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One‐stage size‐selective method of laser electrodispersion (LED) was used to produce nanostructured NiPd, NiMo and NiW coatings on the surface of alumina, HOPG and Sibunit for the catalytic application. The deposition of nanoparticles produced by LED of bimetallic targets from alloyed or pressed metal powders provides the uniform distribution of both metals on the outer support surface; the metal ratio is similar to that in the original target. The catalytic behaviour of produced “core‐shell” catalysts in comparison with monometallic analogues was tested in two model reactions: the CO oxidation with oxygen on NiPd catalysts supported on alumina and Sibunit; and thiophene oxidation with hydrogen peroxide on NiMo and NiW alumina supported catalysts. Novel LED bimetallic catalysts with extremely low metal content (0.005 %) were superior in terms of activity and stability to monometallic ones and the catalysts obtained by “wet” chemistry methods. Improved catalytic properties of bimetallic LED catalysts are related to the high density of single nanoparticles and the formation of active metal‐oxide interfaces on the support surface.

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