Theoretical investigation of the formation mechanism of NH3 and HCN during pyrrole pyrolysis

the effect of H2O

Ji Liu, Qiang Lu, Xiao-yan Jiang, Bin Hu, Xiao-lei Zhang, Chang-qing Dong, Yong-ping Yang

Research output: Contribution to journalArticle

2 Citations (Scopus)

Abstract

Coal is a major contributor to the global emission of nitrogen oxides (NOx). The NOx formation during coal utilization typically derives from the thermal decomposition of N-containing compounds (e.g., pyrrolic groups). NH3 and HCN are common precursors of NOx from the decomposition of N-containing compounds. The existence of H2O has significant influences on the pyrrole decomposition and NOx formation. In this study, the effects of H2O on pyrrole pyrolysis to form NOx precursors HCN and NH3 are investigated using the density functional theory (DFT) method. The calculation results indicate that the presence of H2O can lead to the formation of both NH3 and HCN during pyrrole pyrolysis, while only HCN is formed in the absence of H2O. The initial interaction between pyrrole and H2O determines the N products. NH3 will be formed when H2O attacks the C2 position of pyrrole with its hydroxyl group. On the contrary, HCN will be generated instead of NH3 when H2O attacks the C3 position of pyrrole with its hydroxyl group. In addition, the DFT calculations clearly indicate that the formation of NH3 will be promoted by H2O, whereas the formation of HCN is inhibited
Original languageEnglish
Article number711
Number of pages11
JournalMolecules
Volume23
Issue number4
DOIs
Publication statusPublished - 21 Mar 2018

Fingerprint

Pyrroles
Nitrogen Oxides
pyrroles
nitrogen oxides
pyrolysis
Pyrolysis
Coal
Hydroxyl Radical
attack
Density functional theory
coal utilization
density functional theory
Decomposition
decomposition
coal
thermal decomposition
Hot Temperature
products

Keywords

  • pyrrole pyrolysis
  • H2O
  • NOx precursor
  • NH3
  • HCN
  • DFT

Cite this

Liu, Ji ; Lu, Qiang ; Jiang, Xiao-yan ; Hu, Bin ; Zhang, Xiao-lei ; Dong, Chang-qing ; Yang, Yong-ping. / Theoretical investigation of the formation mechanism of NH3 and HCN during pyrrole pyrolysis : the effect of H2O. In: Molecules. 2018 ; Vol. 23, No. 4.
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abstract = "Coal is a major contributor to the global emission of nitrogen oxides (NOx). The NOx formation during coal utilization typically derives from the thermal decomposition of N-containing compounds (e.g., pyrrolic groups). NH3 and HCN are common precursors of NOx from the decomposition of N-containing compounds. The existence of H2O has significant influences on the pyrrole decomposition and NOx formation. In this study, the effects of H2O on pyrrole pyrolysis to form NOx precursors HCN and NH3 are investigated using the density functional theory (DFT) method. The calculation results indicate that the presence of H2O can lead to the formation of both NH3 and HCN during pyrrole pyrolysis, while only HCN is formed in the absence of H2O. The initial interaction between pyrrole and H2O determines the N products. NH3 will be formed when H2O attacks the C2 position of pyrrole with its hydroxyl group. On the contrary, HCN will be generated instead of NH3 when H2O attacks the C3 position of pyrrole with its hydroxyl group. In addition, the DFT calculations clearly indicate that the formation of NH3 will be promoted by H2O, whereas the formation of HCN is inhibited",
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author = "Ji Liu and Qiang Lu and Xiao-yan Jiang and Bin Hu and Xiao-lei Zhang and Chang-qing Dong and Yong-ping Yang",
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Theoretical investigation of the formation mechanism of NH3 and HCN during pyrrole pyrolysis : the effect of H2O. / Liu, Ji; Lu, Qiang; Jiang, Xiao-yan; Hu, Bin; Zhang, Xiao-lei; Dong, Chang-qing; Yang, Yong-ping.

In: Molecules, Vol. 23, No. 4, 711, 21.03.2018.

Research output: Contribution to journalArticle

TY - JOUR

T1 - Theoretical investigation of the formation mechanism of NH3 and HCN during pyrrole pyrolysis

T2 - the effect of H2O

AU - Liu, Ji

AU - Lu, Qiang

AU - Jiang, Xiao-yan

AU - Hu, Bin

AU - Zhang, Xiao-lei

AU - Dong, Chang-qing

AU - Yang, Yong-ping

PY - 2018/3/21

Y1 - 2018/3/21

N2 - Coal is a major contributor to the global emission of nitrogen oxides (NOx). The NOx formation during coal utilization typically derives from the thermal decomposition of N-containing compounds (e.g., pyrrolic groups). NH3 and HCN are common precursors of NOx from the decomposition of N-containing compounds. The existence of H2O has significant influences on the pyrrole decomposition and NOx formation. In this study, the effects of H2O on pyrrole pyrolysis to form NOx precursors HCN and NH3 are investigated using the density functional theory (DFT) method. The calculation results indicate that the presence of H2O can lead to the formation of both NH3 and HCN during pyrrole pyrolysis, while only HCN is formed in the absence of H2O. The initial interaction between pyrrole and H2O determines the N products. NH3 will be formed when H2O attacks the C2 position of pyrrole with its hydroxyl group. On the contrary, HCN will be generated instead of NH3 when H2O attacks the C3 position of pyrrole with its hydroxyl group. In addition, the DFT calculations clearly indicate that the formation of NH3 will be promoted by H2O, whereas the formation of HCN is inhibited

AB - Coal is a major contributor to the global emission of nitrogen oxides (NOx). The NOx formation during coal utilization typically derives from the thermal decomposition of N-containing compounds (e.g., pyrrolic groups). NH3 and HCN are common precursors of NOx from the decomposition of N-containing compounds. The existence of H2O has significant influences on the pyrrole decomposition and NOx formation. In this study, the effects of H2O on pyrrole pyrolysis to form NOx precursors HCN and NH3 are investigated using the density functional theory (DFT) method. The calculation results indicate that the presence of H2O can lead to the formation of both NH3 and HCN during pyrrole pyrolysis, while only HCN is formed in the absence of H2O. The initial interaction between pyrrole and H2O determines the N products. NH3 will be formed when H2O attacks the C2 position of pyrrole with its hydroxyl group. On the contrary, HCN will be generated instead of NH3 when H2O attacks the C3 position of pyrrole with its hydroxyl group. In addition, the DFT calculations clearly indicate that the formation of NH3 will be promoted by H2O, whereas the formation of HCN is inhibited

KW - pyrrole pyrolysis

KW - H2O

KW - NOx precursor

KW - NH3

KW - HCN

KW - DFT

U2 - 10.3390/molecules23040711

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JO - Molecules

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