Low-Temperature Catalytic Dry Reforming of Methane over Pd Promoted Ni–CaO–Ca₁₂Al₁₄O₃₃ Multifunctional Catalyst

Abstract

The dry reforming of methane (DRM) suffers from high energy consumption and catalyst deactivation over time on stream at high operating temperatures (>800 °C). Here, we demonstrate that DRM is effectively catalyzed at 600 °C by Pd promoted Ni–CaO–Ca12Al14O33 multifunctional adsorbent/catalyst materials with 67% CO2 conversion, 68% CH4 conversion, and a H2/CO ratio close to unity. Notably, the catalyst shows no sign of deactivation at 600 °C for a 50 h continuous on-stream DRM reaction. The high performance is ascribed to the enhanced CH4 dissociation activity with the presence of Pd. CH4 reformed with CaCO3 achieved the transformation between bulk CaCO3 and nanoparticles of CaO. The dynamic transformation may allow for reversible encapsulation and release of Ni particles, thereby suppressing Ni sintering. Furthermore, the coke formed on the catalyst is mainly the active carbon species which is easily removed by CO2 and CaCO3, thus ensuring the long-term stability. The results demonstrated herein shed light on a new paradigm to design low-temperature DRM reaction catalysts.

Preparation of Vermiculite‐based Molecular Sieve‐Supported Ni‐Co Alloy Catalyst Assisted by Oleic Acid and Application in Dry Reforming of Methane

“…Unfortunately, during the high temperature reaction, nickel-based catalysts are prone to the phenomenon of sintering and coking, which can reduce the nickel active sites and lead to catalyst deactivation. Noble metals like Pt, [2] Ru, [3] Pd, [4] Rh [5] as the active metals can remarkably promote catalytic activity and effectively reduce the sintering degree of catalyst, but their expensive price and scarcity have substantially stunted industrial applications. [6] The synergistic effect between nickel and other transition metals has been reported in the relevant literature.…”