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Air pollution is one of the most environmentally harmful to the human health and the climate change. The present study is aimed to investigate the effectiveness and capability of novel composite adsorbents prepared from modification of activated carbons (ACs) in the removal of air pollutants. The effect of both triethoxysilane propylamine (TEPSA) and carbon nanotube (CNT) on the adsorption properties of AC (TEPSA/CNT/AC); in addition, silica gel prepared from TEPSA to form silica nanoparticles (SiNP) along with CNT and AC (SiNP/CNT/AC), was studied. Ammonia gas (NH3) was used in this study as a typical emerging gas air pollutant. The physicochemical characteristics of the prepared ACs samples were analyzed using BET surface area, SEM, EDX, TEM and FTIR. Their results proved considerable changes in the porosity and surface functional groups after modifying AC surface with TEPSA or SiNP and CNT instantly. The adsorption findings showed that the NH3 removal efficiency using the prepared AC samples reached almost 97, 86 and 75% during 90 min at 25 °C for each sample of SiNP/CNT/AC, TESPA/CNT/AC and AC, respectively. Adsorption of NH3 relied mainly on the presence of silica particles and mesopore distributions in CNT rather than large total surface area in AC alone. Thus, the combination of SiNP as silanol and siloxane groups with CNT on AC surface raised significantly the adsorption capacity of NH3 from 194 to 300 mg/g. Conclusively, the SiNP/CNT/AC sample exhibited the best performance among all prepared samples used for the adsorption of NH3 gas from the indoor air. Also, Langmuir and Freundlich models were applied, and the results revealed that Freundlich model fits well the equilibrium adsorption data. [ABSTRACT FROM AUTHOR]