4.7 Article

Nitrogen migration in coal during the chemical looping gasification reduction process using a nickel-based oxygen carrier

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出版社

ELSEVIER
DOI: 10.1016/j.jaap.2021.105331

关键词

Coal; Chemical looping gasification; Nickel-based oxygen carrier; thermogravimetric-mass spectrometry; Gas-phase nitrogen; Solid-phase nitrogen

资金

  1. national key research and development program project [2018YFB0605403-04]
  2. key research and development program of ningxia province of China [2018BCE01002, 2016BY005, 2018BEE03009]
  3. national natural science foundation of China [21868025]
  4. national key research and development program of China [2018YFB0605401]
  5. national academic subjects construction project of ningxia [NXYLXK2017A04]
  6. natural science foundation project of ningxia [2020AAC03020]

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The study found that the distribution and migration of nitrogen during chemical looping gasification may be influenced by different temperature stages and the addition of an oxygen carrier. Nitrogen primarily exists in both solid and gas phases during low-temperature stages, with the addition of an oxygen carrier at high temperatures benefiting the decomposition of nitrogen precursors.
The release of nitrogen from a chemical looping gasification (CLG) system has always been a great concern. In this work, the thermal reactivity of samples obtained from the Jinfeng district, which were involved in the CLG process, was investigated via thermogravimetric-mass spectrometric (TG-MS) analysis. The migration mechanism of gas-phase nitrogen was characterized online, and changes in solid-phase nitrogen were analyzed during different stages using X-ray photoelectron spectroscopy. Results showed that nitrogen mainly existed in the solid and gas phases during different temperature stages of CLG; however, its migration varied at different stages. During the low-temperature pyrolysis stage (320 degrees C-795 degrees C, without adding steam), the addition of a nickel-based oxygen carrier accelerated the decomposition of the aliphatic structure and increased the hydroxyl content in the sample. Further, the release of nitrogen precursors was promoted by the accelerated release of hydrogen-containing free radicals from the aliphatic structure. The interaction between the nitrogen precursor and hydroxyl structure induced NO release at 350 degrees C. During the high-temperature pyrolysis stage (795 degrees C-950 degrees C, without adding steam), the reaction between the oxygen carrier and char exposed protic pyridine (N-Q) in the macromolecular structure. Furthermore, during the gasification stage (670 degrees C-950 degrees C, with steam addition), the addition of the oxygen carrier decreased the degree of graphitization of char and enhanced its gasification performance. As the structural units of char became smaller, N-Q in its macromolecular structure underwent further decomposition. Thus, the addition of the oxygen carrier at high temperatures benefited N-Q decomposition.

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