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Article: Platinum(II) Non-Covalent Crosslinkers for Supramolecular DNA Hydrogels
Title | Platinum(II) Non-Covalent Crosslinkers for Supramolecular DNA Hydrogels |
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Authors | |
Keywords | Crosslinking DNA Hydrogels Ligands Luminescence |
Issue Date | 2020 |
Publisher | Royal Society of Chemistry: Open Access. The Journal's web site is located at http://www.rsc.org/publishing/journals/sc/About.asp |
Citation | Chemical Science, 2020, v. 11 n. 12, p. 3241-3249 How to Cite? |
Abstract | Manipulation of non-covalent metal–metal interactions allows the fabrication of functional metallosupramolecular structures with diverse supramolecular behaviors. The majority of reported studies are mostly designed and governed by thermodynamics, with very few examples of metallosupramolecular systems exhibiting intriguing kinetics. Here we report a serendipitous finding of platinum(II) complexes serving as non-covalent crosslinkers for the fabrication of supramolecular DNA hydrogels. Upon mixing the alkynylplatinum(II) terpyridine complex with double-stranded DNA in aqueous solution, the platinum(II) complex molecules are found to first stack into columnar phases by metal–metal and π–π interactions, and then the columnar phases that carry multiple positive charges crosslink the negatively charged DNA strands to form supramolecular hydrogels with luminescence properties and excellent processability. Subsequent platinum(II) intercalation into DNA competes with the metal–metal and π–π interactions at the crosslinking points, switching on the spontaneous gel-to-sol transition. In the case of a chloro (2,6-bis(benzimidazol-2′-yl)pyridine)platinum(II) complex, with [Pt(bzimpy)Cl]+ serving as a non-covalent crosslinker where the metal–metal and π–π interactions outcompete platinum(II) intercalation, the intercalation-driven gel-to-sol transition pathway is blocked since the gel state is energetically more favorable than the sol state. Interestingly, the ligand exchange reaction of the chloro ligand in [Pt(bzimpy)Cl]+ with glutathione (GSH) has endowed the complexes with enhanced hydrophilicity, decreasing the planarity of the complexes, and turning off the metal–metal and π–π interactions at the crosslinking points, leading to GSH-triggered hydrogel dissociation. |
Persistent Identifier | http://hdl.handle.net/10722/286152 |
ISSN | 2023 Impact Factor: 7.6 2023 SCImago Journal Rankings: 2.333 |
ISI Accession Number ID |
DC Field | Value | Language |
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dc.contributor.author | Zhang, K | - |
dc.contributor.author | Yam, VWW | - |
dc.date.accessioned | 2020-08-31T06:59:52Z | - |
dc.date.available | 2020-08-31T06:59:52Z | - |
dc.date.issued | 2020 | - |
dc.identifier.citation | Chemical Science, 2020, v. 11 n. 12, p. 3241-3249 | - |
dc.identifier.issn | 2041-6520 | - |
dc.identifier.uri | http://hdl.handle.net/10722/286152 | - |
dc.description.abstract | Manipulation of non-covalent metal–metal interactions allows the fabrication of functional metallosupramolecular structures with diverse supramolecular behaviors. The majority of reported studies are mostly designed and governed by thermodynamics, with very few examples of metallosupramolecular systems exhibiting intriguing kinetics. Here we report a serendipitous finding of platinum(II) complexes serving as non-covalent crosslinkers for the fabrication of supramolecular DNA hydrogels. Upon mixing the alkynylplatinum(II) terpyridine complex with double-stranded DNA in aqueous solution, the platinum(II) complex molecules are found to first stack into columnar phases by metal–metal and π–π interactions, and then the columnar phases that carry multiple positive charges crosslink the negatively charged DNA strands to form supramolecular hydrogels with luminescence properties and excellent processability. Subsequent platinum(II) intercalation into DNA competes with the metal–metal and π–π interactions at the crosslinking points, switching on the spontaneous gel-to-sol transition. In the case of a chloro (2,6-bis(benzimidazol-2′-yl)pyridine)platinum(II) complex, with [Pt(bzimpy)Cl]+ serving as a non-covalent crosslinker where the metal–metal and π–π interactions outcompete platinum(II) intercalation, the intercalation-driven gel-to-sol transition pathway is blocked since the gel state is energetically more favorable than the sol state. Interestingly, the ligand exchange reaction of the chloro ligand in [Pt(bzimpy)Cl]+ with glutathione (GSH) has endowed the complexes with enhanced hydrophilicity, decreasing the planarity of the complexes, and turning off the metal–metal and π–π interactions at the crosslinking points, leading to GSH-triggered hydrogel dissociation. | - |
dc.language | eng | - |
dc.publisher | Royal Society of Chemistry: Open Access. The Journal's web site is located at http://www.rsc.org/publishing/journals/sc/About.asp | - |
dc.relation.ispartof | Chemical Science | - |
dc.rights | This work is licensed under a Creative Commons Attribution-NonCommercial-NoDerivatives 4.0 International License. | - |
dc.subject | Crosslinking | - |
dc.subject | DNA | - |
dc.subject | Hydrogels | - |
dc.subject | Ligands | - |
dc.subject | Luminescence | - |
dc.title | Platinum(II) Non-Covalent Crosslinkers for Supramolecular DNA Hydrogels | - |
dc.type | Article | - |
dc.identifier.email | Yam, VWW: wwyam@hku.hk | - |
dc.identifier.authority | Yam, VWW=rp00822 | - |
dc.description.nature | published_or_final_version | - |
dc.identifier.doi | 10.1039/C9SC05910E | - |
dc.identifier.scopus | eid_2-s2.0-85082714259 | - |
dc.identifier.hkuros | 313075 | - |
dc.identifier.volume | 11 | - |
dc.identifier.issue | 12 | - |
dc.identifier.spage | 3241 | - |
dc.identifier.epage | 3249 | - |
dc.identifier.isi | WOS:000528663000012 | - |
dc.publisher.place | United Kingdom | - |
dc.identifier.issnl | 2041-6520 | - |