期刊
ACS CATALYSIS
卷 10, 期 10, 页码 5928-5938出版社
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.0c01305
关键词
catalysis; hydrogen peroxide; palladium; electrocatalysis
资金
- Federal Ministry of Education and Research (BMBF) [FK: 03XP0265]
- Federal Ministry for Economic Affairs and Energy (BMWi) of Germany [03ET6080A]
- IMPRS-SurMat doctoral program
- MAXNET Energy
- Cardiff University
- University of Bath
- EPSRC [EP/S020802/1, EP/S020845/1] Funding Source: UKRI
Palladium nanoparticles have been studied extensively as catalysts for the direct synthesis of hydrogen peroxide, where selectivity remains a key challenge. Alloying Pd with other metals and using acid and halide promoters are commonly employed to increase H2O2 selectivity; however, the sites that can selectively produce H2O2 have not been identified and the role of these additives remains unclear. Here, we report the synthesis of atomically dispersed PdClx/C as a model catalyst for H2O2 production without the presence of extended Pd surfaces. We show that these isolated cationic Pd sites can form H2O2 with significantly higher selectivity than metallic Pd nanoparticles in both the reaction of H-2 and O-2 and the electrochemical oxygen reduction reaction. These results demonstrate that catalysts containing high populations of isolated Pd sites are selective catalysts for this two-electron reduction reaction and that the performance of materials in the direct synthesis reaction and electrocatalytic oxygen reduction reaction has many similarities.
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