Harun Khalida, Adhikari Sushil, Jahromi Hossein
Department of Biosystems Engineering, Auburn University Auburn Alabama 36849 USA
Center for Bioenergy and Bioproducts, Auburn University Auburn Alabama 36849 USA.
RSC Adv. 2020 Nov 10;10(67):40882-40893. doi: 10.1039/d0ra07440c. eCollection 2020 Nov 9.
Thermocatalytic decomposition (TCD) of methane is one of the most effective methods for pure hydrogen production. Catalysts were selected for TCD of methane in this study to utilize biochar as a catalyst. Among these catalysts, two catalysts (named activated biochar (AB) and heat-treated biochar (HB)) were prepared from Douglas fir, whereas the other four were prepared using commercial activated carbon and zeolite with and without doping ruthenium metal. The catalysts were characterized using XRD, SEM imaging, TEM, H-TPR, and BET specific surface area and pore size analysis. The Ru doped commercial activated carbon catalyst (Ru-AC) was deactivated continuously during a 60 h reaction run, whereas AB exhibited comparatively stable methane conversion up to 60 h. The methane conversion was 21% for Ru-AC and 51% for AB after 60 h of reaction time at 800 °C. The very high surface area of AB (∼3250 m g) and its microporosity compared to other catalysts could have resulted in resistance against rapid deactivation. Furthermore, carbon nanotube by-products were observed in TEM images of solid residues that could form due to the presence of alkali metals in the biochar. Carbon nanotube formation could contribute significantly to the extended life of AB.
甲烷的热催化分解(TCD)是制取纯氢最有效的方法之一。本研究选择催化剂用于甲烷的热催化分解,以利用生物炭作为催化剂。在这些催化剂中,两种催化剂(分别命名为活性生物炭(AB)和热处理生物炭(HB))由花旗松制备,而另外四种则使用商业活性炭和沸石制备,其中部分掺杂了钌金属。使用X射线衍射(XRD)、扫描电子显微镜成像(SEM)、透射电子显微镜(TEM)、氢气程序升温还原(H-TPR)以及BET比表面积和孔径分析对催化剂进行了表征。在60小时的反应过程中,掺杂钌的商业活性炭催化剂(Ru-AC)持续失活,而AB在长达60小时的时间内表现出相对稳定的甲烷转化率。在800℃反应60小时后,Ru-AC的甲烷转化率为21%,AB的甲烷转化率为51%。与其他催化剂相比,AB极高的比表面积(约3250 m²/g)及其微孔结构可能使其具有抗快速失活的能力。此外,在固体残渣的TEM图像中观察到了碳纳米管副产物,这些副产物可能是由于生物炭中存在碱金属而形成的。碳纳米管的形成可能对AB的使用寿命延长有显著贡献。