|Table of Contents|

Density Function Theory Studies on Reaction Mechanism of Organic Nitrogen during Coal Pyrolysis

《南京理工大学学报》(自然科学版)[ISSN:1005-9830/CN:32-1397/N]

Issue:
2008年02期
Page:
241-247
Research Field:
Publishing date:

Info

Title:
Density Function Theory Studies on Reaction Mechanism of Organic Nitrogen during Coal Pyrolysis
Author(s):
MENG Yun12JU Xue-hai1XIAO He-ming1
1.School of Chemical Engineering,NUST,Nanjing 210094,China;2.College of Teachers,Qingdao University,Qingdao 266071,China
Keywords:
density functional theory coal organic nitrogen pyrolysis mechanisms
PACS:
TQ530.2
DOI:
-
Abstract:
The models of pyridinic nitrogen and pyrrolic nitrogen in coals are predigested rationally.A reliable density functional theory(DFT) method at B3LYP/6-311++G** level is employed to investigate the reaction pathways of pyridine and pyrrole during coal pyrolysis.All the reactants,transition states and intermediates of the reaction paths are optimized.By comparing the bond Mulliken population,CN bond is found to be the initial bond for pyrolysis.Activation energies of two types of pyrrolic radicals and three types of pyridinic radicals are calculated.The activation energies of pyrrolic radicals are smaller than those of pyridinic radicals,so pyridine is more stable than pyrrole.All the calculated results are in agreement with the experimental results provided by the reference.

References:

[1] Thom asK M. The re lease o f n itrogen ox ides during char combustion [ J]. Fue,l 1997, 76 ( 6): 457- 473.
[2] LaughlinM K, Gav in D G, Reed G P. Coa l and char n itrogen chem istry during pressurized flu id ized bed combustion [ J]. Fue,l 1994, 73 ( 7): 1 027- 1 033.
[3] 赵炜, 常丽萍, 谢克昌, 等. 煤燃烧过程生成氮氧化 物前驱体的研究[ J]. 燃料化学学报, 2004, 32( 4): 385- 388.
[4] 李芳芹, 魏敦崧, 马京程, 等. 燃煤锅炉空气分级燃 烧降低NO排放的数值模拟[ J]. 燃料化学学报, 2004, 32( 5): 537- 541.
[5] 曹欣玉, 牛志刚, 应凌俏, 等. 无烟煤燃料氮的热解 析出规律[ J]. 燃料化学学报, 2003, 31 ( 6) : 538 - 542.
[6] 王宝俊, 张玉贵, 谢克昌, 等. 量子化学计算方法在 煤反应性研究中的应用[ J]. 煤碳转化, 2003, 26 ( 1) : 1- 7.
[7] 肖继军, 张骥, 杨栋, 等. 环四甲撑四硝胺( HMX)结 构和性质的DFT研究[ J]. 化学物理学报, 2002, 15 ( 1) : 41- 45.
[8] Axw orthy A E, Dayan V H, M artin G B. Reactions o f fue-l nitrogen com pounds under cond itions of inert pyro lysis [ J]. Fue,l 1978, 57 ( 1) : 29- 35.
[9] N elson P F, M a rtin D, Ke lly P D, et a.l Convers ion of fue l n itrogen in coal vo la tiles to NOX precursors under rapid heating condition [ J ]. Fue,l 1991, 70 ( 3) : 403- 407.
[10] XuW C, Kum aga iM. N itrogen evo lution dur ing rap id hydropyro lysis of coa l [ J]. Fue,l 2002, 81 ( 18): 2 325- 2 334.
[11] Johnsson J E. Form a tion and reduction of fue l n itrogen ox ides in fluid ized-bed com bustion [ J]. Fue ,l 1994, 73 ( 3) : 1 398- 1 415.
[12] M arek A, Jan R, Jacob A. The fate of nitrogen functionalities in coal dur ing pyrolysis and combustion[ J]. Fue,l 1995, 74 ( 4): 507- 516.

Memo

Memo:
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Last Update: 2008-04-30