Solution-processable Ni3(HITP)2/MXene heterostructures for ppb-level gas detection

Abstract

Developing sensitive metal–organic framework (MOF) systems to overcome the ubiquitous trade-off between porosity and conductivity remains a formidable yet sought-after endeavor. This pursuit is of great significance for the development of MOF-based chemiresistive sensors with enhanced sensitivity and selectivity. Herein, we present an innovative template assisted strategy that utilizes the two-dimensional properties and good conductivity of MXene nanosheets, as well as lattice matching between MXene (Nb₂C) and selected Ni₃(HITP)₂, to achieve controllable self-assembly of Ni₃(HITP)₂ on MXene sheets. This results in Ni₃(HITP)₂/MXene (HITP: 2,3,6,7,10,11-hexaaminotriphenylene) heterostructures with considerable conductivity, porosity, and solution processability. The powder and film electrical conductivity are 4.8 × 10³ and 5.3 × 10⁵ S m⁻¹, respectively, and the BET specific surface area can reach 797.8 m² g⁻¹. It is worth noting that excellent solution processability helps to prepare large-area films (23 cm × 9 cm) with good uniformity. Gas sensors based on Ni₃(HITP)₂/MXene heterostructures exhibit high sensitivity (LOD ∼ 5 ppb) and selectivity towards ultratrace ethanol at room temperature, setting a new benchmark. Such sensing behavior stems from the strong coupling of Ni₃(HITP)₂/MXene heterostructures and their enhanced interaction with ethanol, evidenced by experimental results and theoretical calculations. Real-time respiratory sensing assessments underscore their practicality in healthcare monitoring. This straightforward approach simplifies the integration of MOF-related materials on miniaturized devices with outstanding performance.