State Key Laboratory of Clean Energy Utilization, Zhejiang University, Hangzhou, China.
Chemosphere. 2010 Mar;78(10):1230-5. doi: 10.1016/j.chemosphere.2009.12.043. Epub 2010 Jan 13.
The effect of sulfur dioxide (SO(2)) on de novo synthesis of polychlorinated dibenzo-p-dioxins, dibenzofurans (PCDD/F) and biphenyls (PCB) was investigated in model systems containing carbon, activated by cupric chloride (CuCl(2)). Five types of carbons (activated carbon, three types of carbon blacks, and graphite) were used to test the universal character of our results. The influence of SO(2) on speciation and behavior of copper compounds, catalytic oxidation of carbons, and formation of organic chlorine (extractable organic chlorine and non-extractable organic chlorine) was also studied to investigate the inhibition mechanism of SO(2) on de novo synthesis. It was found that SO(2) can sulfate CuCl(2), but does not react with CuO and CuCl(2).CuO in a 10% O(2)/N(2) atmosphere at 300 degrees C. The suppression by SO(2) of organic chlorine (C-Cl) formation also confirmed these findings. It was also found that catalytic oxidation of carbons was strongly suppressed by SO(2). A dramatic decrease in PCDD/Fs formation was observed for all five carbons, while adding SO(2); at the same time the average chlorination level also decreased. However, the inhibiting effect on PCB was less apparent compared with that on PCDD/F. On the basis of the experimental results, the conversion of both cupric and cuprous chloride into the non-reactive sulfate was proposed as inhibition mechanism.
二氧化硫 (SO(2)) 对新型多氯二苯并对二恶英、二苯并呋喃 (PCDD/F) 和联苯 (PCB) 合成的影响在含有碳的模型系统中进行了研究,该系统由氯化铜 (CuCl(2)) 激活。使用了五种类型的碳(活性炭、三种类型的炭黑和石墨)来测试我们结果的普遍性。还研究了 SO(2) 对铜化合物的形态和行为、碳的催化氧化以及有机氯(可提取有机氯和不可提取有机氯)形成的影响,以研究 SO(2) 对新型合成的抑制机制。结果发现,SO(2) 可以硫酸盐化 CuCl(2),但不与 CuO 和 CuCl(2)反应。在 300°C 的 10% O(2)/N(2)气氛中与 CuO 反应。SO(2)对有机氯 (C-Cl) 形成的抑制也证实了这一点。还发现 SO(2) 强烈抑制了碳的催化氧化。在所有五种碳中,添加 SO(2)时,PCDD/Fs 的形成明显减少,而平均氯化水平也降低了。然而,与 PCDD/F 相比,对 PCB 的抑制作用不太明显。基于实验结果,提出了将一价和二价氯化铜转化为非反应性硫酸盐的转化作为抑制机制。