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Enhancing polyol/sugar cascade oxidation to formic acid with defect rich MnO2 catalysts.
- Source :
- Nature Communications; 7/26/2023, Vol. 14 Issue 1, p1-11, 11p
- Publication Year :
- 2023
-
Abstract
- Oxidation of renewable polyol/sugar into formic acid using molecular O<subscript>2</subscript> over heterogeneous catalysts is still challenging due to the insufficient activation of both O<subscript>2</subscript> and organic substrates on coordination-saturated metal oxides. In this study, we develop a defective MnO<subscript>2</subscript> catalyst through a coordination number reduction strategy to enhance the aerobic oxidation of various polyols/sugars to formic acid. Compared to common MnO<subscript>2</subscript>, the tri-coordinated Mn in the defective MnO<subscript>2</subscript> catalyst displays the electronic reconstruction of surface oxygen charge state and rich surface oxygen vacancies. These oxygen vacancies create more Mn<superscript>δ+</superscript> Lewis acid site together with nearby oxygen as Lewis base sites. This combined structure behaves much like Frustrated Lewis pairs, serving to facilitate the activation of O<subscript>2</subscript>, as well as C–C and C–H bonds. As a result, the defective MnO<subscript>2</subscript> catalyst shows high catalytic activity (turnover frequency: 113.5 h<superscript>−1</superscript>) and formic acid yield (>80%) comparable to noble metal catalysts for glycerol oxidation. The catalytic system is further extended to the oxidation of other polyols/sugars to formic acid with excellent catalytic performance. This work develops defective MnO2 catalysts with Frustrated Lewis Pairs through a coordination number reduction strategy to enhance the aerobic oxidation of various polyols/sugars to formic acid. [ABSTRACT FROM AUTHOR]
Details
- Language :
- English
- ISSN :
- 20411723
- Volume :
- 14
- Issue :
- 1
- Database :
- Complementary Index
- Journal :
- Nature Communications
- Publication Type :
- Academic Journal
- Accession number :
- 167308219
- Full Text :
- https://doi.org/10.1038/s41467-023-40306-w