Journal
ACS CATALYSIS
Volume 9, Issue 9, Pages 8702-8711Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.9b00451
Keywords
bimetallic catalysts; metal nanoparticles; immiscible elements; Rh-Ag; Pt-Au; hydrogen peroxide direct synthesis; interfacial reactions; DFT calculations
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Funding
- Creative Materials Discovery Program through the National Research Foundation of Korea [NRF-2016M3D1A1021140]
- Korea Institute of Science and Technology [2E29280]
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Today, multimetallic nanoparticles (NPs) are extensively studied to search for high-performance catalysts. Unfortunately, a huge material space of NPs composed of immiscible elements has been generally disregarded for catalyst development due to the inherent difficulty of alloy synthesis. Herein, for the direct synthesis of hydrogen peroxide (H2O2), we demonstrate that NPs of immiscible elemental combinations of Rh-Ag, Rh-Au, Pt-Au, and IrAg can efficiently produce H2O2, despite the negligible activities of Rh, Pt, Ir, Ag, and Au alone. In particular, we show that two catalysts, Rh(13)Ag(87)( )and Pt28Au72 NPs, can outperform prototypic Pd NPs. Rh(13)Ag(87)NPs, owing to their high content of the less-expensive element Ag, exhibit a 7.3-fold enhancement in cost-normalized productivity compared to Pd and, thus, may serve as an economical option. The other catalyst of Pt28Au72 NPs exhibits a productivity of 300 mmol g(cat)(-1) h(-1) and a 15-fold increase over that of Pd under isoconversion conditions. The observed remarkable productivities of these NPs are a result of the synergy between the two elemental domains at the interface. The present study suggests that the hitherto underutilized space of immiscible elemental combinations should be more actively searched for the development of improved catalyst materials.
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