煤热解与甲烷蒸汽重整耦合过程焦油在碳基镍催化剂上的原位催化提质

• 作 者: 王政委 魏宝勇 吕剑楠 王一鸣 武云飞 杨赫 胡浩权
• 机 构: 大连理工大学化工学院煤化工研究所,精细化工国家重点实验室,辽宁大连116024
• 出 处: 燃料化学学报
• 发表日期: 2022年2期
• 关键词: coalpyrolysis catalyticupgrading tar steamreformingofmethane isotopetracer

本研究采用Ni/KD-9催化剂,对CP-SRM过程焦油进行原位催化提质研究.结果表明,在650℃热解温度下,CP-SRM在5Ni/KD-9催化作用下的焦油产率为24.4％,略低于不进行催化提质的焦油产率,而轻质焦油产率(18.9％)是未提质时的1.4倍.相比未提质焦油,用5Ni/KD-9提质后焦油中的C2、C3和C4烷基取代苯含量分别增加0.5、0.6和4.0倍;酚和萘的含量也明显提高.采用同位素示踪方法结合典型组分质谱图,探究了催化提质过程的反应机理.结果表明,5Ni/KD-9可以同时催化焦油裂解和甲烷蒸汽重整(SRM),SRM过程产生的小分子自由基,如·CHx,·H和·OH可以与焦油裂解产生的自由基结合,从而避免焦油的过度裂解.“,”In order to improve the tar quality by decreasing the heavy tar content and ensuring high tar yield, in-situ catalytic upgrading of tar from the integrated process of coal pyrolysis coupled with steam reforming of methane was conducted over carbon (KD-9) based Ni catalyst. The results show that at 650 ℃, the tar yield of CP-SRM over 5Ni/KD-9 is 24.4％, which is a little lower than that of without catalyst, while the light tar yield (i.e.,18.9％) is 1.4 times higher than that of without catalyst, and the content of C2, C3 and C4 alkyl used as a substitute for benzene significantly increases tar yields by 0.5, 0.6 and 4.0 times, respectively. The content of phenols and naphthalenes in tar also increases dramatically after upgrading. Isotope tracer approach combined with the mass spectra of typical components was employed in exploring the mechanism of the upgrading process. The results show that 5Ni/KD-9 catalyzes coal tar cracking and SRM at the same time. Small free radicals such as ·CHx, ·H and ·OH generated by SRM can combine with free radicals from tar cracking, thus avoiding excessive cracking of tar.