ABSTRACT
The improvement of air quality in densely-populated urban regions constitutes an environmental challenge of increasing concern. In this respect, the abatement of NO emissions, primarily emanating from combustion processes associated with motor-vehicles, along with industrial/domestic combustion systems, represents one of the main problems. Here, three hydrochars from diverse organic residues were used as activated carbon precursors for their evaluation in the NO removal in two potential application scenarios. Hydrochars were physically activated at 800 °C with pure-CO2 or diluted-O2. These materials were tested in a lab-scale biofilter at different conditions (NO concentration, temperature, relative humidity, NO-containing gas and carbon particle size) and in a larger-scale biofilter to evaluate the long-term NO removal capacity. Hydrochar-derived carbons present a relatively well-developed micro- and mesoporous structure, with BET areas of up to 421 m2/g, and a variety of oxygen surface functionalities (carboxylic, lactone, carbonyl and quinone groups), especially concerning CO2-activated carbons. These exhibited an excellent behaviour at low NO concentration (5 ppmv) between 25 and 75 °C with removal capacities of ≈97 % and > 82 %, respectively; and still good-performance (≈66 %) in a more concentrated gas (120 ppmv). Whilst, carbons obtained by diluted-O2 activation from the same hydrochars, evidenced a higher removal capacity loss at high NO concentration. The O2 presence in the gas stream was confirmed as a crucial factor in the NO elimination, since both co-adsorb on the carbon surface favouring NO oxidation to NO2. Besides, the humidity in the airstream diminished the NO removal capacity from 0.88 to 0.51 mgNO/gcarbon, but still remained at 0.54 mgNO/gcarbon, when the carbon (in pellet) was operated at larger-scale biofilter in 9-fold longer test under humid air. Therefore, this study highlights the potential of renewable carbons to serve as cost-effective component in urban biofilters, to mitigate NO emissions from exhaust gases in biomass boilers and urban semi-close areas.
ABSTRACT
This work presents an innovative and sustainable approach to remove NO emissions from urban ambient air in confined areas (underground parking areas or tunnels) using low-cost activated carbons obtained from Miscanthus biochar (MSP700) by physical activation (with CO2 or steam) at temperatures ranging from 800 to 900 °C. The NO removal capacity of the activated biochars was evaluated under different conditions (temperature, humidity and oxygen concentration) and compared against a commercial activated carbon. This last material showed a clear dependence on oxygen concentration and temperature, exhibiting a maximum capacity of 72.6% in air at 20 °C, whilst, its capacity notably decreased at higher temperatures, revealing that physical NO adsorption is the limiting step for the commercial sample that presents limited oxygen surface functionalities. In contrast, MSP700-activated biochars reached nearly complete NO removal (99.9%) at all tested temperatures in air ambient. Those MSP700-derived carbons only required low oxygen concentration (4 vol%) in the gas stream to achieve the full NO removal at 20 °C. Moreover, they also showed an excellent performance in the presence of H2O, reaching NO removal higher than 96%. This remarkable activity results from the abundance of basic oxygenated surface groups, which act as active sites for NO/O2 adsorption, along with the presence of a homogeneous microporosity of 6 Å, which enables intimate contact between NO and O2. These features promote the oxidation of NO to NO2, which is further retained over the carbon surface. Therefore, the activated biochars studied here could be considered promising materials for the efficient removal of NO at low concentrations from air at moderate temperatures, thus closely approaching real-life conditions in confined spaces.
