Abstract:Abstract:The simultaneous removal of nitrogen oxides (NO x ) and sulfur dioxide (SO 2 ) by absorption is considered to be one of the most promising technologies for flue gas treatment, and sulfite is the main component of the absorption solution. To understand the chemical behaviors of the NO 2 absorption in sulfite solution, the absorption time dependences of concentrations of nitrogen and sulfur compositions in both gas phase and liquid phases were investigated by flue gas analyzer, Ion chromatography (IC), … Show more
“…In many experimental studies on air pollution, NO 2 is often used as a catalyst for producing sulfates from bisulfite ion (HSO 3 – ) or sulfite ion (SO 3 2– ) in the lead chamber process (for producing sulfuric acid in large quantities). − In these studies, the chemical mechanism responsible for the formation of sulfate through active nitrogen was mainly due to the direct contact between NO 2 and HSO 3 – /SO 3 2– , as independently proposed by Lee et al, Clifton et al, and Littlejohn et al Specifically, Spindler et al proposed that at pH 4.5, the first step in the electron-transfer reaction is HSO 3 – (aq) + NO 2 (aq) → SO 3 – (aq) + H + (aq) + NO 2 – (aq), which proceeds through a [HSO 3 –NO 2 ] − intermediate, with the N-atom of NO 2 being directly bonded to one O-atom of HSO 3 – ; at pH 10.0, the initial step in the aqueous reaction of dissolved NO 2 with SO 3 2– is NO 2 (aq) + SO 3 2– (aq) → [SO 3 –NO 2 ] 2– (aq) . These experimental studies on the aqueous conversion of HSO 3 – /SO 3 2– to sulfate via dissolved NO 2 were performed by flowing gaseous NO 2 through bulk solutions of NaHSO 3 or Na 2 SO 3 …”
A source of missing sulfate production associated with high-level fine-particle pollution in the megacities of China is believed to stem from the oxidation of a notable fraction of sulfur dioxide (SO 2 ) by nitrogen dioxide (NO 2 ) in aqueous aerosol environments, suggesting that an unknown reaction pathway exists for aqueous sulfur oxidation. At weakly acidic aerosols, the dissolved SO 2 mainly exists in the form of HSO 3 − , whereas at neutral aerosols, SO 3 2− becomes the main form. Herein, by using both ab initio molecular metadynamics simulations and high-level quantum mechanical calculations, we show a hitherto unreported chemical mechanism for the formation of sulfate through the reaction between HSO 3 − /SO 3 2− anions at the surface/in the interior of a water nanodroplet and gas-phase NO 2 molecules. For weakly acidic aerosols, contrary to the conventional high-barrier electron-transfer pathway in the gas phase, HSO 3 − at the water nanodroplet surface can transfer an electron to NO 2 with a low free-energy barrier of 4.7 kcal/mol through a water bridge. For neutral aerosols, the electron-transfer pathway between SO 3 2− in the interior of the water nanodroplet and NO 2 needs to overcome a lower free-energy barrier of 3.6 kcal/mol to form SO 3 − , with the assistance of the hydrogen-bonding network of water molecules. This new reaction pathway for the sulfate formation from HSO 3 − /SO 3 2− via water nanodroplets and gaseous NO 2 provides a new perspective on the growth of haze particles from pre-existing aqueous aerosols and suggests that new control strategies are needed to address haze pollution.
