期刊
CHEMCATCHEM
卷 14, 期 21, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/cctc.202200853
关键词
density functional theory; direct synthesis of H2O2; electronic metal-support interaction; oxidation state; single-atom catalyst
资金
- National Key R&D Program of China [2021YFB3801600]
- National Natural Science Foundation of China [22078005]
- State Key Laboratory of Catalytic Materials and Reaction Engineering (RIPP, SINOPEC)
In this study, isolated Pd atoms anchored on the Al vacancy of the γ-Al2O3(100) surface (Pd-1@γ-Al2O3(100)) were proposed as a potential heterogeneous catalyst for direct synthesis of H2O2. The Pd-1@γ-Al2O3(100) catalyst exhibited high selectivity and stability, which has promising applications.
Pd-based catalysts are essential for direct synthesis of H2O2 from H-2 and O-2, which still need further improvement of the activity and selectivity by engineering the status of Pd active species. In this work, isolated Pd atoms anchored on Al vacancy of the gamma-Al2O3(100) surface (Pd-1@gamma-Al2O3(100)) are proposed to act as a heterogeneous catalyst for direct synthesis of H2O2 from first-principles theoretical study and micro-kinetic analysis. The thermodynamic stability and whole catalytic mechanism for conversion of O-2 to H2O2 on Pd-1@gamma-Al2O3(100) was studied. It is found that the high selectivity toward H2O2 of Pd-1@gamma-Al2O3(100) is attributed to the high oxidation state of isolated Pd active sites with high stability against atom-aggregation, derived from the strong electronic metal-support interaction. The formation of 3+ cation state of isolated Pd atoms activates adsorbed oxygen molecule for hydrogenation and simnutaously restrains the formation of intermediate toward by-product, compared with traditional bulk Pd catalyst in the metallic state. This work provides theoretical insights into the feasibility of atom-level dispersion Pd to catalyze direct synthesis of H2O2 and guidance for its future development.
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