Erschienen:
Springer Science and Business Media LLC, 2019
Erschienen in:
Nature Communications, 10 (2019) 1
Sprache:
Englisch
DOI:
10.1038/s41467-019-09918-z
ISSN:
2041-1723
Entstehung:
Anmerkungen:
Beschreibung:
<jats:title>Abstract</jats:title><jats:p>As diversified reaction paths exist over practical catalysts towards CO<jats:sub>2</jats:sub> hydrogenation, it is highly desiderated to precisely control the reaction path for developing efficient catalysts. Herein, we report that the ensemble of Pt single atoms coordinated with oxygen atoms in MIL-101 (Pt<jats:sub>1</jats:sub>@MIL) induces distinct reaction path to improve selective hydrogenation of CO<jats:sub>2</jats:sub> into methanol. Pt<jats:sub>1</jats:sub>@MIL achieves the turnover frequency number of 117 h<jats:sup>−1</jats:sup> in DMF under 32 bar at 150 °C, which is 5.6 times that of Pt<jats:sub>n</jats:sub>@MIL. Moreover, the selectivity for methanol is 90.3% over Pt<jats:sub>1</jats:sub>@MIL, much higher than that (13.3%) over Pt<jats:sub>n</jats:sub>@MIL with CO as the major product. According to mechanistic studies, CO<jats:sub>2</jats:sub> is hydrogenated into HCOO* as the intermediate for Pt<jats:sub>1</jats:sub>@MIL, whereas COOH* serves as the intermediate for Pt<jats:sub>n</jats:sub>@MIL. The unique reaction path over Pt<jats:sub>1</jats:sub>@MIL not only lowers the activation energy for the enhanced catalytic activity, but also contributes to the high selectivity for methanol.</jats:p>