“…In many experimental studies on air pollution, NO 2 is often used as a catalyst for producing sulfates from bisulfite ion (HSO 3 – ) or sulfite ion (SO 3 2– ) in the lead chamber process (for producing sulfuric acid in large quantities). − In these studies, the chemical mechanism responsible for the formation of sulfate through active nitrogen was mainly due to the direct contact between NO 2 and HSO 3 – /SO 3 2– , as independently proposed by Lee et al, Clifton et al, and Littlejohn et al Specifically, Spindler et al proposed that at pH 4.5, the first step in the electron-transfer reaction is HSO 3 – (aq) + NO 2 (aq) → SO 3 – (aq) + H + (aq) + NO 2 – (aq), which proceeds through a [HSO 3 –NO 2 ] − intermediate, with the N-atom of NO 2 being directly bonded to one O-atom of HSO 3 – ; at pH 10.0, the initial step in the aqueous reaction of dissolved NO 2 with SO 3 2– is NO 2 (aq) + SO 3 2– (aq) → [SO 3 –NO 2 ] 2– (aq) . These experimental studies on the aqueous conversion of HSO 3 – /SO 3 2– to sulfate via dissolved NO 2 were performed by flowing gaseous NO 2 through bulk solutions of NaHSO 3 or Na 2 SO 3 …”
A source of missing sulfate production associated with high-level fine-particle pollution in the megacities of China is believed to stem from the oxidation of a notable fraction of sulfur dioxide (SO 2 ) by nitrogen dioxide (NO 2 ) in aqueous aerosol environments, suggesting that an unknown reaction pathway exists for aqueous sulfur oxidation. At weakly acidic aerosols, the dissolved SO 2 mainly exists in the form of HSO 3 − , whereas at neutral aerosols, SO 3 2− becomes the main form. Herein, by using both ab initio molecular metadynamics simulations and high-level quantum mechanical calculations, we show a hitherto unreported chemical mechanism for the formation of sulfate through the reaction between HSO 3 − /SO 3 2− anions at the surface/in the interior of a water nanodroplet and gas-phase NO 2 molecules. For weakly acidic aerosols, contrary to the conventional high-barrier electron-transfer pathway in the gas phase, HSO 3 − at the water nanodroplet surface can transfer an electron to NO 2 with a low free-energy barrier of 4.7 kcal/mol through a water bridge. For neutral aerosols, the electron-transfer pathway between SO 3 2− in the interior of the water nanodroplet and NO 2 needs to overcome a lower free-energy barrier of 3.6 kcal/mol to form SO 3 − , with the assistance of the hydrogen-bonding network of water molecules. This new reaction pathway for the sulfate formation from HSO 3 − /SO 3 2− via water nanodroplets and gaseous NO 2 provides a new perspective on the growth of haze particles from pre-existing aqueous aerosols and suggests that new control strategies are needed to address haze pollution.
“…The initial NO 2 and O 3 levels after the plasma discharge process were fixed at 480 ppm and 330 ppm, respectively. It can be concluded that NO 2 and O 3 were completely absorbed by Na 2 SO 3 in the initial 40 min, and the promotion of Na 2 SO 3 absorption concentration and the increase of pH value will prolong NO 2 and O 3 removal effectiveness [ 48 ]. The post sodium-based alkali solution absorption is an effective application of the NTP technique in industrial flue gas treatment.…”
Volatile organic compounds (VOCs) emission from anthropogenic sources has becoming increasingly serious in recent decades owing to the substantial contribution to haze formation and adverse health impact. To tackle this issue, various physical and chemical techniques are applied to eliminate VOC emissions so as to reduce atmospheric pollution. Among these methods, non-thermal plasma (NTP) is receiving increasing attention for the higher removal efficiency, non-selectivity, and moderate operation, whereas the unwanted producing of NO2 and O3 remains important drawback. In this study, a dielectric barrier discharge (DBD) reactor with wedged high voltage electrode coupled CuO foam in an in plasma catalytic (IPC) system was developed to remove toluene as the target VOC. The monolith CuO foam exhibits advantages of easy installation and controllable of IPC length. The influencing factors of IPC reaction were studied. Results showed stronger and more stable plasma discharge in the presence of CuO foam in DBD reactor. Enhanced performance was observed in IPC reaction for both of toluene conversion rate and CO2 selectivity compared to the sole NTP process at the same input energy. The longer the contributed IPC length, the higher the toluene removal efficiency. The toluene degradation mechanism under IPC condition was speculated. The producing of NO2 and O3 under IPC process were effectively removed using Na2SO3 bubble absorption.
“…The interactions between nitrogen and sulfur are highly dependent on the pH level due to the dissociative reaction . At pH values ≥7, SO 3 2– is the dominant form, and reaction creates a potential route for NO 2 hydrolysis − Reaction has been studied experimentally, and it has a significantly higher reaction rate than reaction . This interaction between S(IV) and NO 2 (aq) makes the simultaneous absorption of NO 2 and SO 2 an effective process under alkaline conditions.…”
The concept of coabsorption of NO2 and SO2 from flue gases, in combination with the
enhanced oxidation of NO
by ClO2(g), is studied on three scales, 0.2, 100, and 400
N m3/h, all with flue gases of different origins. The results
obtained from each setup are presented, together with modeling that
was applied to assess the scale-up of the concept and to validate
the model. The measurements confirm that ClO2 is highly
selective toward NO oxidation for temperatures in the range of 70–155
°C. A comparison of the results obtained for each scale reveals
that the 0.2 N m3/h setup confers a higher level of NO
x
absorption than the other setups, although
the trends remain similar. Simulations of the results underpredict
the level of NO2 absorption in the 0.2 N m3/h
setup while capturing the levels of absorption in the 100 N m3/h setup. An important finding is the rapid and complete oxidation
of S(IV) in the presence of NO2, which is not represented
in the reaction kinetics.
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