Benchmarking the placement of hydrosulfide in the Hofmeister series using a bambus[6]uril-based ChemFET sensor.

Autor:	Kuhl GM; Department of Chemistry & Biochemistry, Materials Science Institute, University of Oregon 97403-1253 Eugene OR USA dwj@uoregon.edu https://www.dwjlab.com/., Banning DH; Department of Chemistry & Biochemistry, Materials Science Institute, University of Oregon 97403-1253 Eugene OR USA dwj@uoregon.edu https://www.dwjlab.com/., Fargher HA; Department of Chemistry & Biochemistry, Materials Science Institute, University of Oregon 97403-1253 Eugene OR USA dwj@uoregon.edu https://www.dwjlab.com/., Davis WA; Department of Chemistry & Biochemistry, Materials Science Institute, University of Oregon 97403-1253 Eugene OR USA dwj@uoregon.edu https://www.dwjlab.com/., Howell MM; Department of Chemistry & Biochemistry, Materials Science Institute, University of Oregon 97403-1253 Eugene OR USA dwj@uoregon.edu https://www.dwjlab.com/., Zakharov LN; Department of Chemistry & Biochemistry, Materials Science Institute, University of Oregon 97403-1253 Eugene OR USA dwj@uoregon.edu https://www.dwjlab.com/., Pluth MD; Department of Chemistry & Biochemistry, Materials Science Institute, University of Oregon 97403-1253 Eugene OR USA dwj@uoregon.edu https://www.dwjlab.com/., Johnson DW; Department of Chemistry & Biochemistry, Materials Science Institute, University of Oregon 97403-1253 Eugene OR USA dwj@uoregon.edu https://www.dwjlab.com/.
Jazyk:	angličtina
Zdroj:	Chemical science [Chem Sci] 2023 Sep 05; Vol. 14 (37), pp. 10273-10279. Date of Electronic Publication: 2023 Sep 05 (Print Publication: 2023).
DOI:	10.1039/d3sc03616b
Abstrakt:	Hydrosulfide (HS ^- ) is the conjugate base of gasotransmitter hydrogen sulfide (H 2 S) 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 SO 4 ^2- , F ^- , Cl ^- , Br ^- , NO 3 ^- , ClO 4 ^- , 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. Competing Interests: There are no conflicts to declare. (This journal is © The Royal Society of Chemistry.)
Databáze:	MEDLINE
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