4.8 Article

Environment of Metal-O-Fe Bonds Enabling High Activity in CO2 Reduction on Single Metal Atoms and on Supported Nanoparticles

Journal

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 143, Issue 14, Pages 5540-5549

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/jacs.1c02276

Keywords

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Funding

  1. U.S. Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences and Biosciences (Transdisciplinary Approaches to Realize Novel Catalytic Pathways to Energy Carriers) [FWP 47319]
  2. DOE [DE-AC02-06CH11357, DE-AC05-76RL01830]
  3. Canadian Light Source
  4. DOE's Office of Biological and Environmental Research
  5. EMSL
  6. PNNL's Research Computing facility
  7. National Energy Research Scientific Computing Center, a DOE Office of Science User Facility [DE-AC02-05CH11231]

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Research demonstrates that single atoms of Pt-group metals embedded into the surface of Fe3O4 have a stronger interaction with CO2, leading to significantly higher conversion rates compared to nanoparticles. The high activity of single atoms is primarily attributed to the influence of partially oxidic sites.
Single-atom catalysts are often reported to have catalytic properties that surpass those of nanoparticles, while a direct comparison of sites common and different for both is lacking. Here we show that single atoms of Pt-group metals embedded into the surface of Fe3O4 have a greatly enhanced interaction strength with CO2 compared with the Fe3O4 surface. The strong CO2 adsorption on single Rh atoms and corresponding low activation energies lead to 2 orders of magnitude higher conversion rates of CO2 compared to Rh nanoparticles. This high activity of single atoms stems from the partially oxidic state imposed by their coordination to the support. Fe3O4-supported Rh nanoparticles follow the behavior of single atoms for CO2 interaction and reduction, which is attributed to the dominating role of partially oxidic sites at the Fe3O4Rh interface. Thus, we show a likely common catalytic chemistry for two kinds of materials thought to be different, and we show that single atoms of Pt-group metals on Fe3O4 are especially successful materials for catalyzed reactions that depend primarily upon sites with the metal-O-Fe environment.

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