Abstract
Supramolecular DNA hydrogels have been synthesized based on the assembly of DNA building-blocks such as branched DNA and long DNA chains. The structures and functions of sole-module DNA hydrogels remain limitations. New methodologies by integrating hybrid components are desired to expand the synthesis of DNA hydrogel. Herein, we synthesized a Ln3+-containing luminescent supramolecular hydrogel by employing the coordination and electrostatic interactions between lanthanide ions (Tb3+ and Eu3+) and linear single-stranded DNA (ssDNA). Through the coordination between ssDNA and Ln3+, a series of luminescent supramolecular hydrogels were synthesized, among which the Tb-Gn/Tn and Eu-Tn hydrogels emitted the characteristic luminescence of Tb and Eu, respectively. The luminescent intensities of the hydrogels were adjusted by designing DNA sequences with programmable bases and chain lengths. Notably, the Tb/Eu co-doped luminescent supramolecular hydrogel displayed tunable luminescence from green to yellow by regulating the stoichiometric ratio of Tb/Eu. Moreover, the hydrogel had reversible luminescent stimulation responsiveness toward Ag+/L-Cys. We expected that the synthesis of Ln3+-containing luminescent supramolecular hydrogels enriched the strategies of the construction of DNA hydrogels, and promoted the development of stimuli-responsive supramolecular materials.
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Jastrząb R, Nowak M, Skrobańska M, et al. DNA as a target for lanthanide(iii) complexes influence. Coord Chem Rev, 2019, 382: 145–159
Li F, Tang J, Geng J, et al. Polymeric DNA hydrogel: Design, synthesis and applications. Prog Polym Sci, 2019, 98: 101163–101188
Li F, Lyu D, Liu S, et al. DNA hydrogels and microgels for biosensing and biomedical applications. Adv Mater, 2020, 32: 1806538–1806547
Wang Y, Shao Y, Ma X, et al. Constructing tissuelike complex structures using cell-laden DNA hydrogel bricks. ACS Appl Mater Interfaces, 2017, 9: 12311–12315
Gao T, Chen T, Feng C, et al. Design and fabrication of flexible DNA polymer cocoons to encapsulate live cells. Nat Commun, 2019, 10: 2946–2956
Zhao Z, Wang C, Yan H, et al. Soft robotics programmed with double crosslinking DNA hydrogels. Adv Funct Mater, 2019, 29: 1905911–1905921
Dong Y, Yao C, Zhu Y, et al. DNA functional materials assembled from branched DNA: Design, synthesis, and applications. Chem Rev, 2020, 120: 9420–9481
Zhou W, Saran R, Liu J. Metal sensing by DNA. Chem Rev, 2017, 117: 8272–8325
Xue S F, Chen Z H, Han X Y, et al. DNA encountering terbium(III): A smart “chemical nose/tongue” for large-scale time-gated luminescent and lifetime-based sensing. Anal Chem, 2018, 90: 3443–3451
Mehwish N, Dou X, Zhao C, et al. Chirality transfer in supramolecular co-assembled fibrous material enabling the visual recognition of sucrose. Adv Fiber Mater, 2020, 2: 204–211
Yang S, Macharia D K, Ahmed S, et al. Flexible and reusable non-woven fabric photodetector based on polypyrrole/crystal violate lactone for NIR light detection and writing. Adv Fiber Mater, 2020, 2: 150–160
Zhu M, Wang W, Zhang C, et al. Photo-responsive behaviors of hydrogen-bonded polymer complex fibers containing azobenzene functional groups. Adv Fiber Mater, 2021, 3: 172–179
Eliseeva S V, Bünzli J C G. Lanthanide luminescence for functional materials and bio-sciences. Chem Soc Rev, 2010, 39: 189–227
He Y, Lopez A, Zhang Z, et al. Nucleotide and DNA coordinated lanthanides: From fundamentals to applications. Coord Chem Rev, 2019, 387: 235–248
Ma Q, Zhang M, Xu X, et al. Multiresponsive supramolecular luminescent hydrogels based on a nucleoside/lanthanide complex. ACS Appl Mater Interfaces, 2019, 11: 47404–47412
Ma Q, Zhang M, Yao C, et al. Supramolecular hydrogel with luminescence tunablility and responsiveness based on co-doped lanthanide and deoxyguanosine complex. Chem Eng J, 2020, 394: 124894–124903
Xu L, Zhang P, Liu Y, et al. Continuously tunable nucleotide/lanthanide coordination nanoparticles for DNA adsorption and sensing. ACS Omega, 2018, 3: 9043–9051
Zhang M, Le H N, Jiang X Q, et al. Time-resolved probes based on guanine/thymine-rich DNA-sensitized luminescence of terbium(iii). Anal Chem, 2013, 85: 11665–11674
