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Reforming of Tar Model Compounds over Sustainable and Low-cost Biochar: Special Focus on Spontaneous Gasification Reactivity and Tar Reforming Kinetics for Reformer Design
Chemical Engineering Journal ( IF 15.1 ) Pub Date : 2020-10-16 , DOI: 10.1016/j.cej.2020.127350
Yen–Hau Chen , Ashak Mahmud Parvez , Max Schmid , Günter Scheffknecht

In this study, the spontaneous gasification and catalytic activity of wood char were experimentally evaluated in simulated sorption enhanced gasification (SEG) environments with toluene and naphthalene as tar model compounds. Besides, CaO was used as a reference catalyst for the comparison purpose since CaO is a commonly used sorbent in the SEG process. A model of gasification reactivity during reforming of tar model compounds over wood char was developed in this work based on the reactivity at 20 % carbon conversion adopting the Extended Random Pore Model, where the pre-exponential factor, activation energy, and structural parameter were calculated to be 1.65·1010 min-1, 265.8 kJ mol-1, and 127, respectively. During the catalytic activity investigation, hydrogen was found to inhibit tar-reforming performance over CaO while the impact of hydrogen was insignificant over wood char. The results showed that spontaneous gasification during tar surrogates reforming led to mass loss, pore collapse, and inorganics agglomeration, which contributed to the catalytic deactivation of wood char. By considering gasification-caused deactivation, the carbon conversion was then used as a variable to modify the kinetic equations of the tar surrogates reforming. The activation energy and pre-exponential factor of naphthalene reforming (and toluene reforming) over wood char were calculated with the values of 422.5 kJ mol-1 and 2.92·1022 m3 kg-1 h-1 (284.8 kJ mol-1 and 1.90·1015 m3 kg-1 h-1), respectively, whereas the values for CaO were 126.9 kJ mol-1 and 6.79·104 m3 kg-1 h-1 (254.5 kJ mol-1 and 6.73·1011 m3 kg-1 h-1), respectively. The kinetic models developed in this study were later used for designing a tar reformer integrated with the SEG process.



中文翻译:

可持续和低成本生物炭上焦油模型化合物的重整:特别关注自发气化反应性和重整器设计的焦油重整动力学

在这项研究中,以甲苯和萘为焦油模型化合物,在模拟吸附增强气化(SEG)环境中,通过实验评估了木炭的自发气化和催化活性。此外,由于CaO是SEG工艺中常用的吸附剂,因此CaO被用作参考催化剂以进行比较。在这项工作的基础上,采用扩展随机孔模型,在20%碳转化率下的反应性的基础上,开发了焦油模型化合物在木炭上重整时的气化反应性模型,其中计算了前指数因子,活化能和结构参数为1.65×10 10分钟-1,265.8千焦耳摩尔-1,和127。在催化活性研究中,发现氢抑制了CaO的焦油重整性能,而氢对木炭的影响则微不足道。结果表明,焦油替代物重整过程中的自发气化导致质量损失,孔塌陷和无机物团聚,这有助于木炭的催化失活。通过考虑气化引起的失活,然后将碳转化率用作变量来修改焦油替代物重整的动力学方程式。计算得出木炭上萘重整(和甲苯重整)的活化能和指数前因子为422.5 kJ mol -1和2.92·10 22 m 3 kg -1h -1(分别为284.8 kJ mol -1和1.90·10 15 m 3 kg -1 h -1),而CaO值为126.9 kJ mol -1和6.79·10 4 m 3 kg -1 h -1(分别为254.5 kJ mol -1和6.73·10 11 m 3 kg -1 h -1)。在这项研究中开发的动力学模型后来用于设计与SEG工艺集成的焦油重整器。

更新日期:2020-10-17
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