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学者姓名：郭智勇
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Abstract ：
The ability to rapidly produce large single crystals is crucial for advancing the applications of covalent organic frameworks (COFs). Although the modulation strategy provides a straightforward method for growing high-quality single crystals, the slow crystallization process of COFs often limits their practical use. In this study, we combined the principles of crystallization thermodynamics and kinetics with the modulation strategy to develop a binary solvent-supersaturation method, enabling the growth of single-crystal COFs in a significantly shorter time. By systematically investigating the crystal-growth kinetics across different solvent ratios, we established a diffusion-reaction growth model, highlighting the essential role of supersaturation in controlling COF crystal growth. Especially, under this crystallization guidance, elegant single crystals of COFs built with heteroatom or other functionality can also facilely obtained, which spontaneously validate the universality of the protocol. Importantly, the resulting single-crystal COFs, characterized by high structural symmetry, exhibited notable second harmonic generation (SHG) activity, which could open new avenues for future research in this field.
Keyword ：
Binary solvent-supersaturation Binary solvent-supersaturation Crystal-growth kinetics Crystal-growth kinetics Diffusion-reaction growth model Diffusion-reaction growth model Second harmonic generation Second harmonic generation Single-crystal Single-crystal
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| GB/T 7714 | Jia, Ruiqiang , Ye, Ronglong , Chang, Zhen et al. Supersaturation-Controlled Single-Crystal Growth of Covalent Organic Frameworks with Binary Solvents [J]. | CHEMISTRY-A EUROPEAN JOURNAL , 2025 , 31 (22) . |
| MLA | Jia, Ruiqiang et al. "Supersaturation-Controlled Single-Crystal Growth of Covalent Organic Frameworks with Binary Solvents" . | CHEMISTRY-A EUROPEAN JOURNAL 31 . 22 (2025) . |
| APA | Jia, Ruiqiang , Ye, Ronglong , Chang, Zhen , Yu, Hao , Wang, Ming , Xu, Guohai et al. Supersaturation-Controlled Single-Crystal Growth of Covalent Organic Frameworks with Binary Solvents . | CHEMISTRY-A EUROPEAN JOURNAL , 2025 , 31 (22) . |
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Room-temperature phosphorescence (RTP) emissions of metal-free organic materials have garnered considerable research attention from the fields of organic electronics and bioelectronics. However, achieving ultralong phosphorescence lifetimes and high quantum efficiencies of pure organic materials without relying on the heavy-atom effect remains challenging. Herein, a heavy-metal-free organic compound-1,4-phenylenebis((4-(9H-carbazol-9-yl)phenyl)methanone) (BCzPMB)-exhibiting two types of crystal structures with highly efficient afterglow features was synthesized. In these crystals, BCzPMB-DCM exhibited a high phosphorescence quantum efficiency of 9.1% and a lifetime of 368.7 ms. BCzPMB-N showed a phosphorescence quantum efficiency of 5.7% and a lifetime of 404.9 ms. Experimental and theoretical studies attributed this persistent RTP emission to intermolecular interactions, including pi-pi and intermolecular hydrogen bonding interactions. Additionally, the luminescence behavior of BCzPMB-DCM resembled that of BCzPMB-N after treatment with n-hexane, and a visual anticounterfeiting application instance was successfully demonstrated. Overall, the results of this study are anticipated to provide valuable insights for advancing the applications of organic luminogens with RTP properties.
