Deciphering transient carbon footprint for methane dry reforming over Ni@S-1 nanosheet zeolite catalyst
Carbon deposition, an inevitable product operated at high temperatures, is a headache-inducing obstacle to enhance catalyst stability for methane dry reforming (MDR). Herein, we have ingeniously designed sintering-resistant Ni@S-1 nanosheet zeolites to purposefully induce common linear and non-linear deactivation of catalysts during MDR reaction for deciphering carbon footprint. Multiple evidences unveiled that "transient carbon", composed of multi-phenyl-rings via rapidly rearrangement of CH x * fragments, was a crucial vane for catalyst deactivation. Accordingly, we proposed a dynamic equilibrium theory for the generation and elimination of "transient carbon". Achieving this balance was dependent of the matching degree between Ni 0 nanoparticles and NiO x (OH) y , which both separately originated from the evolutions of 1:1 and 2:1 Ni phyllosilicates controlled by nanosheet thickness. Delightfully, synthetic Ni@S-1–60nm catalyst with an optimal ratio of Ni 0 /NiO x (OH) y contributed higher MDR activity and durability. These findings derived a new MDR reaction pathway and afforded value-filled information for developing high carbon-resistant MDR catalysts.
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