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学者姓名：袁耀锋
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Abstract ：
This study presents the design, synthesis, and comprehensive characterization of a novel series of D-π-A type malononitrile-derived chromophores, BTC-1–BTC-4. Combining various spectroscopic techniques, nonlinear Z-scan measurements, and quantum chemical calculations, we revealed the intricate relationship between nonlinear optical properties and the interplay of molecular structure, intramolecular charge transfer (ICT), and dipole moments (μ). Our experimental and computational findings corroborate that the polarization degree in the ground state, the charge separation in the excited state and twisted intramolecular charge transfer (TICT) collectively dictate the nonlinear optical properties of the compounds. Notably, BTC-1 exhibits an exceptional nonlinear absorption coefficient β value (2×10−8 m W−1), attributed to its optimized charge transfer efficiency and pronounced degree of charge separation. Our findings provide actionable insights for the rational design of high-performance organic Nonlinear optics (NLO) materials with potential applications in advanced photonic devices. © 2024 Wiley-VCH GmbH.
Keyword ：
Alkylation Alkylation Aromatic compounds Aromatic compounds Charge transfer Charge transfer Chromophores Chromophores Organometallics Organometallics Spectroscopic analysis Spectroscopic analysis
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| GB/T 7714 | Zhu, Xiang-Zhao , Chen, Song-Hua , Xu, Jia-Bei et al. Unveiling the Twisted Aromatic Donor Effect on the Nonlinear Response of D-π-A Type Malononitrile-Derived Chromophores [J]. | Chemistry - A European Journal , 2024 , 30 (53) . |
| MLA | Zhu, Xiang-Zhao et al. "Unveiling the Twisted Aromatic Donor Effect on the Nonlinear Response of D-π-A Type Malononitrile-Derived Chromophores" . | Chemistry - A European Journal 30 . 53 (2024) . |
| APA | Zhu, Xiang-Zhao , Chen, Song-Hua , Xu, Jia-Bei , Huang, Jian-hua , Yan, Jian-Feng , Yuan, Yao-Feng . Unveiling the Twisted Aromatic Donor Effect on the Nonlinear Response of D-π-A Type Malononitrile-Derived Chromophores . | Chemistry - A European Journal , 2024 , 30 (53) . |
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Two o-carborane based tetraphenylethene (TPE) cationic cyclophanes O1·4PF6 and O2·4PF6 were synthesized through an SN2 reaction. Their structures were confirmed both possessing Z-shaped cavities in single crystal analysis. The optical properties of these macrocycles were systematically investigated using UV–vis spectroscopy and fluorescence techniques. It is worth noting that the introduction of a methoxy group to the TPE unit enables the synthesis of a near-infrared-emitting macrocycle O2·4PF6. The recognition behaviors of these two macrocycles towards nucleotides were investigated using various techniques including fluorescence titration, UV–vis titration, and transmission electron microscopy (TEM). Interestingly, these cyclophanes exhibited aggregation-induced emission (AIE) effects in water or under the induction of nucleotides. © 2024
Keyword ：
AIE effect AIE effect Cationic cyclophanes Cationic cyclophanes Nucleotides Nucleotides o-Carborane o-Carborane Tetraphenylethene Tetraphenylethene
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| GB/T 7714 | Chen, R. , Liu, J. , Lin, C. et al. Synthesis and properties of tetraphenylethene cationic cyclophanes based on o-carborane skeleton [J]. | Chinese Chemical Letters , 2024 , 35 (12) . |
| MLA | Chen, R. et al. "Synthesis and properties of tetraphenylethene cationic cyclophanes based on o-carborane skeleton" . | Chinese Chemical Letters 35 . 12 (2024) . |
| APA | Chen, R. , Liu, J. , Lin, C. , Li, Y. , Geng, Y. , Yuan, Y. . Synthesis and properties of tetraphenylethene cationic cyclophanes based on o-carborane skeleton . | Chinese Chemical Letters , 2024 , 35 (12) . |
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Efficient control over several possible reaction pathways of free radicals is the chemical basis of their highly selective transformations. Among various competing reaction pathways, sulfonimidyl radicals generated from the electrolysis of 2-alkynylbenzenesulfonamides undergo cascade migratory or ortho-cyclization cyclization selectively. It is found that the incorporation of an extra 2-methyl substituent biases the selective migration of the acyl- over vinyl-linker of the key spirocyclic cation intermediate and thus serves as an enabling handle to achieve the synthetically interesting yet under-investigated cascade migratory cyclization of spirocyclic cations.
