Because of the recent global warming environmental issues,
dry
reforming of methane (DRM)which converts greenhouse gases
(CO2 and CH4) into syngases (CO and H2)is receiving significant attention. Recently, density functional
theory (DFT) calculations have been effectively used to obtain fundamental
information on DRM reactions. The DFT calculations can provide valuable
theoretical knowledge in various heterogeneous catalyst systems, which
is difficult to derive from experiments alone due to the complexity
of reaction pathways. This work introduces theoretical studies concerning
the most plausible reaction pathways, catalytic activities, and stabilities
of Ni- and non-Ni-based metal catalysts. The review includes fundamental
analyses of reaction mechanisms, catalytic activities, and several
strategies to improve the catalytic properties of Ni- and non-Ni-based
catalysts. Such strategies include doping, introducing promoters,
forming bimetallics, and utilizing various catalyst supports. In addition,
DFT-based descriptors provide guidelines for DRM catalyst design in
terms of activity and stability. In conclusion, this review also suggests
DFT-based analyses of catalysts based on morphological and compositional
engineering, such as core–shell nanoparticles, single-atom
catalysts, phosphides, and reduced solid solution catalysts. Finally,
this review suggests a rational catalyst design for DRM by tuning
catalytic properties based on engineered catalyst characteristics
under a comprehensive understanding provided by DFT calculations and
experiments.