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| GB/T 7714 | Xiao, Hui , Ma, Huili , Wang, Jingyi et al. Crystallization-induced highly efficient phosphorescence in metal-free organic phosphors [J]. | CRYSTENGCOMM , 2025 , 27 (18) : 2931-2936 . |
| MLA | Xiao, Hui et al. "Crystallization-induced highly efficient phosphorescence in metal-free organic phosphors" . | CRYSTENGCOMM 27 . 18 (2025) : 2931-2936 . |
| APA | Xiao, Hui , Ma, Huili , Wang, Jingyi , An, Zhongfu , Guo, Zhiyong . Crystallization-induced highly efficient phosphorescence in metal-free organic phosphors . | CRYSTENGCOMM , 2025 , 27 (18) , 2931-2936 . |
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Covalent organic frameworks (COFs) with ordered pi structures are very promising in porous light-emitting materials. However, most of these COFs are either poor in luminescence or lack of water-stability. Herein, a series of isostructural D-A vinylene-linked COFs were constructed based a new D2h symmetric linker 1,4-bis(4,6-dimethyl-1,3,5-triazin-2-yl)benzene (TMTA) with high crystallinity, comparative high surface area and excellent chemical/thermal stability. Impressively, their adsorption and luminescence wavelength vary with respect to the density of pi-systems in the electron-donating group, which constitute the foundation for molecular engineering the luminescent properties of vinylene-linked COFs. The DFT calculations further established the relationship between the luminescence properties and the donor electronic structure. Moreover, one of representative COF named FZU-203 showed inspiring applications in bioimaging, which may further provide strategic guidance for the use of vinylene-linked COFs as fluorescent nanoprobes in non-invasive medical diagnosis and visualization therapy of tumors. A series of isostructural vinylene-linked 2D COFs were constructed based on a new tetratopic D2h-symmetric monomer with two highly electron deficient s-triazine core. The fluorescence emission of the resulting D-A type COFs red-shifted with respect to the enhancement of the electronegativity of the donor unit. Their ability in non-invasive tumor visualization was further demonstrated. image
Keyword ：
and Cell imaging and Cell imaging Donor-acceptor (D-A) interaction Donor-acceptor (D-A) interaction Tunable emission Tunable emission Vinylene-linked COFs Vinylene-linked COFs
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| GB/T 7714 | Wang, Jun , Wang, Jiande , Qiao, Shujie et al. Modular Construction of Vinylene-Linked Covalent Organic Frameworks with Tunable Emission for Tumor Visualization [J]. | CHEMISTRY-A EUROPEAN JOURNAL , 2024 , 30 (36) . |
| MLA | Wang, Jun et al. "Modular Construction of Vinylene-Linked Covalent Organic Frameworks with Tunable Emission for Tumor Visualization" . | CHEMISTRY-A EUROPEAN JOURNAL 30 . 36 (2024) . |
| APA | Wang, Jun , Wang, Jiande , Qiao, Shujie , Guo, Zhiyong . Modular Construction of Vinylene-Linked Covalent Organic Frameworks with Tunable Emission for Tumor Visualization . | CHEMISTRY-A EUROPEAN JOURNAL , 2024 , 30 (36) . |
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As one of the most direct methods to construct molecular scaffolds in fine chemicals, C-H bond oxidation is a hot research area in catalysis. One-dimensional covalent organic frameworks (1D-COFs) developed recently have attracted growing attention for catalytic applications owing to their unique edge microstructure. Herein, a novel crystalline 1D-COF (FZU-66) was constructed and further decorated with cobalt(II), which led to excellent heterogeneous catalytic performance in the C-H bond oxidation of ethylbenzene. In an aqueous solution at room temperature within 16 h, the conversion is nearly 100%, while the acetophenone selectivity is around 99%. More impressively, the designed single-dispersed cobalt(II)-coordinated 1D-COF (FZU-66-Co) retained good catalytic activity while maintaining high crystallinity after at least five consecutive recycling experiments. This work will prompt the application of porous polymers in the catalyzed oxidation of C-H bonds and make it an efficient and sustainable platform for activating C-H bonds of aromatic hydrocarbons.
