(2)/C_(2)H_(4) and C_(2)H_(2)/CO_(2) mixtures as well as equimolar ternary C_(2)H_(2)/C_(2)H_(4)/CO_(2) and C_(2)H_(2)/C_(2)H_(4)/C_(2)H_(6) mixtures with excellent reusability.

关键词： indium-organic framework crystal structure gas adsorption acetylene(C_(2)H_(2))separation

Denitration of Nitroarenes Under Ambient Physiological Conditions Catalyzed by Graphdiyne-Supported Palladium

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CCS chemistry 2024年第3期6卷 641-651页

作者： Endong Zhang Yanyan Chen Fengting Lv Zicheng Zuo Feng He Yongjun Li Yiming Huang Yuliang Li Shu Wang Beijing National laboratory for Molecular Sciences Key Laboratory of Organic SolidsInstitute of ChemistryChinese Academy of SciencesBeijing 100190 College of chemistry University of Chinese Academy of SciencesBeijing 100049

The direct cleavage of C–NO_(2)bonds for reductive denitration of nitroarenes remains a challenging transformation in synthetic organic ***,we report a biocompatible palladium-deposited graphdiyne nanocatalyst(Pd@GDY/DSPE-PEG)that can catalyze reductive denitration of nitroarenes under ambient physiological *** studies support this transformation via the oxidative addition of nitroarenes with Pd(0)and subsequent ligand exchange to form arylpalladium *** one-step reductive denitration via Pd@GDY/DSPE-PEG successfully facilitates the repair of the nitrated proteins arising from endogenic ONOO−and restores their physiological function,including blocking the apoptosis pathway in living ***,Pd@GDY/DSPE-PEG was further successfully applied for catalytic denitration to reduce the level of 3-nitrotyrosine residues of proteins located in the mouse brain hippocampus in *** study provides an ideal strategy for designing highly active enzymatic mimicking synthetic catalysts for the regulation of the nitrated protein level and the detoxification of nitrative damage of living cells and tissues.

关键词： 3-nitrotyrosine artificial nanaocatalysts reductive denitration palladium-deposited graphdiyne repairing nitrated protein