We have already proposed that a “Combinatorial Computational Chemistry” approach is very
effective for performing the theoretical high-throughput screening of new catalysts, and its validity
was strongly confirmed in various catalyst systems. In the present study, we applied our
combinatorial computational chemistry approach to the design of new metal sulfide catalysts for
the CO hydrogenation process and proposed new guidance for designing the highly selective
catalysts for methanol synthesis. We investigated H2 and CO adsorption on a large number of
metal and metal sulfide catalysts by first-principles calculations, and succeeded in clarifying the
relationship between the metal species in the metal and metal sulfide catalysts and the products
of the CO hydrogenation processes. Our results indicated that Co, Mo, Ru, Rh, Ir, and Pd sulfide
catalysts selectively produce methanol, while Re and Os sulfide catalysts selectively produce
hydrocarbons. The above results are in good agreement with the experimental results of Koizumi
and co-workers. Moreover, we proposed that the Pd sulfide catalyst has the highest selectivity
for methanol from the CO hydrogenation process. This result strongly supports the experimental
results by Koizumi and co-workers. Moreover, we propose that the metal sulfide catalysts, which
realize the bridge-site adsorption of the CO molecule on both the metal and sulfur atoms, have
high selectivity for methanol. This proposed guidance for designing the highly selective metal
sulfide catalysts for methanol may be useful for the experiments.