MOF/Polymer-Integrated Multi-Hotspot Mid-Infrared Nanoantennas for Sensitive Detection of CO(2) Gas

Metal–organic frameworks (MOFs) have been extensively used for gas sorption, storage and separation owing to ultrahigh porosity, exceptional thermal stability, and wide structural diversity. However, when it comes to ultra-low concentration gas detection, technical bottlenecks of MOFs appear due to the poor adsorption capacity at ppm-/ppb-level concentration and the limited sensitivity for signal transduction. Here, we present hybrid MOF-polymer physi-chemisorption mechanisms integrated with infrared (IR) nanoantennas for highly selective and ultrasensitive CO(2) detection. To improve the adsorption capacity for trace amounts of gas molecules, MOFs are decorated with amino groups to introduce the chemisorption while maintaining the structural integrity for physisorption. Additionally, leveraging all major optimization methods, a multi-hotspot strategy is proposed to improve the sensitivity of nanoantennas by enhancing the near field and engineering the radiative and absorptive loss. As a benefit, we demonstrate the competitive advantages of our strategy against the state-of-the-art miniaturized IR CO(2) sensors, including low detection limit, high sensitivity (0.18%/ppm), excellent reversibility (variation within 2%), and high selectivity (against C(2)H(5)OH, CH(3)OH, N(2)). This work provides valuable insights into the integration of advanced porous materials and nanophotonic devices, which can be further adopted in ultra-low concentration gas monitoring in industry and environmental applications. [Image: see text] SUPPLEMENTARY INFORMATION: The online version contains supplementary material available at 10.1007/s40820-022-00950-1.