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Abstract: Experiments on CO2 removal from flue gas using polypropylene (PP) hollow fiber membrane contactors were conducted in this study. Absorbents including aqueous potassium glycinate (PG) solution, aqueous solutions of monoethanolamine (MEA) and methyldiethanolamine (MDEA) were used to absorb CO2 in the experiments. Based on the wetting experimental results, aqueous PG solution can offer a higher surface tension than water, aqueous MEA and MDEA solutions. Aqueous PG solution has a lower potential of membrane wetting after a continuously steady operation for 40 h to maintain CO2 removal efficiency of about 90%. Under moderate operating conditions, effects of the temperature, flow rate, and concentration of absorbents, and the flow rate of flue gas as well as the volumetric concentration of carbon dioxide in the flue gas on the mass transfer rate of CO2 were studied on a pilot-scale test facility. Unlike conventional absorbents, the mass transfer decreases with an increasing liquid temperature when using aqueous PG solution. Results show that CO2 removal efficiency was above 90% and the mass transfer rate was above 2.0 mol/(m2 h) using the PG aqueous solution. It indicates that the hollow fiber membrane contactor has a great potential in the area of CO2 separation from flue gas when absorbent''s concentration and liquid–gas pressure difference are designed elaborately. [Copyright &y& Elsevier]

Abstract: The NO and SO2 gas conversion processes in a pulsed corona discharge field have been studied. The experiments were conducted to investigate the influences of water vapor and fly ash addition on the conversion efficiencies of NO and SO2. Experimental results show that positive pulsed corona discharge can facilitate NO and SO2 conversion processes, and the conversion efficiencies of NO and SO2 are primarily dependent on the radicals OH, O and the active species O3, HO2, H2O2, etc. With water vapor addition, SO2 conversion efficiency is improved, but NO conversion process is restrained. Low fly ash concentration helps to enhance the conversion of NO and SO2; however, the conversion efficiencies of NO and SO2 are drastically degraded by high fly ash concentration addition. The synergistic effects of water vapor and fly ash addition strengthen the chemical adsorption ability of the fly ash surface, which results in a considerable improvement in the conversion of NO and SO2. Furthermore, the specific input energy plays an important role in NO and SO2 conversion efficiencies. Measured conversion efficiencies of NO and SO2 reach about 60% and 90%, respectively, under the conditions tested. [Copyright &y& Elsevier]

Pulsed corona discharge in atmosphere has been widely regarded as an efficient flue gas treatment technology for the generation of active radical species, such as the OH radicals. The spatial distribution of OH radicals generated by pulsed corona discharge plays an important role in decomposing pollutants. The two-dimensional (2-D) distribution of OH radicals of positive wire--plate pulsed corona discharge was detected using laser-induced fluorescence (LIF). The influence of relative humidity (RH) and oxygen concentration on the 2-D distribution of OH radicals were investigated. The results indicated that the 2-D distribution of OH radicals was characterized by a fan-shaped distribution from the wire electrode to plate electrode, and both the maximum values of vertical length and horizontal width of the fan area was less than 1 cm. The 2-D distribution area of OH radicals increased significantly with increasing the RH and the optimum condition was 65% RH. The optimal level of the oxygen concentration for the 2-D distribution area of OH radicals was 2%. The process of OH radical generation and 2-D distribution area of OH radicals were significantly interfered when the oxygen concentration was larger than 15%. The total quenching rate coefficients for different RH values and oxygen concentration in this study were used to calculate the fluorescence yield of OH radical. The fluorescence yield, which is the ratio between the emission rate (Einstein coefficient) and the sum of the emission rate and quenching rate, was used to normalize the 2-D distribution area of OH radicals. The fluorescence yield of OH radical decreased with increasing the RH and oxygen concentration linearly and rapidly. It was also found that compared with the RH, the influence of the oxygen concentration had more notable effect on the fluorescence yield of OH radical and 2-D distribution area of OH radicals.