Keyword ：
1D structure 1D structure C-H-oxidation C-H-oxidation covalent organic framework covalent organic framework ethylbenzene transformation ethylbenzene transformation single-sitecatalyst single-sitecatalyst
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| GB/T 7714 | Lin, Kaifu , Wang, Jiawei , Qiao, Shujie et al. Novel Cobalt(II)-Decorated 1D Covalent Organic Framework for Selective Oxidation of Ethylbenzene [J]. | ACS SUSTAINABLE CHEMISTRY & ENGINEERING , 2024 , 12 (17) : 6719-6727 . |
| MLA | Lin, Kaifu et al. "Novel Cobalt(II)-Decorated 1D Covalent Organic Framework for Selective Oxidation of Ethylbenzene" . | ACS SUSTAINABLE CHEMISTRY & ENGINEERING 12 . 17 (2024) : 6719-6727 . |
| APA | Lin, Kaifu , Wang, Jiawei , Qiao, Shujie , Guo, Zhiyong . Novel Cobalt(II)-Decorated 1D Covalent Organic Framework for Selective Oxidation of Ethylbenzene . | ACS SUSTAINABLE CHEMISTRY & ENGINEERING , 2024 , 12 (17) , 6719-6727 . |
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van der Waals (vdW) superlattices, comprising different 2D materials aligned alternately by weak interlayer interactions, offer versatile structures for the fabrication of novel semiconductor devices. Despite their potential, the precise control of optoelectronic properties with interlayer interactions remains challenging. Here, we investigate the discrepancies between the SnS/TiS2 superlattice (SnTiS3) and its subsystems by comprehensive characterization and DFT calculations. The disappearance of certain Raman modes suggests that the interactions alter the SnS subsystem structure. Specifically, such structural changes transform the band structure from indirect to direct band gap, causing a strong PL emission (similar to 2.18 eV) in SnTiS3. In addition, the modulation of the optoelectronic properties ultimately leads to the unique phenomenon of thermally activated photoluminescence. This phenomenon is attributed to the inhibition of charge transfer induced by tunable intralayer strains. Our findings extend the understanding of the mechanism of interlayer interactions in van der Waals superlattices and provide insights into the design of high-temperature optoelectronic devices.
Keyword ：
interlayer interactions interlayer interactions photoluminescence photoluminescence SnTiS3 SnTiS3 temperature-dependent temperature-dependent van der Waals heterostructures van der Waals heterostructures
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| GB/T 7714 | Huang, Siting , Bai, Jiahui , Long, Hanyan et al. Thermally Activated Photoluminescence Induced by Tunable Interlayer Interactions in Naturally Occurring van der Waals Superlattice SnS/TiS2 [J]. | NANO LETTERS , 2024 , 24 (20) : 6061-6068 . |
| MLA | Huang, Siting et al. "Thermally Activated Photoluminescence Induced by Tunable Interlayer Interactions in Naturally Occurring van der Waals Superlattice SnS/TiS2" . | NANO LETTERS 24 . 20 (2024) : 6061-6068 . |
| APA | Huang, Siting , Bai, Jiahui , Long, Hanyan , Yang, Shichao , Chen, Wenwei , Wang, Qiuyan et al. Thermally Activated Photoluminescence Induced by Tunable Interlayer Interactions in Naturally Occurring van der Waals Superlattice SnS/TiS2 . | NANO LETTERS , 2024 , 24 (20) , 6061-6068 . |
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2D transition metal dichalcogenides (TMDs) have emerged as a novel class of semiconductors with promising applications in optoelectronics, owing to their rich and tunable valley fine structure, known as valleytronics. Strain engineering in TMDs presents opportunities to tailor their valley fine structures and band alignment, which greatly expands the potential to investigate their intrinsic properties and improve device performance, thus opening a new field of straintronics. In this review, recent advances in strain-engineered 2D TMDs are summarized, with a focus on new phenomena and applications enabled by precision tuning of valley physics. The underlying mechanisms and connections are delineated between strain-induced modifications to the valley fine structures based on intravalley, intervalley, and interlayer band alignment in single and heterostructure TMDs. These insights allow targeted strain control strategies to be devised for optimizing optoelectronic characteristics. This review provides perspectives and guidance on the future directions of valley-straintronics and flexible 2D optoelectronics using TMDs, highlighting the substantial promise of valley-strain engineering in TMDs for fundamental valley physics studies as well as practical device applications. Presenting a comprehensive review on recent advancements in strain-engineered 2D transition metal dichalcogenides (TMDs). This review delves into precision tuning of valley physics through strain engineering, elucidating mechanisms and connections between strain-induced modifications and optoelectronic characteristics. It offers insights into future directions of valley-straintronics, underscoring the significant promise of valley-strain engineering in TMDs for fundamental studies and practical applications. image
