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33 results on '"Xu, Hai-Sen"'

6. Multipocket Cage Enables the Binding of High-Order Bulky and Drug Guests Uncovered by MS Methodology

Author

Huang, Yin-Hui, Lu, Yu-Lin, Cao, Zhong-Min, Zhang, Xiao-Dong, Liu, Chen-Hui, Xu, Hai-Sen, and Su, Cheng-Yong

Abstract

Achieving high guest loading and multiguest-binding capacity holds crucial significance for advancement in separation, catalysis, and drug delivery with synthetic receptors; however, it remains a challenging bottleneck in characterization of high-stoichiometry guest-binding events. Herein, we describe a large-sized coordination cage (MOC-70-Zn8Pd6) possessing 12 peripheral pockets capable of accommodating multiple guests and a high-resolution electrospray ionization mass spectrometry (HR-ESI–MS)-based method to understand the solution host–guest chemistry. A diverse range of bulky guests, varying from drug molecules to rigid fullerenes as well as flexible host molecules of crown ethers and calixarenes, could be loaded into open pockets with high capacities. Notably, these hollow cage pockets provide multisites to capture different guests, showing heteroguest coloading behavior to capture binary, ternary, or even quaternary guests. Moreover, a pair of commercially applied drugs for the combination therapy of chronic lymphocytic leukemia (CLL) has been tested, highlighting its potential in multidrug delivery for combined treatment.

Published
2024
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14. Dynamic Stereochemistry of M8Pd6 Supramolecular Cages Based on Metal‐Center Lability for Differential Chiral Induction, Resolution, and Recognition.

Author

Huang, Yin‐Hui, Lu, Yu‐Lin, Zhang, Xiao‐Dong, Liu, Chen‐Hui, Ruan, Jia, Qin, Yu‐Han, Cao, Zhong‐Min, Jiang, Jijun, Xu, Hai‐Sen, and Su, Cheng‐Yong

Subjects
STEREOCHEMISTRY, CHIRALITY, ENANTIOMERS, HOST-guest chemistry, ASYMMETRIC synthesis, CHIRAL recognition, ANIONS
Abstract

A series of isostructural supramolecular cages with a rhombic dodecahedron shape have been assembled with distinct metal‐coordination lability (M8Pd6‐MOC‐16, M=Ru2+, Fe2+, Ni2+, Zn2+). The chirality transfer between metal centers generally imposes homochirality on individual cages to enable solvent‐dependent spontaneous resolution of Δ8/Λ8−M8Pd6 enantiomers; however, their distinguishable stereochemical dynamics manifests differential chiral phenomena governed by the cage stability following the order Ru8Pd6>Ni8Pd6>Fe8Pd6>Zn8Pd6. The highly labile Zn centers endow the Zn8Pd6 cage with conformational flexibility and deformation, enabling intrigue chiral‐Δ8/Λ8−Zn8Pd6 to meso‐Δ4Λ4−Zn8Pd6 transition induced by anions. The cage stabilization effect differs from inert Ru2+, metastable Fe2+/Ni2+, and labile Zn2+, resulting in different chiral‐guest induction. Strikingly, solvent‐mediated host–guest interactions have been revealed for Δ8/Λ8−(Ru/Ni/Fe)8Pd6 cages to discriminate the chiral recognition of the guests with opposite chirality. These results demonstrate a versatile procedure to control the stereochemistry of metal‐organic cages based on the dynamic metal centers, thus providing guidance to maneuver cage chirality at a supramolecular level by virtue of the solvent, anion, and guest to benefit practical applications. [ABSTRACT FROM AUTHOR]

Published
2024
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17. Divergent Chemistry Paths for 3D and 1D Metallo‐Covalent Organic Frameworks (COFs)

Author

Xu, Hai‐Sen, primary, Luo, Yi, additional, See, Pei Zhen, additional, Li, Xing, additional, Chen, Zhongxin, additional, Zhou, Yi, additional, Zhao, Xiaoxu, additional, Leng, Kai, additional, Park, In‐Hyeok, additional, Li, Runlai, additional, Liu, Cuibo, additional, Chen, Fangzheng, additional, Xi, Shibo, additional, Sun, Junliang, additional, and Loh, Kian Ping, additional

Published
2020
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19. Divergent Chemistry Paths for 3D and 1D Metallo-Covalent Organic Frameworks (COFs)

