Benchmarking the placement of hydrosulfide in the Hofmeister series using a bambus[6]uril-based ChemFET sensor.
Benchmarking the placement of hydrosulfide in the Hofmeister series using a bambus[6]uril-based ChemFET sensor.
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DOI：
10.1039/d3sc03616b
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发表时间：
2023-09-27
期刊：
影响因子：
8.4
通讯作者：
Johnson, Darren W.
中科院分区：
文献类型：
--
作者：
Kuhl, Grace M.;Banning, Douglas H.;Fargher, Hazel A.;Davis, Willow A.;Howell, Madeline M.;Zakharov, Lev N.;Pluth, Michael D.;Johnson, Darren W.
Hydrosulfide (HS−) is the conjugate base of gasotransmitter hydrogen sulfide (H2S) and is a physiologically-relevant small molecule of great interest in the anion sensing community. However, selective sensing and molecular recognition of HS− in water remains difficult because, in addition to the diffuse charge and high solvation energy of anions, HS− is highly nucleophilic and readily oxidizes into other reactive sulfur species. Moreover, the direct placement of HS− in the Hofmeister series remains unclear. Supramolecular host–guest interactions provide a promising platform on which to recognize and bind hydrosulfide, and characterizing the placement of HS− in the Hofmeister series would facilitate the future design of selective receptors for this challenging anion. Few examples of supramolecular HS− binding have been reported, but the Sindelar group reported HS− binding in water using bambus[6]uril macrocycles in 2018. We used this HS− binding platform as a starting point to develop a chemically-sensitive field effect transistor (ChemFET) to facilitate assigning HS− to a specific place in the Hofmeister series. Specifically, we prepared dodeca-n-butyl bambus[6]uril and incorporated it into a ChemFET as the HS− receptor motif. The resultant device provided an amperometric response to HS−, and we used this device to measure the response of other anions, including SO42−, F−, Cl−, Br−, NO3−, ClO4−, and I−. Using this response data, we were able to experimentally determine that HS− lies between Cl− and Br− in the Hofmeister series, which matches recent theoretical computational work that predicted a similar placement. Taken together, these results highlight the potential of using molecular recognition coupled with ChemFET architectures to develop new approaches for direct and reversible HS− detection and measurement in water and further advance our understanding of different recognition approaches for this challenging anion. Bambusuril-containing ChemFET sensor membranes show excellent selectivity for HS− and inform on its placement in the Hofmeister series.
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