Study on NH_3 and HCN formation mechanisms during rapid pyrolysis of pyrrolic nitrogen
Study on NH_3 and HCN formation mechanisms during rapid pyrolysis of pyrrolic nitrogen
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发表时间：
2011
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通讯作者：
W. Fuchen
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作者：
W. Fuchen
根据煤中吡咯与其他杂环化合物结合形式的不同，选取了5种典型的吡咯-氮化合物作为研究对象。计算了这5种吡咯-氮化合物及其中间热解产物的Mayer键序。通过对Mayer键序的比较，推导了热解过程中键的裂解过程，并分析了热解过程中NH3和HCN的形成机理。结果表明：硝基氮在nh和nh2自由基中释放，主要形成NH3；吡咯循环与其他循环组合形式的多样性导致氮素释放过程的多样性。为了验证计算结论，在液滴式高频炉中对吡咯和咔唑进行了快速热解。实验结果表明，吡咯和咔唑在热解过程中同时生成NH3和HCN，但NH3是主要的含氮气态产物。计算得出的结论可以得到实验结果的支持。
5 typical pyrrolic-nitrogen compounds were chosen as the investigating objects according to the different pyrrole cycle combination forms with other heterocycles in coal.The Mayer bond orders of these 5 pyrrolic-nitrogen compunds and their intermediate pyrolysis products were calculated.By comparing the Mayer bond orders,the bonds cracking during pyrolysis were deduced,and NH3 and HCN formation mechanisms during pyrrolic-N pyrolysis were analyzed consequently.The results show that the pyrrolic-nitrogen is released in-NH and-NH2 free radicals,which mainly form NH3.The diversity of pyrrole cycles combination forms with other cycles can lead to the variety of nitrogen release processes.To verify the conclusions from calculation,the rapid pyrolysis of pyrrolic-N model compounds pyrrole and carbazole was carried out in a drop style high frequency furnace.The experiment results show that both NH3 and HCN are formed during pyrolysis of pyrrole and carbazole,but NH3 is the main nitrogen containing gaseous product.The conclusions deduced from calculation can get some supports from the experiment results.