The dry reforming of methane (DRM) is a new potential technology that converts two major greenhouse gases into useful chemical feedstocks. The main challenge faced by this process is maintaining the catalyst with high catalytic activity and long-term stability. Here, a simple and effective preparation route for the synthesis of functional nanomolecular sieve catalysts (NiRu x CZZ5) from kaolinite tailings was developed for dry reforming of methane with CO 2 . The silica monoliths with flower-like spherical and micropore structures (ZSM-5) were prepared by crystal growth method, and the metal components were loaded by ultrasonic-assisted impregnation method. The NiRu 0.5 CZZ5 catalyst exhibited excellent catalytic performance (maxmium CO 2 and CH 4 conversions up to 100 and 95.6%, respectively) and very good stability (up to 100h). The interfacial confinement and the strong support interaction are principally responsible for the excellent catalytic activity of the catalyst. The in situ DRIFTS was used to elucidate the possible carbon conversion steps, and stable surface intermediates were also identified.
In
this work, a Ni-based catalyst supported on a core–shell
structure catalytic carrier material (Ni/ZSM-5@MCM-41) based on kaolinite
tailings is reported, which exhibits excellent CO2 methanation
performance at atmospheric pressure. At 400 °C, CO2 conversion and CH4 selectivity reach 80 and 97% with
the space velocity of 12,000 mL gcat
–1 h–1, respectively, and it can maintain good stability
during the 80 h stability test. Compared with traditional Ni/ZSM-5
and Ni/MCM-41 catalysts, Ni/ZSM-5@MCM-41 has more substantial confinement
effects on the active components, and the active components are more
evenly dispersed on surface of the carrier. In addition, it is confirmed
by the in situ diffuse reflectance infrared Fourier
transform spectroscopy technique that CO2 methanation over
the Ni/ZSM-5@MCM-41 catalyst follows the path of formate and CO as
intermediates.
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