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In situ tuning of the electronic structure of active sites is a long-standing challenge. Herein, we propose a strategy by controlling the hydrogen spillover distance to in situ tune the electronic structure. The strategy is demonstrated to be feasible with the assistance of CoO  x  /Al 2 O 3 /Pt catalysts prepared by atomic layer deposition in which CoO  x   and Pt nanoparticles are separated by hollow Al 2 O 3  nanotubes. The strength of hydrogen spillover from Pt to CoO  x   can be precisely tailored by varying the Al 2 O 3  thickness. Using CoO  x  /Al 2 O 3  catalyzed styrene epoxidation as an example, the CoO  x  /Al 2 O 3 /Pt with 7 nm Al 2 O 3  layer exhibits greatly enhanced selectivity (from 74.3% to 94.8%) when H 2  is added. The enhanced selectivity is attributed to the introduction of controllable hydrogen spillover, resulting in the reduction of CoO  x   during the reaction. Our method is also effective for the epoxidation of styrene derivatives. We anticipate this method is a general strategy for other reactions.

In situ tuning of electronic structure of catalysts using controllable hydrogen spillover for enhanced selectivity