Ammonia (NH3)/nitrogen (N2) torrefaction pretreatment of waste biomass for the production of renewable nitrogen-containing chemicals via catalytic ammonization pyrolysis: Evolution of fuel-N under a N2/NH3-rich atmosphere

加热 生物炭 化学 除氧 热解 氮气 燃烧热 傅里叶变换红外光谱 热重分析 催化作用 核化学 材料科学 化学工程 有机化学 燃烧 工程类
作者
Yunwu Zheng,Donghua Li,Jida Wang,Yifei Chen,Can Liu,Yi Lu,Xu Lin,Bohan Lv,Jirong Li,Zhifeng Zheng
出处
期刊:Journal of The Energy Institute [Elsevier BV]
卷期号:102: 143-159 被引量:51
标识
DOI:10.1016/j.joei.2022.03.011
摘要

To investigate the nitrogen migration and transformation mechanisms that produce high value-added N-containing chemicals, the NH 3 /N 2 torrefaction pretreatments of waste biomass for the production of renewable N-containing compounds were explored, and the effects of torrefaction temperature (200, 225, 250, 275, 300 °C) on fuel properties, structure, crystallinity, surface functional groups and thermal kinetics were evaluated by element analysis, X-ray diffraction (XRD), scanning electron microscopy (SEM), fourier infrared spectroscopy (FTIR) and thermogravimetric analysis (TG-DTG). The effects of subsequent catalytic ammonization pyrolysis upgrading of the torrefied biomass with Co/HZSM-5/HZSM-5 catalysts under an NH 3 /N 2 atmosphere on product yield and N-containing compound selectivity were also evaluated with GC/MS and UV-fluorescence spectrometry. Furthermore, nitrogen fixation and migration mechanisms were also proposed in depth. The results showed that NH 3 torrefaction was more effective in enhancing N fixation and retarding the release of N-containing volatiles in torrefied biochar (0.26%–9.43%) and reducing the oxygen content (43.18%–21.81%) via Maillard reactions compared with N 2 torrefaction. With increasing torrefaction severity, the N-containing compound content, higher heating values (HHV), deoxygenation ratio (DEO) and nitrogen-doping ratio (NDR) increased, which were much higher than those of conventional N 2 torrefaction. Higher temperatures promoted the evolution of graphitic-N and oxidized-N and reduced pyrrolic-N and pyridinic-N group formation in torrefied biochar. The maximum content of N-containing compounds of 88.71% was obtained at a torrefaction temperature of 275 °C under NH 3 pyrolysis coupled with the Co/HZSM-5 catalyst, and was achieved via substrate interaction with the -Co-O-Si- catalyst sites and Maillard reactions. Furthermore, the N 2 atmosphere combined with the HZSM-5 catalyst significantly promoted the conversion of HC compounds (∼56.97% at 225 °C during N 2 torrefaction), while the Co/HZSM-5 catalyst combined with the NH 3 atmosphere significantly improved N-containing compound formation. NH 3 pyrolysis facilitated the formation of pyrroles and pyrazines while reducing the formation of amides by deamination and dehydrogenation reactions. Cellulose was conducive to the transformation of pyrrole in NH 3 pyrolysis, while lignin was conducive to the formation of aniline. These results could offer strategies to regulate nitrogen functional groups to enhance N-containing chemicals. • A novel N-containing chemicals production method was developed with NH 3 torrefaction and pyrolysis. • Nitrogen fixation and migration mechanism in solid-gas-liquid phase was proposed. • Higher torrefaction temperature promoted the formation of N-containing compounds under NH 3 atmosphere. • The maximum yield of N-containing chemicals in bio-oil was 88.71%. • NH 3 pyrolysis coupling with Co/HZSM-5was facilitating to production of pyrroles and pyrazines.
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