Anti-Exfoliation and Stable Ni@S1@SiC Catalysts by In Situ Crystallization for Electrothermal Dry Reforming of Methane.

Alkane utilization via direct cleavage of C─H bonds is highly industrially relevant yet is practically limited by high endothermicity. Electrothermal catalysis addresses this challenge by delivering internal Joule heating through the catalyst, offering direct, and efficient heat supply. However, the severe exfoliation related to the interfacial temperature gradient causes irreversible deactivation, severely limiting the applicability of electrothermal catalysis for industrial application. In this study, we developed an in situ crystallization strategy to fabricate a robust structured catalyst based on foamed silicon carbide (Ni@S1@SiC) that overcomes this limitation. This is achieved via hydrothermal crystallization of Ni-embedded zeolite directly on the SiC foam, resulting in a homogeneously grown and intimately bonded zeolite layer. The in situ crystallized Ni@S1@SiC exhibits weight losses of less than 5 wt% in harsh exfoliation tests, much lower than the conventional washcoated catalyst (45.4%-91.8%). The durability of Ni@S1@SiC was exemplified in electrothermal dry reforming of methane (EDRM), presenting stable operation at 800°C at high conversions (93.2% for CH4 and 97.3% for CO2) and exfoliation of merely 3.6 wt%. This work provides a universal design principle for developing stable electrothermal catalysts, addressing the severe deactivation issue by exfoliation and paving the way for industrial application in endothermic reactions.