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Ni-catalyzed dry reforming of methane is usually subjected to coke-induced instability due to an epitaxial lattice match between carbon and Ni step edge that stabilizes the carbon nucleus. Herein, we propose an innovative strategy through coupling Ni step-edge sites with N-heteroatoms to prevent the carbon nucleation. The N-heteroatoms preferentially are coupled at the Ni step sites, and the coupling effect attenuates the generation and adsorption of carbon intermediates via directionally regulating the d-band center of Ni-atoms around the step sites and further inhibits the carbon nucleation and growth. Moreover, the Ni step sites with N coverage accelerate the gasification rate of carbon with CO2, which further restrains the carbon deposition and substantially improves the catalytic stability for methane dry reforming.
Guo et al. (Wed,) studied this question.