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| GB/T 7714 | Shi, Zhaojiang , Dong, Shicheng , Liu, Ting et al. Electrochemical cascade migratory versus ortho-cyclization of 2-alkynylbenzenesulfonamides [J]. | CHEMICAL SCIENCE , 2024 , 15 (8) : 2827-2832 . |
| MLA | Shi, Zhaojiang et al. "Electrochemical cascade migratory versus ortho-cyclization of 2-alkynylbenzenesulfonamides" . | CHEMICAL SCIENCE 15 . 8 (2024) : 2827-2832 . |
| APA | Shi, Zhaojiang , Dong, Shicheng , Liu, Ting , Wang, Wei-Zhen , Li, Nan , Yuan, Yaofeng et al. Electrochemical cascade migratory versus ortho-cyclization of 2-alkynylbenzenesulfonamides . | CHEMICAL SCIENCE , 2024 , 15 (8) , 2827-2832 . |
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Abstract ：
The development of efficient and sustainable methods to obtain spirocyclic compounds is of significance as these structures are widely found in pharmaceuticals and agrochemicals. Herein, we disclose an electrochemical dearomative spirocyclization of N-acyl sulfonamides in a continuous-flow cell. The reaction is simple and efficient without external catalysts or supporting electrolytes and could be applied in a decagram-scale synthesis.
Keyword ：
Continuous-flow Continuous-flow Cyclization Cyclization Dearomatization Dearomatization Electrochemistry Electrochemistry Methodology and reactions Methodology and reactions Spirocyclization Spirocyclization Sulfonamides Sulfonamides
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| GB/T 7714 | Liu, Ting , Shi, Zhaojiang , Yuan, Yaofeng et al. Electrochemical Dearomative Spirocyclization of N-Acyl Sulfonamides in a Continuous-Flow Cell [J]. | CHINESE JOURNAL OF CHEMISTRY , 2024 , 42 (9) : 980-984 . |
| MLA | Liu, Ting et al. "Electrochemical Dearomative Spirocyclization of N-Acyl Sulfonamides in a Continuous-Flow Cell" . | CHINESE JOURNAL OF CHEMISTRY 42 . 9 (2024) : 980-984 . |
| APA | Liu, Ting , Shi, Zhaojiang , Yuan, Yaofeng , Lin, Yuqi , Ye, Ke-Yin . Electrochemical Dearomative Spirocyclization of N-Acyl Sulfonamides in a Continuous-Flow Cell . | CHINESE JOURNAL OF CHEMISTRY , 2024 , 42 (9) , 980-984 . |
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Here, α- or β-thiophene-substituted derivatives bridged by an o-carborane group were synthesized. Scanning tunneling microscope break junction techniques have revealed that the thiophene anchoring groups form a single-molecule junction with an Au electrode. Flicker noise analysis suggests the existence of through-space transmission pathways between the thiophene units. Furthermore, the electronic coupling of the β-thiophene substituted molecule with the electrode is found to be more stable, resulting in a 70 % increase in conductance compared to the α-isomer counterpart.These findings offer valuable insights for the design and development of o-carborane-based molecules, underscoring the significance of molecular backbones and substitution patterns on their electrical transport properties. © 2024
Keyword ：
Electronic coupling Electronic coupling O-carborane O-carborane Single-molecule conductance Single-molecule conductance STM-BJ STM-BJ Thiophene Thiophene
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| GB/T 7714 | Chen, Z.-Y. , Dai, Y.-H. , Xu, S.-N. et al. Synthesis, characterization, and electronic transport properties of o-carborane-bridged thiophene derivatives [J]. | Journal of Organometallic Chemistry , 2024 , 1016 . |
| MLA | Chen, Z.-Y. et al. "Synthesis, characterization, and electronic transport properties of o-carborane-bridged thiophene derivatives" . | Journal of Organometallic Chemistry 1016 (2024) . |
| APA | Chen, Z.-Y. , Dai, Y.-H. , Xu, S.-N. , Yan, J.-F. , Geng, Y.-H. , Yuan, Y.-F. . Synthesis, characterization, and electronic transport properties of o-carborane-bridged thiophene derivatives . | Journal of Organometallic Chemistry , 2024 , 1016 . |
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Abstract ：
Organic nonlinear optical materials have attracted much attention due to their large nonlinear optical coefficients and ultrafast response speeds, as well as their potential applications in optical limiting (OL). Among them, nonlinear optical materials with phenanthrenone as the backbone are consistently understudied. We have successfully realized the transformation of organic small molecules in the nonlinear optical direction by replacing the carbonyl group on the structure of phenanthrenone with a malononitrile group. The nonlinear optical properties of CN-2 were investigated under different excitation conditions at 532 nm and the kinetic process of nonlinear optics was analyzed by transient absorption spectroscopy. In addition, we also investigated the OL properties of CN-2 , and the OL experiments showed that CN-2 with a lower OL threshold has superior OL properties than C 60 .
