Triphenylene-Based 2D cMOFs: Unraveling the H2S Sensing Mechanism and Applications for a Real-Time Wireless Chemiresistive Sensor

Abstract

Two-dimensional conductive metal-organic frameworks (2D cMOFs) stand at the forefront of chemiresistive sensing innovations due to their high surface areas, distinctive morphologies, and substantial electronic conductivity. Particularly, 2D cMOFs crafted using 2,3,6,7,10,11-hexahydroxytriphenylene (HHTP) and 2,3,6,7,10,11-hexaiminotriphenylene (HITP) organic ligands have garnered a large amount of attention due to their designable active sites and proper conductive characteristics. Nevertheless, a deeper exploration into their sensing mechanisms is imperative for a comprehensive understanding of the intrinsic chemistry, which is crucial for the intricate design of specialized 2D cMOF chemiresistive sensors. In this study, we fabricate six M-HXTP (M = Co, Ni, and Cu; X = H and I) chemiresistive sensors, focusing on the application of hydrogen sulfide (H2S) detection. Among these, the 2D cMOFs incorporating Cu metal manifested a remarkably enhanced response to H2S. A combination of experimental and computational studies unveils the mechanisms of sulfur oxidation and Cu reduction, wherein distortion of the reduced MX4 cluster markedly amplifies the sensing response. Lastly, a real-time and portable wireless H2S sensing module has been demonstrated by using the Cu-HHTP composite material, highlighting the substantial practical significance and potential applicability.