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Development of room-temperature gas sensors with excellent sensing performances for detection of dimethyl methylphosphonate (DMMP, a simulant of organophosphate) has aroused considerable attention. However, the weak adsorption ability of sensing materials toward DMMP molecules causes poor sensing performances. In this work, a multisite strategy for enhancing sensitivity was proposed by introduction of both N-doped carbon nanoparticles (N-CNPs) and copper ions onto the surface of rGO (designated as GNC). Impressively, optimal GNC-3 exhibits the response value of 10.2% toward 100 ppm DMMP, which is 5.3 times higher than that of pristine rGO. This mechanism for multisite-assisted enhanced DMMP sensing performances was investigated by combined characterizations of Fourier-transform infrared spectra, UV-Vis spectra, photoluminescence spectra and Mott-Schottky curves. Besides the construction of multisite, improvement of hydrogen bonding interactions between DMMP molecules and N-CNPs in hybrids assisted by copper ions, and decrease of conduction band potential by formation of ternary hybrids also contribute to enhance the sensitivity of DMMP sensors. These findings not only provided new insights into designing high-performance room-temperature gas sensors, but also promoted the fundamental research on sensing mechanism for room-temperature gas sensors. • A multisite strategy for enhancing sensitivity was proposed by constructing three kinds of DMMP adsorption active sites. • GNC hybrids demonstrate 5.3-fold improvement in response to 100 ppm DMMP compared to pristine rGO hybrids. • This mechanism for multisite-assisted enhanced DMMP sensing performances was confirmed by the spectroscopy. [ABSTRACT FROM AUTHOR]

The hydrogen bonding interactions are potentially employed to fabricate high-performance room-temperature gas sensors for detection of organophosphorus. Nevertheless, the low response toward target gases of conventional sensing materials hinders their further applications. Herein, an isolated Cu-N 5 sites engineering strategy is reported to improve sensing performances for polypyrrole-reduced graphene oxide hybrids (PPy-rGO)-based room-temperature dimethyl methyl phosphate (DMMP) sensors. The isolated Cu-N 5 sites were simply constructed by adsorption of Cu2+ ions with PPy-rGO hybrids owing to strong metal-support interactions. X-ray absorption fine structure analysis indicates that Cux+ ions with mean chemical valence of + 1.07 nearly atomically distributed on support with coordination structure of Cu-N 5. Benefiting from the structure regulation by Cux+ ions, as-constructed DMMP sensor demonstrated 4.5-fold improvement in response to 100 ppm DMMP and 2.5-fold improvement in limit of detection, compared to PPy-rGO hybrids. The density functional theory, spectroscopic characterizations and quartz crystal microbalance tests prove that the construction of Cu-N 5 sites not only heightens hydrogen bonding interactions between N H bonds and DMMP molecules induced by newly formed coordination interactions between Cux+ ions and N H bonds, but also serves as new active sites for adsorption of DMMP molecules. This work offers a new avenue for developing high-performance room-temperature gas sensors by heightening hydrogen bonding interactions. • Isolated Cu-N 5 sites-assisted heightening hydrogen bonds strategy is proposed to construct room-temperature DMMP sensors. • Cux+-PPy-rGO hybrids demonstrate 4.5-fold improvement in response to 100 ppm DMMP compared to PPy-rGO hybrids. • The limit of detection of the Cux+-PPy-rGO based sensor is 2 ppm. [ABSTRACT FROM AUTHOR]