Journal
NATURE COMMUNICATIONS
Volume 11, Issue 1, Pages -Publisher
NATURE PUBLISHING GROUP
DOI: 10.1038/s41467-020-16830-4
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Funding
- U.S. Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences (BES), Division of Chemical Sciences, Geosciences and Biosciences (Transdisciplinary Approaches to Realize Novel Catalytic Pathways to Energy Carriers) [FWP 47319]
- DOE BES Geosciences program at Pacific Northwest National Laboratory (PNNL) (Fundamental Mechanisms of Reactivity at Complex Geochemical Interfaces) [FWP 56674]
- DOE's Office of Biological and Environmental Research
- U.S. DOE [DE-AC02-06CH11357]
- Canadian Light Source
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Key chemical transformations require metal and redox sites in proximity at interfaces; however, in traditional oxide-supported materials, this requirement is met only at the perimeters of metal nanoparticles. We report that galvanic replacement can produce inverse FeOx/metal nanostructures in which the concentration of oxide species adjoining metal domains is maximal. The synthesis involves reductive deposition of rhodium or platinum and oxidation of Fe2+ from magnetite (Fe3O4). We discovered a parallel dissolution and adsorption of Fe2+ onto the metal, yielding inverse FeOx-coated metal nanoparticles. This nanostructure exhibits the intrinsic activity in selective CO2 reduction that simple metal nanoparticles have only at interfaces with the support. By enabling a simple way to control the surface functionality of metal particles, our approach is not only scalable but also enables a versatile palette for catalyst design. While typical catalysts involve oxide-supported metals, inverse catalysts of oxides on metal supports offer an attractive alternative. Here, authors prepare FeOx-coated Rh nanoparticles via galvanic replacement and dissolution-precipitation to form effective CO2 reduction catalysts.
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