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| GB/T 7714 | Chen, Songhua , Zhu, Xiangzhao , Zhang, Ruiying et al. Third-order nonlinear optics and optical limiting of phenanthrenone derivatives [J]. | DYES AND PIGMENTS , 2024 , 225 . |
| MLA | Chen, Songhua et al. "Third-order nonlinear optics and optical limiting of phenanthrenone derivatives" . | DYES AND PIGMENTS 225 (2024) . |
| APA | Chen, Songhua , Zhu, Xiangzhao , Zhang, Ruiying , Huang, Mingyang , Song, Yinlin , Huang, Jianhua et al. Third-order nonlinear optics and optical limiting of phenanthrenone derivatives . | DYES AND PIGMENTS , 2024 , 225 . |
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Development of earth-abundant, low-cost and easily synthesizable catalysts for the semi-hydrogenation of acetylene is urgently needed. Here, we have systematically investigated the structure, electronic properties, hydrogen dissociation, and acetylene semi-hydrogenation activity and selectivity of poly(heptazine imide) (PHI) loaded with different sizes of Cun (n = 1,2,4,13) clusters (Cun/PHI) by density functional theory calculations. The results show that Cu4/PHI with tetrahedral configuration has a better hydrogenation activity in the acetylene semi-hydrogenation reaction with H adsorbed in the vicinity of acetylene and subsequent intermediates in a non-bridge position, resulting in a smaller hydrogenation energy barrier. In addition, the top Cu atom transfers a large number of electrons to the bottom Cu atoms and PHI, and only a small number of electrons transfer to ethylene, resulting in weak adsorption of ethylene and easy desorption, which makes it good selectivity and therefore it can be used as a candidate catalyst for the semi-hydrogenation of acetylene. This study provides insights into the design of catalysts with suitable size clusters loaded on carbon nitride materials for efficient acetylene semi-hydrogenation reactions. © 2024 Elsevier B.V.
Keyword ：
Acetylene Acetylene Carbon nitride Carbon nitride Copper alloys Copper alloys Hydrogenation Hydrogenation Reaction intermediates Reaction intermediates
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| GB/T 7714 | Chen, Xiaoxiao , Li, Yi , Yuan, Yaofeng et al. What size of Cun clusters loaded on poly(heptazine imide) have better catalytic performance for acetylene semi-hydrogenation? [J]. | Molecular Catalysis , 2024 , 569 . |
| MLA | Chen, Xiaoxiao et al. "What size of Cun clusters loaded on poly(heptazine imide) have better catalytic performance for acetylene semi-hydrogenation?" . | Molecular Catalysis 569 (2024) . |
| APA | Chen, Xiaoxiao , Li, Yi , Yuan, Yaofeng , Lin, Wei . What size of Cun clusters loaded on poly(heptazine imide) have better catalytic performance for acetylene semi-hydrogenation? . | Molecular Catalysis , 2024 , 569 . |
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Polyferrocene macrocycles hold immense potential in the fields of molecular electronics and electrochemistry, primarily due to their multiple metal centers. However, developing highly efficient synthetic strategies for constructing these rings remains a significant challenge. In this study, we successfully synthesized triferrocenyl macrocycles using Pt-mediated coupling strategy and determined their configuration using single-crystal X-ray diffraction analysis, revealing a structure reminiscent of the Penrose Stair. We comprehensively investigated the macrocycle’s structure, photophysical properties, and employed density functional theory (DFT) calculations to gain further insights. Notably, this macrocycle exhibits several advantageous features, including a flexible structure, good solubility, and a highly efficient synthetic pathway. (Figure presented.). © Jilin University, The Editorial Department of Chemical Research in Chinese Universities and Springer-Verlag GmbH 2024.