Keyword ：
2D semiconductors 2D semiconductors straintronics straintronics transition metal dichalcogenides transition metal dichalcogenides valley fine structure valley fine structure valleytronics valleytronics
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| GB/T 7714 | Yang, Shichao , Long, Hanyan , Chen, Wenwei et al. Valleytronics Meets Straintronics: Valley Fine Structure Engineering of 2D Transition Metal Dichalcogenides [J]. | ADVANCED OPTICAL MATERIALS , 2024 , 12 (14) . |
| MLA | Yang, Shichao et al. "Valleytronics Meets Straintronics: Valley Fine Structure Engineering of 2D Transition Metal Dichalcogenides" . | ADVANCED OPTICAL MATERIALS 12 . 14 (2024) . |
| APA | Yang, Shichao , Long, Hanyan , Chen, Wenwei , Sa, Baisheng , Guo, Zhiyong , Zheng, Jingying et al. Valleytronics Meets Straintronics: Valley Fine Structure Engineering of 2D Transition Metal Dichalcogenides . | ADVANCED OPTICAL MATERIALS , 2024 , 12 (14) . |
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Covalent organic framework (COF)-based membranes are burgeoning candidates for separation technologies owing to their well-ordered channel structures. However, it is still a significant challenge to obtain high-quality COF membranes with a mild and convenient preparation strategy. In this paper, we adopted a simple liquidliquid interfacial polymerization method to manufacture a self-standing COF membrane with decent crystallinity at room temperature. Aldehyde monomer and catalyst were dissolved in water as the bottom layer and the amine monomer was dissolved in ethyl acetate as the top layer, and new COF membranes were subsequently obtained by interfacial polymerization in the two-phase interface. The synthetic conditions including precursor and catalyst dosage were further optimized, and thus-synthesized PDA-TAPB-ABC membrane displayed a stable rejection to MB of 97.57% with a high water permeance of up to 101. 32 L m-(2)h(-1)bar(-1). Its dyes separation performance was much better than their AA-stacking counterpart. Moreover, the prepared membrane endowed favorable chemical stability and long-term durability.
Keyword ：
ABC-Stacking ABC-Stacking Covalent organic frameworks Covalent organic frameworks Dye separation Dye separation Rejection Rejection Self-standing membrane Self-standing membrane
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| GB/T 7714 | Wang, Jiande , Wang, Jun , Qiao, Shujie et al. Interfacial polymerization of self-standing ABC-stacking Covalent organic framework membranes for dye separation [J]. | POLYMER , 2024 , 300 . |
| MLA | Wang, Jiande et al. "Interfacial polymerization of self-standing ABC-stacking Covalent organic framework membranes for dye separation" . | POLYMER 300 (2024) . |
| APA | Wang, Jiande , Wang, Jun , Qiao, Shujie , Li, Nanwen , Guo, Zhiyong . Interfacial polymerization of self-standing ABC-stacking Covalent organic framework membranes for dye separation . | POLYMER , 2024 , 300 . |
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Vinylene-linked COFs, as an emerging class of crystalline porous polymers, have been regarded as ideal heterogenous photocatalysts due to their ordered structure, tailored pore size, outstanding stability and fully pi-conjugated structure. Unfortunately, their photocatalytic performances are usually impeded by high exciton binding energy and unsatisfactory exciton dissociation efficiency. Herein, the authors broke through this dilemma by arrangement of complementary donor-acceptor (D-A) pairs within the COF skeleton to improve charge transfer/separation. Two vinylene-linked COFs (TMT-BT-COF and TMT-TT-COF) are synthesized by Aldol condensation using highly photoactive thienothiophene and benzothiazole groups as donor and electron-deficient triazine units as acceptor. Photochemical/electrochemical studies as well as DFT calculation suggest that these D-A type vinylene-linked COFs endow high charge transfer efficiency and low charge recombination. As a result, both of them demonstrate remarkably catalytic activity in the oxidation of styrene to benzaldehyde with molecular oxygen, with an exceptionally high conversion rate (>= 92%) and selectivity (>= 90%). Intriguingly, in the presence of NaHCO3, the above COFs could photocatalyze epoxidation styrene in water, and the styrene oxide selectivity reached 53%. This work elucidates the prominent capability of vinylene-linked COFs in the photocatalytic transformation of organic compounds in aqueous media, which may pave a new avenue for their future development.
