Department of Mechanical & Mechatronics Engineering, ‡Department of Civil & Environmental Engineering, University of Waterloo , 200 University Avenue West, Waterloo, Ontario, Canada N2L 3G1.
Environ Sci Technol. 2014 Feb 18;48(4):2453-63. doi: 10.1021/es403901r. Epub 2014 Feb 7.
Experiments were conducted using a custom double-stirred tank reactor to determine the rate constants of reactions between nitric oxide (NO) and both pentaaminecobalt(II) and hexaaminecobalt(II) at temperatures of 298.2 and 303.2 K and pH levels between 8.50 and 9.87 under atmospheric pressure. The NO concentration of simulated flue gas stream ranged from 400 to 1400 ppmv. Ammoniacal cobalt(II) solutions were prepared by adding aqueous ammonia into a cobalt(II) nitrate solution in the presence of concentrated ammonium nitrate. The reaction rate constants were calculated with an enhancement factor for gas absorption associated with parallel chemical reactions. The results showed that the reaction between NO and pentaaminecobalt(II) was first order with respect to both the NO and the pentaamminecobalt(II) ion. Similarly, the reaction between NO and hexaamminecobalt(II) was first order with respect to both the NO and the hexaamminecobalt(II) ion. The forward reaction rate constants of these two reactions were 6.43 × 10(6) and 1.00 × 10(7) L · mol(-1) · s(-1) at 298.2 K, respectively, and increased to 7.57 × 10(6) and 1.12 × 10(7) L · mol(-1) · s(-1) at 303.2 K, respectively. Ammoniacal cobalt(II) solutions also have the potential to simultaneously remove CO2, SO2, and NOx from postcombustion flue gas.
实验采用定制的双搅拌釜式反应器进行,在 298.2 和 303.2 K 的温度下,以及在大气压力下的 8.50 至 9.87 的 pH 值范围内,确定了一氧化氮 (NO) 与五氨合钴(II)和六氨合钴(II)之间反应的速率常数。模拟烟道气中 NO 的浓度范围为 400 至 1400 ppmv。氨合钴(II)溶液是通过在存在浓硝酸铵的情况下,将氨水溶液加入到硝酸钴(II)溶液中来制备的。反应速率常数是通过与平行化学反应相关的气体吸收增强因子计算得出的。结果表明,NO 与五氨合钴(II)的反应对 NO 和五氨合钴(II)离子均为一级反应。同样,NO 与六氨合钴(II)的反应对 NO 和六氨合钴(II)离子也均为一级反应。这两个反应的正向反应速率常数在 298.2 K 时分别为 6.43×10(6)和 1.00×10(7)L·mol(-1)·s(-1),在 303.2 K 时分别增加到 7.57×10(6)和 1.12×10(7)L·mol(-1)·s(-1)。氨合钴(II)溶液也有可能同时从燃烧后烟道气中去除 CO2、SO2 和 NOx。