Author

Xu, Hai-Sen, Luo, Yi, See, Pei Zhen, Li, Xing, Chen, Zhongxin, Zhou, Yi, Zhao, Xiaoxu, Leng, Kai, Park, In-Hyeok, Li, Runlai, Liu, Cuibo, Chen, Fangzheng, Xi, Shibo, Sun, Junliang, Loh, Kian Ping, Xu, Hai-Sen, Luo, Yi, See, Pei Zhen, Li, Xing, Chen, Zhongxin, Zhou, Yi, Zhao, Xiaoxu, Leng, Kai, Park, In-Hyeok, Li, Runlai, Liu, Cuibo, Chen, Fangzheng, Xi, Shibo, Sun, Junliang, and Loh, Kian Ping

Abstract

The marriage of dynamic covalent chemistry (DCC) and coordination chemistry is a powerful tool for assembling complex architectures from simple building units. Recently, the synthesis of woven covalent organic frameworks (COFs) with topologically fascinating structures has been achieved using this approach. However, the scope is highly limited and there is a need to discover new pathways that can assemble covalently linked organic threads into crystalline frameworks. Herein, we have identified branching pathways leading to the assembly of three-dimensional (3D) woven COFs or one-dimensional (1D) metallo-COFs (mCOFs), where the mechanism is underpinned by the absence or presence of ligand exchange.

Published
2020
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22. Tuneable near white-emissive two-dimensional covalent organic frameworks

Author

Li, Xing, primary, Gao, Qiang, additional, Wang, Juefan, additional, Chen, Yifeng, additional, Chen, Zhi-Hui, additional, Xu, Hai-Sen, additional, Tang, Wei, additional, Leng, Kai, additional, Ning, Guo-Hong, additional, Wu, Jishan, additional, Xu, Qing-Hua, additional, Quek, Su Ying, additional, Lu, Yixin, additional, and Loh, Kian Ping, additional

Published
2018
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23. Exploring Applications of Covalent Organic Frameworks: Homogeneous Reticulation of Radicals for Dynamic Nuclear Polarization

Author

Cao, Wei, primary, Wang, Wei David, additional, Xu, Hai-Sen, additional, Sergeyev, Ivan V., additional, Struppe, Jochem, additional, Wang, Xiaoling, additional, Mentink-Vigier, Frederic, additional, Gan, Zhehong, additional, Xiao, Ming-Xing, additional, Wang, Lu-Yao, additional, Chen, Guo-Peng, additional, Ding, San-Yuan, additional, Bai, Shi, additional, and Wang, Wei, additional

Published
2018
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27. Stereochemical Control of Redox CoII/CoIII-Cages with Switchable Cotton Effects Based on Labile-Static States

Author

Lu, Yu-Lin, Wu, Kai, Huang, Yin-Hui, Li, Wei-Chun, Cao, Zhong-Min, Yan, Xiang-Han, Zhang, Xiao-Dong, Liu, Chen-Hui, Ruan, Jia, Xu, Hai-Sen, Pan, Mei, and Su, Cheng-Yong

Abstract

The structural dynamics of artificial assemblies, in aspects such as molecular recognition and structural transformation, provide us with a blueprint to achieve bioinspired applications. Here, we describe the assembly of redox-switchable chiral metal–organic cages Λ8/Δ8-[Pd6(CoIIL3)8]28+and Λ8/Δ8-[Pd6(CoIIIL3)8]36+. These isomeric cages demonstrate an on–off chirality logic gate controlled by their chemical and stereostructural dynamics tunable through redox transitions between the labile CoII-state and static CoIII-state with a distinct Cotton effect. The transition between different states is enabled by a reversible redox process and chiral recognition originating in the tris-chelate Co-centers. All cages in two states are thoroughly characterized by NMR, ESI-MS, CV, CD, and X-ray crystallographic analysis, which clarify their redox-switching behaviors upon chemical reduction/oxidation. The stereochemical lability of the CoII-center endows the Λ8/Δ8-CoII-cages with efficient chiral-induction by enantiomeric guests, leading to enantiomeric isomerization to switch between Λ8/Δ8-CoII-cages, which can be stabilized by oxidation to their chemically inert forms of Λ8/Δ8-CoIII-cages. Kinetic studies reveal that the isomerization rate of the Δ8-CoIII-cage is at least an order of magnitude slower than that of the Δ8-CoII-cage even at an elevated temperature, while its activation energy is 16 kcal mol–1higher than that of the CoII-cage.