Keyword ：
covalent organic frameworks covalent organic frameworks donor-acceptor (D-A) donor-acceptor (D-A) photocatalytic photocatalytic selective oxidation of styrene selective oxidation of styrene vinylene-linked vinylene-linked
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| GB/T 7714 | Wang, Jun , Qiao, Shujie , Yang, Mingshuan et al. Vinylene-Linked Covalent Organic Frameworks for Visible-Light-Promoted Selective Oxidation of Styrene in Water [J]. | SMALL , 2024 . |
| MLA | Wang, Jun et al. "Vinylene-Linked Covalent Organic Frameworks for Visible-Light-Promoted Selective Oxidation of Styrene in Water" . | SMALL (2024) . |
| APA | Wang, Jun , Qiao, Shujie , Yang, Mingshuan , Guo, Zhiyong . Vinylene-Linked Covalent Organic Frameworks for Visible-Light-Promoted Selective Oxidation of Styrene in Water . | SMALL , 2024 . |
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Sulfur functionalized biocarbons were prepared from naturally abundant lignin alkali with sodium thiocyanate as an activation agent and a sulfur source. The resultant biocarbon sorbents showed a high mercury isolation ability from aqueous solutions, where high surface area and doping of sulfur significantly aid the uptake of mercury, i.e., 0.05 g of biocarbon sorbent removed 99% of mercury from 250 mL of simulated wastewater with an initial concentration of mercury of 10 mg L-1. Sulfur functionalized biocarbons were prepared from naturally abundant lignin alkali with sodium thiocyanate as an activation agent and a sulfur source.
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| GB/T 7714 | Austin, Douglas , Jahan, Kousar , Feng, Xu et al. Sulfur functionalized biocarbon sorbents for low-concentration mercury isolation [J]. | DALTON TRANSACTIONS , 2023 , 53 (5) : 2098-2107 . |
| MLA | Austin, Douglas et al. "Sulfur functionalized biocarbon sorbents for low-concentration mercury isolation" . | DALTON TRANSACTIONS 53 . 5 (2023) : 2098-2107 . |
| APA | Austin, Douglas , Jahan, Kousar , Feng, Xu , Carney, Jared , Hensley, Dale K. , Chen, Jihua et al. Sulfur functionalized biocarbon sorbents for low-concentration mercury isolation . | DALTON TRANSACTIONS , 2023 , 53 (5) , 2098-2107 . |
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Fine-tuning of the physical stacking structure for microporous polyimide (PI) membranes via the stretching processing is a practical way of achieving advanced membrane materials with improved aging resistance as well as high gas separation performance. Here, a fluorinated polyimide 6FDA:BPDA-TFDB(1:1:2) is used as a prototype and a series of stretched membranes X%-PI are fabricated by uniaxially stretching the membrane to different elongation ratio and then annealing. Based on birefringence and wide-angle X-ray diffraction measurements, it's found that regular orientation of polymer chains along the stretching direction and fine-tuning of d-spaces from interchain packing and pi-pi stacking happen during the uniaxial stretching process. As such, compared to pristine PI membrane, the stretched membranes show better mechanical and thermal stability, especially for the one with higher stretching ratio. In addition, owing to the increased packing density of polymer chains, the highly stretched membrane of 40%-PI shows significantly improved gas perm-selectivity by 32.8%, 24.3%, and 12.6% for He/CH4, H2/CH4, and CO2/CH4 gas pairs, respectively, in comparison to pristine membrane. Furthermore, 40%-PI exhibits much higher gas permeability retention rate than that of other membranes after three months' aging. We expect that this work can offer polymer materials processing guidance for the preparation of high-performance gas separation membrane in future.
Keyword ：
Aging resistance Aging resistance Gas separation Gas separation Polyimide membrane Polyimide membrane Stretch-induced orientation Stretch-induced orientation
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| GB/T 7714 | Huo, Guolong , Guo, Zhiyong , Zhang, Zhiguang et al. Effect of uniaxial stretching on gas separation performance of polyimide membranes [J]. | JOURNAL OF MEMBRANE SCIENCE , 2023 , 687 . |
| MLA | Huo, Guolong et al. "Effect of uniaxial stretching on gas separation performance of polyimide membranes" . | JOURNAL OF MEMBRANE SCIENCE 687 (2023) . |
| APA | Huo, Guolong , Guo, Zhiyong , Zhang, Zhiguang , Zhou, Xiaowei , Xin, Junhao , Zhang, Yuchen et al. Effect of uniaxial stretching on gas separation performance of polyimide membranes . | JOURNAL OF MEMBRANE SCIENCE , 2023 , 687 . |
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