Nanopore surface engineering of molecular imprinted mesoporous organosilica for rapid and selective detection of L-thyroxine

Abstract

To develop a biosensing platform for precise diagnosis and management of thyroid-related diseases, the sensitive and selective recognition and identification of L-thyroxine (T4), a thyroid hormone, remains challenging. We herein introduce T4-imprinted mesoporous organosilica (T4-IMO) for sensitive and specific detection of T4 via the sophisticated engineering of pore surfaces using additives with different polarities. The pore surface of T4-IMO emitting a stable fluorescence signal is simply modified by fixed additives. Additives embedded in the pore surface promote the rebinding response of T4 into the recognized cavities, subsequently sensitizing T4 detection. Notably, T4-IMO containing abundant fluorine elements on the pore surface shows a high affinity toward T4, remarkably boosting the rebinding capacity. In addition to good selectivity to T4, the "turn-off" fluorescent signal exhibits a linear relationship with the logarithm of T4 concentration in a range of 0-500 nM with a detection limit of 0.47 nM in synthetic urine samples. Our findings can establish an insightful strategy for the rational design of molecular-recognition-based sensor systems for the selective and sensitive detection of target analytes.

Keywords: L-thyroxine; Mesoporous organosilica; Molecular recognition; Pore surface engineering; Rebinding.