Size Discrimination of Carbohydrates via Conductive Carbon Nanotube@Metal Organic Framework Composites

DL White and BA Day and ZD Zeng and ZM Schulte and NR Borland and NL Rosi and CE Wilmer and A Star, JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 143, 8022-8033 (2021).

DOI: 10.1021/jacs.1c01673

Traditional chemical sensing methodologies have typically relied on the specific chemistry of the analyte for detection. Modifications to the local environment surrounding the sensor represent an alternative pathway to impart selective differentiation. Here, we present the hybridization of a 2-D metal organic framework (Cu-3(HHTP)(2)) with single-walled carbon nanotubes (SWCNTs) as a methodology for size discrimination of carbohydrates. Synthesis and the resulting conductive performance are modulated by both mass loading of SWCNTs and their relative oxidation. Liquid gated field-effect transistor (FET) devices demonstrate improved on/off characteristics and differentiation of carbohydrates based on molecular size. Glucose molecule detection is limited to the single micromolar concentration range. Molecular Dynamics (MD) calculations on model systems revealed decreases in ion diffusivity in the presence of different sugars as well as packing differences based on the size of a given carbohydrate molecule. The proposed sensing mechanism is a reduction in gate capacitance initiated by the filling of the pores with carbohydrate molecules. Restricting diffusion around a sensor in combination with FET measurements represents a new type of sensing mechanism for chemically similar analytes.

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