Published
2024
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32. Single crystal of a one-dimensional metallo-covalent organic framework

Author

Hai-Sen Xu, Junliang Sun, Xiangyan Shi, Zhongxin Chen, Pei Zhen See, Tianqiong Ma, Yi Luo, Kai Leng, Yi Zhou, Kian Ping Loh, Xiaoxu Zhao, Lin Liang, Xiu Fang Lu, Runlai Li, Xing Li, Cuibo Liu, Lin Wang, Ibrahim Abdelwahab, Xu, Hai-Sen [0000-0003-4137-9005], Luo, Yi [0000-0002-6468-2990], Li, Xing [0000-0002-5470-1043], Leng, Kai [0000-0003-3408-5033], Abdelwahab, Ibrahim [0000-0002-0107-5827], Wang, Lin [0000-0003-3430-7345], Sun, Junliang [0000-0003-4074-0962], Loh, Kian Ping [0000-0002-1491-743X], and Apollo - University of Cambridge Repository

Subjects
Materials science, Science, Crystal engineering, General Physics and Astronomy, 010402 general chemistry, 01 natural sciences, Article, General Biochemistry, Genetics and Molecular Biology, Crystal, Metal, lcsh:Science, Molecular self-assembly, chemistry.chemical_classification, 3403 Macromolecular and Materials Chemistry, Multidisciplinary, 34 Chemical Sciences, 010405 organic chemistry, Dynamic covalent chemistry, General Chemistry, Polymer, 0104 chemical sciences, 3402 Inorganic Chemistry, Crystallography, chemistry, Electron diffraction, Covalent bond, visual_art, visual_art.visual_art_medium, Materials chemistry, lcsh:Q, Polymer synthesis, Single crystal, Covalent organic framework
Abstract

Although polymers have been studied for well over a century, there are few examples of covalently linked polymer crystals synthesised directly from solution. One-dimensional (1D) covalent polymers that are packed into a framework structure can be viewed as a 1D covalent organic framework (COF), but making a single crystal of this has been elusive. Herein, by combining labile metal coordination and dynamic covalent chemistry, we discover a strategy to synthesise single-crystal metallo-COFs under solvothermal conditions. The single-crystal structure is rigorously solved using single-crystal electron diffraction technique. The non-centrosymmetric metallo-COF allows second harmonic generation. Due to the presence of syntactic pendant amine groups along the polymer chains, the metallopolymer crystal can be further cross-linked into a crystalline woven network., Although polymers have been studied for well over a century, there are few examples of covalently linked polymer crystals synthesized directly from solution. Here, the authors demonstrate a strategy to synthesize single crystalline 1D metallo-covalent organic frameworks by combining dynamic covalent chemistry and metal-ligand coordination.

Published
2020
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33. Stereochemical Control of Redox Co II /Co III -Cages with Switchable Cotton Effects Based on Labile-Static States.

Author

Lu YL, Wu K, Huang YH, Li WC, Cao ZM, Yan XH, Zhang XD, Liu CH, Ruan J, Xu HS, Pan M, and Su CY

Abstract

The structural dynamics of artificial assemblies, in aspects such as molecular recognition and structural transformation, provide us with a blueprint to achieve bioinspired applications. Here, we describe the assembly of redox-switchable chiral metal-organic cages Λ 8 /Δ 8 -[Pd 6 (Co II L 3 ) 8 ] 28+ and Λ 8 /Δ 8 -[Pd 6 (Co III L 3 ) 8 ] 36+ . These isomeric cages demonstrate an on-off chirality logic gate controlled by their chemical and stereostructural dynamics tunable through redox transitions between the labile Co II -state and static Co III -state with a distinct Cotton effect. The transition between different states is enabled by a reversible redox process and chiral recognition originating in the tris-chelate Co-centers. All cages in two states are thoroughly characterized by NMR, ESI-MS, CV, CD, and X-ray crystallographic analysis, which clarify their redox-switching behaviors upon chemical reduction/oxidation. The stereochemical lability of the Co II -center endows the Λ 8 /Δ 8 -Co II -cages with efficient chiral-induction by enantiomeric guests, leading to enantiomeric isomerization to switch between Λ 8 /Δ 8 -Co II -cages, which can be stabilized by oxidation to their chemically inert forms of Λ 8 /Δ 8 -Co III -cages. Kinetic studies reveal that the isomerization rate of the Δ 8 -Co III -cage is at least an order of magnitude slower than that of the Δ 8 -Co II -cage even at an elevated temperature, while its activation energy is 16 kcal mol -1 higher than that of the Co II -cage.

Published
2024
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