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Engineering Crystal Facet of α‑MnO2 Nanowire for Highly Efficient Catalytic Oxidation of Carcinogenic Airborne Formaldehyde

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journal contribution
posted on 2018-03-14, 00:00 authored by Shaopeng Rong, Pengyi Zhang, Fang Liu, Yajie Yang
The activity of exposed crystal facets directly determines its physicochemical properties. Thus, acquiring a high percentage of reactive facets by crystal facet engineering is highly desirable for improving the catalytic reactivity. Herein, single-crystalline α-MnO2 nanowires with major exposed high-index {310} facets were synthesized via a facile hydrothermal route with the assistance of a capping agent of oxalate ions. Comparing with two other low-index facets ({100} and {110}), the resulting α-MnO2 nanowires with exposed {310} facets exhibited much better activity and stability for carcinogenic formaldehyde (HCHO) oxidation, making 100% of 100 ppm of HCHO mineralize into CO2 at 60 °C, even better than some Ag supported catalysts. The density functional theory (DFT) calculations were used to investigate the difference in the catalytic activity of α-MnO2 with exposed {100}, {110}, and {310} facets. The experimental characterization and theoretical calculations all confirm that the {310} facets with high surface energy can not only facilitate adsorption/activation of O2 and H2O but also be beneficial to the generation of oxygen vacancies, which result in significantly enhanced activity for HCHO oxidation. This is a valuable report on engineering surface facets in the preparation of α-MnO2 as highly efficient oxidation catalysts. This study deepens the understanding of facet-dependent activity of α-MnO2 and points out a strategy to improve their catalytic activity by crystal facet engineering.

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