A New Generation of Platinum‐Copper Electrocatalysts with Ultra‐Low Concentrations of Platinum for Oxygen‐Reduction Reactions in Alkaline Media
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Abstract In order to reduce the cost and enhance the performance of the cathode catalyst for fuel cell, support‐less, ultra‐low Pt contents based nanostructured platinum copper (Pt−Cu) nanoparticles (NPs), with differential Pt‐contents, were prepared using CTAB‐reduction approach and avoiding utilization of high Pt contents, while keeping high electrocatalytic activity and durability. The novelty of present work lies in the suggested synthesis method for support‐free Pt−Cu NPs with lower Pt loadings (0.04‐0.25 wt.%). Pt 0.25 Cu NPs (E o 0.98 V vs. RHE) exhibits high ORR performance compared to Pt/C (20 wt.%) (E o 0.97 V vs. RHE). The synthesis method of our Pt−Cu NPs will find wide application in the preparation of bimetallic nanocatalysts.Keywords:
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A highly active Pt–Cu bimetallic catalyst for the electrocatalytic oxygen reduction reaction, with an average diameter of 2.9 nm and a Cu/Pt ratio of 0.30 for the bimetallic nanoparticles, was prepared by capturing Pt–Cu alloy nanoparticles on melem-modified carbon, followed by removing 90% of copper from the alloy NPs.
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Synthesis of bimetallic nanomaterials with well controlled shape is an important topic in heterogeneous catalysis, low-temperature fuel cell technology, and many other fields. Compared with monometallic counterparts, bimetallic nanocatalysts endow scientists with more opportunities to optimize the catalytic performance by modulating the charge transfer between different metals, local coordination environment, lattice strain and surface element distribution. Considering the current challenges in shape controlled synthesis of bimetallic nanocatalysts, this tutorial review highlights some significant achievements in preparing bimetallic alloy, core-shell and heterostructure nanocrystals with well-defined morphologies, summarizes four general routes and some key factors of the bimetallic shape control scenarios, and provides some general ideas on how to design synthetic strategies to control the shape and exposing facets of bimetallic nanocrystals. The composition and shape dependent catalytic behaviours of bimetallic nanocrystals are reviewed as well.
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Three dimensional PtCu@Pt bimetallic alloy nanofoams show enhanced electrocatalytic activities for oxygen reduction reaction.
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Abstract Bimetallic nanocatalysts are key enablers of current chemical technologies, including car exhaust converters and fuel cells, and play a crucial role in industry to promote a wide range of chemical reactions. However, owing to significant characterization challenges, insights in the dynamic phenomena that shape and change the working state of the catalyst await further refinement. Herein, we discuss the atomic‐scale processes leading to mono‐ and bimetallic nanoparticle formation and highlight the dynamics and kinetics of lifetime changes in bimetallic catalysts with showcase examples for Pt‐based systems. We discuss how in situ and operando X‐ray spectroscopy, scattering, and diffraction can be used as a complementary toolbox to interrogate the working principles of today's and tomorrow's bimetallic nanocatalysts.
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Abstract Bimetallic nanocatalysts are key enablers of current chemical technologies, including car exhaust converters and fuel cells, and play a crucial role in industry to promote a wide range of chemical reactions. However, owing to significant characterization challenges, insights in the dynamic phenomena that shape and change the working state of the catalyst await further refinement. Herein, we discuss the atomic‐scale processes leading to mono‐ and bimetallic nanoparticle formation and highlight the dynamics and kinetics of lifetime changes in bimetallic catalysts with showcase examples for Pt‐based systems. We discuss how in situ and operando X‐ray spectroscopy, scattering, and diffraction can be used as a complementary toolbox to interrogate the working principles of today's and tomorrow's bimetallic nanocatalysts.
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Compared with their monometallic counterparts, bimetallic nanoparticles often show enhanced catalytic activity associated with the bimetallic interface. Direct quantitation of catalytic activity at the bimetallic interface is important for understanding the enhancement mechanism, but challenging experimentally. Here using single-molecule super-resolution catalysis imaging in correlation with electron microscopy, we report the first quantitative visualization of enhanced bimetallic activity within single bimetallic nanoparticles. We focus on heteronuclear bimetallic PdAu nanoparticles that present a well-defined Pd-Au bimetallic interface in catalyzing a photodriven fluorogenic disproportionation reaction. Our approach also enables a direct comparison between the bimetallic and monometallic regions within the same nanoparticle. Theoretical calculations further provide insights into the electronic nature of N-O bond activation of the reactant (resazurin) adsorbed on bimetallic sites. Subparticle activity correlation between bimetallic enhancement and monometallic activity suggests that the favorable locations to construct bimetallic sites are those monometallic sites with higher activity, leading to a strategy for making effective bimetallic nanocatalysts. The results highlight the power of super-resolution catalysis imaging in gaining insights that could help improve nanocatalysts.
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Shape-controlled synthesis of bimetallic nanocrystals has been one of attractive research directions in the fields of synthetic chemistry and catalysis. The driving force for the development of synthetic chemistry derives from the dependent relationship of the size, composition, shape and structure of nanocrystals with their catalytic performances. This chapter summarizes some significant achievements in preparing bimetallic nanopolyhedrons and nanospheres, and highlights shape effect of bimetallic nanocrystals on the associated catalytic performances. It is expected to provide some general ideas on the designed synthesis of shape-tunable bimetallic nanocatalysts with high performances.
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Bimetallic nanocatalysts, with efficient and controllable catalytic performance, have a promising application in chemical production. In this study, surface Pt-rich bimetallic AuPt nanoparticles with different Pt/Au ratios were prepared and tested in selective hydrogenation reactions of substituted nitroaromatics. Au nanoparticles were first prepared with n-butyllithium as a rapid reducer, which were further used as seeds in the slow growth process of Pt atoms. Because of the employed sequential reduction method and the following atom diffusion, surface Pt-rich bimetallic AuPt nanoparticles were obtained. Compared with the uniform AuPt alloy nanocatalysts synthesized by the co-reduction method with n-butyllithium as the reducer and monometallic Pt nanocatalysts, the obtained surface Pt-rich AuPt bimetallic nanocatalysts presented an enhanced catalytic selectivity or activity. The performance enhancement is assigned to the optimized Au/Pt interaction in the surface Pt-rich bimetallic nanostructures. This work demonstrates that the optimization of the stoichiometry and construction of bimetallic materials is a feasible method to synthesize controllable and efficient nanocatalysts.
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