Zhang M, Xue J, Zhu Y, et al. Multiresponsive white-light emitting aerogel prepared with codoped lanthanide/thymidine/carbon dots. ACS Appl Mater Interfaces, 2020, 12: 22191–22199
Hu Y, Guo W, Ding Y, et al. Modulating luminescence of Tb3+ with biomolecules for sensing heparin and its contaminant OSCS. Biosens Bioelectron, 2016, 86: 858–863
Navarro J A R, Lippert B. Molecular architecture with metal ions, nucleobases and other heterocycles. Coord Chem Rev, 1999, 185–186: 653–667
Chen J, Hickey B L, Wang L, et al. Selective discrimination and classification of G-quadruplex structures with a host-guest sensing array. Nat Chem, 2021, 13: 488–495
Wang Y, Suzuki H, Xie J, et al. Mimicking natural photosynthesis: Solar to renewable H2 fuel synthesis by Z-scheme water splitting systems. Chem Rev, 2018, 118: 5201–5241
Yao C, Wang W, Wang P, et al. Near-infrared upconversion mesoporous cerium oxide hollow biophotocatalyst for concurrent pH-/H2O2-responsive O2-evolving synergetic cancer therapy. Adv Mater, 2018, 30: 1704833–1704841
Zhou X, Mandal S, Jiang S, et al. Efficient long-range, directional energy transfer through DNA-templated dye aggregates. J Am Chem Soc, 2019, 141: 8473–8481
Li K, Shang M, Lian H, et al. Recent development in phosphors with different emitting colors via energy transfer. J Mater Chem C, 2016, 4: 5507–5530
Mara M W, Tatum D S, March A M, et al. Energy transfer from antenna ligand to europium(iii) followed using ultrafast optical and X-ray spectroscopy. J Am Chem Soc, 2019, 141: 11071–11081
Wu L, Chen G, Li Z. Layered rare-earth hydroxide/polyacrylamide nanocomposite hydrogels with highly tunable photoluminescence. Small, 2017, 13: 1604070–1604077
Wu L, Gao C, Li Z, et al. Tunable photoluminescence from layered rare-earth hydroxide/polymer nanocomposite hydrogels by a cascaded energy transfer effect. J Mater Chem C, 2017, 5: 5207–5213
Chen P, Li Q, Grindy S, et al. White-light-emitting lanthanide metallogels with tunable luminescence and reversible stimuli-responsive properties. J Am Chem Soc, 2015, 137: 11590–11593
SeethaLekshmi S, Ramya A R, Reddy M L P, et al. Lanthanide complex-derived white-light emitting solids: A survey on design strategies. J Photochem Photobiol C, 2017, 33: 109–131
Li J, Li W, Xia D, et al. Dynamic coordination of natural amino acidslanthanides to control reversible luminescent switching of hybrid hydrogels and anti-counterfeiting. Dyes Pigments, 2019, 166: 375–380
Sebastian A, Mahato M K, Prasad E. A mixed ligand approach towards lanthanide-based gels using citric acid as assembler ligand: White light emission and environmental sensing. Soft Matter, 2019, 15: 3407–3417
Weng G, Thanneeru S, He J. Dynamic coordination of Eu-iminodiacetate to control fluorochromic response of polymer hydrogels to multistimuli. Adv Mater, 2018, 30: 1706526–1706533
Zhang Z, Liu F, Xu Q, et al. Covalent grafting terbium complex to alginate hydrogels and their application in Fe3+ and pH sensing. Glob Chall, 2019, 3: 1800067–1800073
Chen Z H, Han X Y, Deng L X, et al. A self-calibrating logic system and oxidase-based biosensor using Tb3+-doped carbon dots/DNA conjugates. Talanta, 2019, 191: 235–240
Zhang M, Le H N, Wang P, et al. A versatile molecular beacon-like probe for multiplexed detection based on fluorescence polarization and its application for a resettable logic gate. Chem Commun, 2012, 48: 10004–10006
Wang X, Yao X, Huang Q, et al. Triple-wavelength-region luminescence sensing based on a color-tunable emitting lanthanide metal organic framework. Anal Chem, 2018, 90: 6675–6682
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This work was supported in part by Tianjin Natural Science Foundation (Basic Research Plan, Grant Nos. 18JCJQJC47600 and 19JCQNJC02200).
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Yang, S., Pan, X., Tang, J. et al. Lanthanide-DNA supramolecular hydrogels with tunable and responsive luminescence. Sci. China Technol. Sci. 65, 1043–1051 (2022). https://doi.org/10.1007/s11431-021-1975-9
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DOI: https://doi.org/10.1007/s11431-021-1975-9