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Taming Pt 5d state occupancy via PtOMn electronic linkage for enhanced dehydrogenation activity.
- Source :
- AIChE Journal; Sep2023, Vol. 69 Issue 9, p1-13, 13p
- Publication Year :
- 2023
-
Abstract
- The enhancement of catalytic activity is always limited by the dilemma in activation and desorption due to Sabatier principle. Locating the Sabatier optimum by manipulating catalyst electronic structure has been a long‐standing challenge in heterogeneous catalysis. Herein, we presented a generic strategy to continuously tailor the Pt 5d state occupancy via tuning the PtOMn electronic linkage over Al2O3‐confined MnOx islands, aiming at accommodating the CH cleavage and product desorption capabilities in dehydrogenation of liquid organic hydrogen carriers (monocyclic/bicyclic hydrides). Rising Mn valence can decrease the Pt 5d state occupancy through more electron transfer from Pt 5d to O 2p due to the strong π‐donation of O 2p to Mn 3d. This will lead to the lower initial CH activation energy barrier while higher product desorption energy barrier. An intermediate Pt 5d filling of ~8.4 in PtMn2O3/Al2O3 enables the balanced level of product desorption and CH activation, thus ensuring a superior dehydrogenation activity. The electron structure‐adsorption‐performance modulation mechanism described herein provides a benchmark to locate the Sabatier optimum for the metal catalyst design. [ABSTRACT FROM AUTHOR]
Details
- Language :
- English
- ISSN :
- 00011541
- Volume :
- 69
- Issue :
- 9
- Database :
- Complementary Index
- Journal :
- AIChE Journal
- Publication Type :
- Academic Journal
- Accession number :
- 169915373
- Full Text :
- https://doi.org/10.1002/aic.18149