Abstract
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 CO2 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 CO2 sensors, including low detection limit, high sensitivity (0.18%/ppm), excellent reversibility (variation within 2%), and high selectivity (against C2H5OH, CH3OH, N2). 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.