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In situ formation of cocatalytic sites boosts single-atom catalysts for nitrogen oxide reduction.

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Nitrogen oxide (NOx) pollution presents a severe threat to the environment and human health. Catalytic reduction of NOx with H2 using single-atom catalysts poses considerable potential in the remediation of… Click to show full abstract

Nitrogen oxide (NOx) pollution presents a severe threat to the environment and human health. Catalytic reduction of NOx with H2 using single-atom catalysts poses considerable potential in the remediation of air pollution; however, the unfavorable process of H2 dissociation limits its practical application. Herein, we report that the in situ formation of PtTi cocatalytic sites (which are stabilized by Pt-Ti bonds) over Pt1/TiO2 significantly increases NOx conversion by reducing the energy barrier of H2 activation. We demonstrate that two H atoms of H2 molecule are absorbed by adjacent Pt atoms in Pt-O and Pt-Ti, respectively, which can promote the cleave of H-H bonds. Besides, PtTi sites facilitate the adsorption of NO molecules and further lower the activation barrier of the whole de-NOx reaction. Extending the concept to Pt1/Nb2O5 and Pd1/TiO2 systems also sees enhanced catalytic activities, demonstrating that engineering the cocatalytic sites can be a general strategy for the design of high-efficiency catalysts that can benefit environmental sustainability.

Keywords: situ formation; nitrogen oxide; single atom; cocatalytic sites; atom catalysts; reduction

Journal Title: Proceedings of the National Academy of Sciences of the United States of America
Year Published: 2023

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