Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 60, Issue 18, Pages 10089-10094Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202015554
Keywords
bioinorganic chemistry; DNA; metal-mediated base pair; palladium; self-assembly
Categories
Funding
- Spanish MINECO [CTQ2017-89311-P]
- Spanish MICIU (Salvador Madariaga Program) [PRX19/00290]
- University of Granada [A-FQM-465-UGR18]
- Junta de Andalucia [FQM-293, FQM-283]
- COST Action [CA-18202]
- Grup de Recerca de la Generalitat de Catalunya [2017SGR-864]
- FEDER [BIO2015-67358-C2-2-P]
- U.S. Department of Energy, Office of Basic Energy Sciences, Division of Material Sciences and Engineering [DE SC0010802]
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The study demonstrates that 1Pd-DNA molecules with a continuous single chain of Pd-II ions can be prepared by a simple self-assembly reaction between complex [Pd(Cheld)(CH3CN)] (1Pd_CH3CN) and single-stranded DNA homopolymers containing adenine (A) or 7-deazaadenine (X). The resulting structures resemble natural Watson-Crick base pairs and double-stranded DNA, with one strand being replaced by a supramolecular stack of continuous Pd-II complexes.
Atomic-level control over the position and growth of a single and continuous metal chain is an ambitious goal that often requires complex and costly processes. Herein, we demonstrate that 1Pd-DNA molecules, comprising a continuous single chain of Pd-II ions, can be prepared by a simple self-assembly reaction between the complex [Pd(Cheld)(CH3CN)] (1Pd_CH3CN) (Cheld=chelidamic acid) and single-stranded DNA homopolymers (ss-DNA) containing adenine (A) or 7-deazaadenine (X) bases. The single Pd-II-base pairs [1Pd(N1-A)] and [1Pd(N1-X)] were synthesized and characterized in solution and solid-state (X-ray diffraction) revealing an arrangement similar to that of natural Watson-Crick base pairs. Subsequently, 1Pd-DNA hybrids were prepared, characterized, and their structures studied by small-angle X-ray scattering (SAXS) and ab-initio calculations. The results indicate that the 1Pd-DNA structures resemble that of double-stranded DNA, with one strand being replaced by a supramolecular stack of continuous Pd-II complexes.
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