Abstract
Atomic-level insight into the unique catalytic capability of single-atom catalysts that distinguished from nanometer-sized counterparts is highly desirable for catalyst design and catalysis research. By synthesizing single Pd atoms supported on TiO2 as a catalyst, here we demonstrate a steric hindrance effect of single atoms induced by the unique isolation of single-atom active sites to achieve a remarkable enhancement on catalytic performance in the synthesis of dimethyl carbonate. Experimental results and density functional theory calculations reveal that such steric hindrance effect of single atoms favors the yield of the desired product dimethyl carbonate against further reacting with intermediates to form byproduct, because no extra Pd species around single Pd atoms provide active sites to further adsorb and activate substrates directly. The discovery of such steric hindrance effect is a valuable supplement to single-atom catalysis, and may promote single-atom catalysts to be widely applied in selective catalytic reactions.
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