Toward Complete Resolution of DNA/Carbon Nanotube Hybrids by Aqueous Two-Phase Systems

Lyu, Min; Meany, Brendan; Yang, Juan; Li, Yan; Zheng, Ming

doi:10.1021/jacs.9b09953

Cited by 56 publications

(62 citation statements)

References 96 publications

(166 reference statements)

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“…In the past years ATPE of SWCNTs made tremendous progress in isolation of various small and large SWCNT chiralities. 40,[44][45][46][47] In this approach SWCNTs are dispersed either in a surfactant such as deoxycholate (DOC) or chirality-specific ssDNA 48,49 sequences and separated between aqueous phases of two different polymers. This fast, reliable and low-cost separation method appears to be an optimal starting point to obtain monochiral sensors.…”

Section: Introductionmentioning

confidence: 99%

Sensing with Chirality-Pure Near-Infrared Fluorescent Carbon Nanotubes

et al. 2021

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Semiconducting single wall carbon nanotubes (SWCNTs) fluoresce in the near infrared (NIR) and the emission wavelength depends on their chirality (n,m). Interactions with the environment affect the fluorescence and can be tailored by functionalizing SWCNTs with biopolymers such as DNA, which is the basis for fluorescent biosensors. So far, such biosensors were mainly assembled from mixtures of SWCNT chiralities with large spectral overlap, which affects sensitivity as well as selectivity and prevents multiplexed sensing. The main challenge to gain chirality pure sensors has been to combine approaches to isolate specific SWCNTs and generic (bio)functionalization approaches. Here, we created chirality pure SWCNT-based NIR biosensors for important analytes such as neurotransmitters and investigated the impact of SWCNT chirality/handedness as well as long-term stability and sensitivity. For this purpose, we used aqueous two-phase extraction (ATPE) to gain chirality pure (6,5)-, (7,5)-, (9,4)-and (7,6)-SWCNTs (emission at ~ 990, 1040, 1115 and 1130 nm). Exchange of the surfactant sodium deoxycholate (DOC) to specific singlestranded (ss)DNA sequences yielded monochiral sensors for small analytes (dopamine, riboflavin, ascorbic acid, pH). DOC used in the separation process was completely removed because residues impaired sensing. The assembled monochiral sensors were up to 10 times brighter than their non-purified counterparts and the ssDNA sequence affected absolute fluorescence intensity as well as colloidal (long-term) stability and selectivity for the analytes. (GT)40-(6,5)-SWCNTs displayed the maximum fluorescence response to the neurotransmitter dopamine (+140 %, Kd = 1.9 x10-7 M) and a long-term stability > 14 days. Furthermore, the specific ssDNA sequences imparted selectivity to the analytes independent of SWCNT chirality and handedness of (+/-) (6,5)-SWCNTs. These monochiral/single-color SWCNTs enabled ratiometric/multiplexed sensing of dopamine, riboflavin, H2O2 and pH. In summary, we demonstrated the assembly, characteristics and potential of monochiral (single-color) SWCNTs for multiple NIR fluorescent sensing applications.File list (2) download file view on ChemRxiv Chirality pure sensing_MS.pdf (1.87 MiB) download file view on ChemRxiv Chirality pure sensing_SI.pdf (3.43 MiB)

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Section: Introductionmentioning

confidence: 99%

Sensing with Chirality-Pure Near-Infrared Fluorescent Carbon Nanotubes

et al. 2021

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“…It has to be noted that the outcome of the separation could also be affected by varying the MW of the polymer. Lyu et al reported that by changing the MW of the employed PEG different partitioning can be obtained 51 . The impact of Pluronic MW and its composition on the course of the separation will be studied by us in the future.…”

Section: Resultsmentioning

confidence: 99%

“…We wanted to evaluate whether the ATPE system can be optimized, using high-throughput analysis, to non-ionic surfactant and DNA-SWCNT hybrids. For this experiment, we selected a TTT-CCC-TTT-CCC-CCC ssDNA super-sequence recently reported to have a high affinity towards (8,3) and a few other SWCNT types in ATPE 51 . A super-sequence, according to this work, is a sequence able to resolve more than two kinds of SWCNTs from a single DNA-SWCNT dispersion.…”

Section: Resultsmentioning

confidence: 99%

En route to single-step, two-phase purification of carbon nanotubes facilitated by high-throughput spectroscopy

Podlesny

Olszewska

Yaari

et al. 2021

Sci Rep

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Chirality purification of single-walled carbon nanotubes (SWCNTs) is desirable for applications in many fields, but general utility is currently hampered by low throughput. We discovered a method to obtain single-chirality SWCNT enrichment by the aqueous two-phase extraction (ATPE) method in a single step. To achieve appropriate resolution, a biphasic system of non-ionic tri-block copolymer surfactant is varied with an ionic surfactant. A nearly-monochiral fraction of SWCNTs can then be harvested from the top phase. We also found, via high-throughput, near-infrared excitation-emission photoluminescence spectroscopy, that the parameter space of ATPE can be mapped to probe the mechanics of the separation process. Finally, we found that optimized conditions can be used for sorting of SWCNTs wrapped with ssDNA as well. Elimination of the need for surfactant exchange and simplicity of the separation process make the approach promising for high-yield generation of purified single-chirality SWCNT preparations.

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“…24,46,49 DNA-assisted sorting is another attractive option since its sequence can be engineered to enhance its interaction towards a specific type of SWCNT. 50 Similarly, various other polymers and copolymers have been designed to selectively interact with specific SWCNTs. For example, Tetronic with hydrophilic blocks favors metallic SWCNTs while Pluronic that has short hydrophobic chains shows high affinity towards semiconductor SWCNTs.…”

Section: Separation and Sortingmentioning

confidence: 99%