Simultaneous production of syngas and carbon nanotubes from CO2/CH4 mixture over high-performance NiMo/MgO catalyst
Nonthicha Sae-tang, Supanida Saconsint, Atthapon Srifa, Wanida Koo-amornpattana, Suttichai Assabumrungrat, Choji Fukuhara, Sakhon Ratchahat
Abstract
Abstract Direct conversion of biogas via the integrative process of dry reforming of methane (DRM) and catalytic methane decomposition (CDM) has received a great attention as a promising green catalytic process for simultaneous production of syngas and carbon nanotubes (CNTs). In this work, the effects of reaction temperature of 700–1100 °C and CH 4 /CO 2 ratio of biogas were investigated over NiMo/MgO catalyst in a fixed bed reactor under industrial feed condition of pure biogas. The reaction at 700 °C showed a rapid catalyst deactivation within 3 h due to the formation of amorphous carbon on catalyst surface. At higher temperature of 800–900 °C, the catalyst can perform the excellent performance for producing syngas and carbon nanotubes. Interestingly, the smallest diameter and the highest graphitization of CNTs was obtained at high temperature of 1000 °C, while elevating temperature to 1100 °C leads to agglomeration of Ni particles, resulting in a larger size of CNTs. The reaction temperature exhibits optimum at 800 °C, providing the highest CNTs yield with high graphitization, high syngas purity up to 90.04% with H 2 /CO ratio of 1.1, and high biogas conversion (X CH4 = 86.44%, X CO2 = 95.62%) with stable performance over 3 h. The typical composition biogas (CH 4 /CO 2 = 1.5) is favorable for the integration process, while the CO 2 rich biogas caused a larger grain size of catalyst and a formation of molybdenum oxide nanorods (MoO 3 ). The long-term stability of NiMo/MgO catalyst at 800 °C showed a stable trend (> 20 h). The experimental findings confirm that NiMo/MgO can perform the excellent activity and high stability at the optimum condition, allowing the process to be more promising for practical applications.