Department of Biochemical Engineering, Seoul University, 28, Yongmasan-ro 90-gil, Jungnang-gu, Seoul 02192, Republic of Korea.
Department of Chemical & Biological Engineering, Hanbat National University, Daejeon 34158, Republic of Korea.
Int J Mol Sci. 2023 Jul 22;24(14):11793. doi: 10.3390/ijms241411793.
The removal of nitrogen from coal tar pitch (CTP) through the hydrodenitrogenation (HDN) of CTP and its molecular behavior were evaluated in the presence of NiMo/γ-alumina and CoMo/γ-alumina catalysts. Fourier transform ion cyclotron resonance mass spectrometry with atmospheric pressure photoionization was used to analyze the complicated chemical classes and species of CTP and the treated products at the molecular level. Nitrogen species were qualitatively analyzed before and after hydrotreatment. A single-stage hydrotreatment with an HDN catalyst resulted in a high sulfur removal performance (85.6-94.7%) but a low nitrogen removal performance (26.8-29.2%). Based on relative abundance analyses of nitrogen and binary nitrogen species, CH-NS was the most challenging species to remove during HDN treatment. Furthermore, prior hydrodesulfurization was combined with HDN treatment, and the dual hydrotreatments yielded a significantly improved nitrogen removal performance (46.4-48.7%).
通过 NiMo/γ-氧化铝和 CoMo/γ-氧化铝催化剂对煤焦油沥青(CTP)进行加氢脱氮(HDN),评估了从 CTP 中脱除氮以及其分子行为。采用大气压光离子化傅里叶变换离子回旋共振质谱法在分子水平上分析了 CTP 和处理产物的复杂化学类和物质。在加氢处理前后对氮化物进行了定性分析。采用单段加氢处理,HDN 催化剂具有较高的脱硫性能(85.6-94.7%),但脱氮性能较低(26.8-29.2%)。基于氮和双氮物质的相对丰度分析,CH-NS 是 HDN 处理过程中最难去除的物质。此外,先进行加氢脱硫处理,再进行 HDN 处理,双加氢处理可显著提高脱氮性能(46.4-48.7%)。