A crucial problem for the promising absorbent aqueous ammonia (NH3) is the low CO2 absorption rate. The mass transfer coefficient (K(G)) of CO2 in aqueous NH3-based absorbents on a wetted wall column facility was investigated. Monoethanolamine (MEA), piperazine (PZ), 1-methyl piperazine (1-MPZ) and 2-methyl piperazine (2-MPZ) were introduced into NH3 solutions as additives, all of which significantly increased the mass transfer coefficient of CO2 in the solutions. With CO2 loading of 0, 0.1, 0.3, 0.5 mol x mol(-1), K(G) of 3 mol x L(-1) NH3 + 0.3 mol x L(-1) PZ blended solution increased by 2, 2.2, 2.2, and 1.9 fold as compared to that of 3 mol x L(-1) NH3. Typically, PZ, the additive with best performance, was chosen for further study. The effects of temperature and PZ concentration on CO2 absorption in PZ solution and the blended NH3/PZ solution. The calculated pseudo first order rate constant [42.7 m3 x (mol x s)(-1)] was analyzed to further elucidate the reaction mechanism in the blended NH3/PZ solution.

Biomass pyrolysis in presence of abundant CaO additives is a fundamental process prior to CaO sorption enhanced gasification in biomass-based zero emission system. In the present study, thermogravimetric Fourier transform infrared (TG-FTIR) analysis was adopted to examine the effects of CaO additives on the mass loss process and volatiles evolution of wheat-straw pyrolysis. Observations from TG and FTIR analyses simultaneously demonstrated a two-stage process for CaO catalyzed wheat-straw pyrolysis, different from the single stage process for pure wheat-straw pyrolysis. CaO additives could not only absorb the released CO2 but also reduce the yields of tar species such as toluene, phenol, and formic acid in the first stage, resulting in decreased mass loss and maximum mass loss rate in this stage with an increase in CaO addition. The second stage was attributed to the CaCO3 decomposition and the mass loss and maximum mass loss rate increased with increasing amount of CaO additives. The results of the present study demonstrated the great potential of CaO additives to capture CO2 and reduce tars yields in biomass-based zero emission system. The gasification temperature in the system should be lowered down to avoid CaCO3 decomposition.

Three kinds of blended absorbents were investigated on bench-scale experimental bench according to absorption rate and regeneration grade to select a reasonable additive concentration. The results show that, among methyldiethanolamine (MDEA) and piperazine (PZ) mixtures, comparing MDEA : PZ = 1 : 0.4 (m : m) with MDEA : PZ = 1 : 0.2 (m : m), the absorption rate is increased by about 70% at 0.2 mol x mol(-1). When regeneration lasting for 40 min, regeneration grade of blended absorbents with PZ concentration of 0.2, 0.4, and 0.8 is decreased to 83.06%, 77.77% and 76.67% respectively while 91.04% for PZ concentration of 0. MDEA : PZ = 1 : 0.4(m : m) is a suitable ratio for MDEA/PZ mixtures as absorption and regeneration properties of the blended absorbents are all improved. The aqueous blends with 10% primary amines and 2% tertiary amines could keep high CO2 absorption rate, and lower regeneration energy consumption. Adding 2% 2-Amino-2-methyl-1-propanol (AMP) to 10% diethanolamine (DEA), the blended amine solvents have an advantage in absorption and regeneration properties over other DEA/AMP mixtures. Blended solvents, which consist of a mixture of primary amines with a small amount of tertiary amines, have the highest absorption rate among the three. And mixed absorbents of secondary amines and a small amount of sterically hindered amines have the best regeneration property. To combine absorption and regeneration properties, blends with medium activator addition to tertiary amines are competitive.

Three typical absorbents such as aqueous of aminoacetic acid potassium (AAAP), monoethanolamine (MEA) and methyldiethanolamine(MDEA) are selected to investigate the performance of CO2 separation from flue gas via membrane contactors made of hydrophobic hollow fiber polypropylene porous membrane. Impacts of absorbents, concentrations and flow rates of feeding gas and absorbent solution, cyclic loading of CO2 on the removal rate and the mass transfer velocity of CO2 are discussed. The results demonstrate that the mass transfer velocity was 7.1 mol x (m2 x s)(-1) for 1 mol x L(-1) MEA with flow rate of 0.1 m x s(-1) and flue gas with that of 0.211 m x s(-1). For 1 mol L(-1) AAAP with flow rate of 0.05 m x s(-1) and flue gas of 0.211 m x s(-1), CO2 removal rate (eta) was 93.2 % and eta was 98% for 4 mol x L(-1) AAAP under the same conditions. AAAP being absorbent, eta was higher than 90% in a wider range of concentrations of CO2. It indicates that membrane-based absorption process is a widely-applied and promising way of CO2 removal from flue gas of power plants, which not only appropriates for CO2 removal of flue gas of widely-used PF and NGCC, but also for that of flue gas of IGCC can be utilized widely in future.