Keyword ：
Conjugated macrocycle Conjugated macrocycle Organometallic macrocycle Organometallic macrocycle Pt-template method Pt-template method
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| GB/T 7714 | Xu, J. , Lan, B. , Zhu, L. et al. Synthesis and Properties of Ferrocene Conjugated Macrocycles with Illusory Topology of the Penrose Stairs [J]. | Chemical Research in Chinese Universities , 2024 , 40 (5) : 881-886 . |
| MLA | Xu, J. et al. "Synthesis and Properties of Ferrocene Conjugated Macrocycles with Illusory Topology of the Penrose Stairs" . | Chemical Research in Chinese Universities 40 . 5 (2024) : 881-886 . |
| APA | Xu, J. , Lan, B. , Zhu, L. , Xu, H. , Chen, X. , Li, W. et al. Synthesis and Properties of Ferrocene Conjugated Macrocycles with Illusory Topology of the Penrose Stairs . | Chemical Research in Chinese Universities , 2024 , 40 (5) , 881-886 . |
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Both synthesis and DFT calculation of [3 + 2] cycloaddition reaction (32CA) of quinolone-5,8-dione with 1,3dipole CF3CHN2 are studied. The focus of this work is to study the orbital interactions of this reaction by using molecular orbital tracing (MOT) method. MOT result shows that both quinolone-5,8-dione and CF3CHN2 use three electrons occupied molecular orbitals (MOs) to interact with each other, and the evolutive courses of the six molecular orbitals of reactants (initial MOs) to six electrons occupied molecular orbitals of product (final MOs) are given in this work. Three of the six initial MOs can evolve as final MOs directly, but rest of them need to go through media orbitals to complete the evolution. Perhaps the role of the media orbitals is to enable the reaction to proceed concertedly. APT charges analysis and changes of bond lengths during the reaction are also afforded in this work, and the result shows that the reaction begins with a nucleophilic attack of CF3CHN2 on quinolone-5,8-dione. Accompanying with the attack, negative charge transfers from CF3CHN2 to a carbon atom of quinolone-5,8-dione, then the carbon atom attacks nitrogen atom of CF3CHN2 to complete the cycloaddition. At last, a mechanism and a diagram of the molecular orbital interactions of the reaction are given.
Keyword ：
[3+2] cycloaddition reaction [3+2] cycloaddition reaction DFT calculation DFT calculation Media orbital Media orbital Molecular orbital tracing Molecular orbital tracing synthesis synthesis
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| GB/T 7714 | Huang, Zhiyong , Lei, Chun , Cheng, Yao et al. A study on the orbital interactions of [3+2] cycloaddition by means of molecular orbital tracing method [J]. | JOURNAL OF MOLECULAR STRUCTURE , 2024 , 1306 . |
| MLA | Huang, Zhiyong et al. "A study on the orbital interactions of [3+2] cycloaddition by means of molecular orbital tracing method" . | JOURNAL OF MOLECULAR STRUCTURE 1306 (2024) . |
| APA | Huang, Zhiyong , Lei, Chun , Cheng, Yao , Yuan, Yaofeng , Zhang, Yongfan , Wang, Wenfeng . A study on the orbital interactions of [3+2] cycloaddition by means of molecular orbital tracing method . | JOURNAL OF MOLECULAR STRUCTURE , 2024 , 1306 . |
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Abstract ：
A class of side-chain type ferrocene macrocycles with a radially conjugated system is introduced in this study. The stereo configurations of these ferrocene rings were determined through single-crystal X-ray diffraction analysis. Notably, in the solid state, the ferrocene rings exhibit a distinctive herringbone stacking pattern imposed by a ferrocene-to-ring host-guest interaction. Through UV-vis absorption spectroscopy, electrochemical measurements, and theoretical calculations, valuable insights into the electronic properties of these rings were obtained. In addition, the single crystal of macrocycle A2B demonstrates a second-order nonlinear optical response. As a class of organometallic nanorings, this work holds great potential for further exploration in the fields of organometallic chemistry, molecular electronics, and host-guest chemistry. © 2024 The Authors. Co-published by University of Science and Technology of China and American Chemical Society.
Keyword ：
Conjugated Macrocycles Conjugated Macrocycles Ferrocene Ferrocene Nanoring Nanoring Organometallic Macrocycles Organometallic Macrocycles Second-Order Nonlinear Optical Second-Order Nonlinear Optical
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| GB/T 7714 | Lan, B. , Xu, J. , Zhu, L. et al. Side-Chain Type Ferrocene Macrocycles [J]. | Precision Chemistry , 2024 , 2 (4) : 143-150 . |
| MLA | Lan, B. et al. "Side-Chain Type Ferrocene Macrocycles" . | Precision Chemistry 2 . 4 (2024) : 143-150 . |
| APA | Lan, B. , Xu, J. , Zhu, L. , Chen, X. , Kono, H. , Wang, P. et al. Side-Chain Type Ferrocene Macrocycles . | Precision Chemistry , 2024 , 2 (4) , 143-150 . |
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