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 Ir–Ag can
efficiently produce H2O2, despite the negligible
activities of Rh, Pt, Ir, Ag, and Au alone. In particular, we show
that two catalysts, Rh13Ag87 and Pt28Au72 NPs, can outperform prototypic Pd NPs. Rh13Ag87 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 gcat
–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.
To accelerate the discovery of materials through computations and experiments, a well-established protocol closely bridging these methods is required. We introduce a high-throughput screening protocol for the discovery of bimetallic catalysts that replace palladium (Pd), where the similarities in the electronic density of states patterns were employed as a screening descriptor. Using first-principles calculations, we screened 4350 bimetallic alloy structures and proposed eight candidates expected to have catalytic performance comparable to that of Pd. Our experiments demonstrate that four bimetallic catalysts indeed exhibit catalytic properties comparable to those of Pd. Moreover, we discover a bimetallic (Ni-Pt) catalyst that has not yet been reported for H2O2 direct synthesis. In particular, Ni61Pt39 outperforms the prototypical Pd catalyst for the chemical reaction and exhibits a 9.5-fold enhancement in cost-normalized productivity. This protocol provides an opportunity for the catalyst discovery for the replacement or reduction in the use of the platinum-group metals.
We propose a novel high-throughput screening platform using a centrifugal microfluidic device for producing combinatorial tri-metallic catalysts. The centrifugal device was designed to perform sixty reactions under different conditions on...
In this study, we developed a method to monitor the phosphorylation and translocation of the extracellular signal-regulated kinase (ERK2) proteins after PC12 cells have been stimulated by a mitogen. The method involves the use of green fluorescent protein (GFP), capillary electrophoresis and the measurement of laser-induced fluorescence (CE-LIF). We showed the prescence of the non-phosphorylated GFP-ERK2 and phosphorylated GFP-ERK2 in cell lysates by CE-LIF, and then compared the phosphorylations of GFP-ERK2 and GFP-183A. Phosphorylated GFP-ERK2 was detected at 6.7 min and the non-phosphorylated GFP-ERK2 at 5.3-5.5 min. The results were compared with confocal laser scanning microscope imaging and western blot results, and suggest that the developed method can be used to detect other enzymatic modifications.
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