An ionic liquid form of DNA: Redox-active molten salts of nucleic acids

A. M. Leone; S. C. Weatherly; M. E. Williams; H. H. Thorp; R. W. Murray

doi:10.1021/ja003332c

An ionic liquid form of DNA: Redox-active molten salts of nucleic acids

A. M. Leone, S. C. Weatherly, M. E. Williams, H. H. Thorp, R. W. Murray

Research output: Contribution to journal › Article › peer-review

123 Scopus citations

Abstract

Ionic liquids are described that contain duplex DNA as the anion and polyether-decorated transition metal complexes based on M(MePEG-bpy)₃²⁺ as the cation (M = Fe, Co; MePEG-bpy = 4,4′-(CH₃(OCH₂ -CH₂)₇OCO)₂-2,2′-bipyridine). When the undiluted liquid DNA - or molten salt - is interrogated electrochemically by a microelectrode, the molten salts exhibit cyclic voltammograms due to the physical diffusion (D_PHYS) of the polyether-transition metal complex. When M = Co(II), the cyclic voltammogram of the melt shows an oxidative wave due to the Co(III/II) couple at E_1/2 = 0.40 V (versus Ag/AgCl) and a D_PHYS of 6 × 10^-12 cm²/s, which is significantly lower than that for Co(MePEG-bpy)₃(ClO₄)₂ (D_PHYS = 2.6 × 10^-10 cm²/s) due to greater viscosity provoked by the DNA polymer. When a 1:1 mixture is made of the Co(MePEG-bpy)₃. DNA and Fe(MePEG-bpy)₃(ClO₄)₂ melts, two redox waves are observed. The first is due to the Co(III/II) couple, and the second is a catalytic wave due to oxidation of guanine in DNA by electrogenerated Fe(III) in the undiluted melt. Independent experiments show that the Fe(III) form of the complex selectively oxidizes guanine in duplex DNA. These DNA molten salts constitute a new class of materials whose properties can be controlled by nucleic acid sequence and that can be interrogated in undiluted form on microelectrode arrays.

Original language	English (US)
Pages (from-to)	218-222
Number of pages	5
Journal	Journal of the American Chemical Society
Volume	123
Issue number	2
DOIs	https://doi.org/10.1021/ja003332c
State	Published - Jan 17 2001

All Science Journal Classification (ASJC) codes

Catalysis
General Chemistry
Biochemistry
Colloid and Surface Chemistry

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10.1021/ja003332c

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@article{f474e155918a43da822e2a63b1d9701e,

title = "An ionic liquid form of DNA: Redox-active molten salts of nucleic acids",

abstract = "Ionic liquids are described that contain duplex DNA as the anion and polyether-decorated transition metal complexes based on M(MePEG-bpy)32+ as the cation (M = Fe, Co; MePEG-bpy = 4,4′-(CH3(OCH2 -CH2)7OCO)2-2,2′-bipyridine). When the undiluted liquid DNA - or molten salt - is interrogated electrochemically by a microelectrode, the molten salts exhibit cyclic voltammograms due to the physical diffusion (DPHYS) of the polyether-transition metal complex. When M = Co(II), the cyclic voltammogram of the melt shows an oxidative wave due to the Co(III/II) couple at E1/2 = 0.40 V (versus Ag/AgCl) and a DPHYS of 6 × 10-12 cm2/s, which is significantly lower than that for Co(MePEG-bpy)3(ClO4)2 (DPHYS = 2.6 × 10-10 cm2/s) due to greater viscosity provoked by the DNA polymer. When a 1:1 mixture is made of the Co(MePEG-bpy)3. DNA and Fe(MePEG-bpy)3(ClO4)2 melts, two redox waves are observed. The first is due to the Co(III/II) couple, and the second is a catalytic wave due to oxidation of guanine in DNA by electrogenerated Fe(III) in the undiluted melt. Independent experiments show that the Fe(III) form of the complex selectively oxidizes guanine in duplex DNA. These DNA molten salts constitute a new class of materials whose properties can be controlled by nucleic acid sequence and that can be interrogated in undiluted form on microelectrode arrays.",

author = "Leone, {A. M.} and Weatherly, {S. C.} and Williams, {M. E.} and Thorp, {H. H.} and Murray, {R. W.}",

year = "2001",

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doi = "10.1021/ja003332c",

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T2 - Redox-active molten salts of nucleic acids

AU - Leone, A. M.

AU - Weatherly, S. C.

AU - Williams, M. E.

AU - Thorp, H. H.

AU - Murray, R. W.

PY - 2001/1/17

Y1 - 2001/1/17

N2 - Ionic liquids are described that contain duplex DNA as the anion and polyether-decorated transition metal complexes based on M(MePEG-bpy)32+ as the cation (M = Fe, Co; MePEG-bpy = 4,4′-(CH3(OCH2 -CH2)7OCO)2-2,2′-bipyridine). When the undiluted liquid DNA - or molten salt - is interrogated electrochemically by a microelectrode, the molten salts exhibit cyclic voltammograms due to the physical diffusion (DPHYS) of the polyether-transition metal complex. When M = Co(II), the cyclic voltammogram of the melt shows an oxidative wave due to the Co(III/II) couple at E1/2 = 0.40 V (versus Ag/AgCl) and a DPHYS of 6 × 10-12 cm2/s, which is significantly lower than that for Co(MePEG-bpy)3(ClO4)2 (DPHYS = 2.6 × 10-10 cm2/s) due to greater viscosity provoked by the DNA polymer. When a 1:1 mixture is made of the Co(MePEG-bpy)3. DNA and Fe(MePEG-bpy)3(ClO4)2 melts, two redox waves are observed. The first is due to the Co(III/II) couple, and the second is a catalytic wave due to oxidation of guanine in DNA by electrogenerated Fe(III) in the undiluted melt. Independent experiments show that the Fe(III) form of the complex selectively oxidizes guanine in duplex DNA. These DNA molten salts constitute a new class of materials whose properties can be controlled by nucleic acid sequence and that can be interrogated in undiluted form on microelectrode arrays.

AB - Ionic liquids are described that contain duplex DNA as the anion and polyether-decorated transition metal complexes based on M(MePEG-bpy)32+ as the cation (M = Fe, Co; MePEG-bpy = 4,4′-(CH3(OCH2 -CH2)7OCO)2-2,2′-bipyridine). When the undiluted liquid DNA - or molten salt - is interrogated electrochemically by a microelectrode, the molten salts exhibit cyclic voltammograms due to the physical diffusion (DPHYS) of the polyether-transition metal complex. When M = Co(II), the cyclic voltammogram of the melt shows an oxidative wave due to the Co(III/II) couple at E1/2 = 0.40 V (versus Ag/AgCl) and a DPHYS of 6 × 10-12 cm2/s, which is significantly lower than that for Co(MePEG-bpy)3(ClO4)2 (DPHYS = 2.6 × 10-10 cm2/s) due to greater viscosity provoked by the DNA polymer. When a 1:1 mixture is made of the Co(MePEG-bpy)3. DNA and Fe(MePEG-bpy)3(ClO4)2 melts, two redox waves are observed. The first is due to the Co(III/II) couple, and the second is a catalytic wave due to oxidation of guanine in DNA by electrogenerated Fe(III) in the undiluted melt. Independent experiments show that the Fe(III) form of the complex selectively oxidizes guanine in duplex DNA. These DNA molten salts constitute a new class of materials whose properties can be controlled by nucleic acid sequence and that can be interrogated in undiluted form on microelectrode arrays.

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An ionic liquid form of DNA: Redox-active molten salts of nucleic acids

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