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Single Ru atoms with precise coordination on a monolayer layered double hydroxide for efficient electrooxidation catalysis.

ABSTRACT: The catalytic properties of single-atom catalysts (SACs) can be influenced largely by the chemical environment exerted by supports. Therefore, a precise location of the single atom is essential for understanding of the reaction mechanism and design of novel SACs. However, the preparation of SACs with a precise location remains a great challenge. Herein, we report a facile one-step method to synthesize single Ru atoms supported on a monolayer NiFe-layered double hydroxide (mono-NiFe). Detailed studies demonstrate that the single Ru atoms are not dispersed randomly in the LDH structure, but are uniquely located on the top of the Fe-metal atom of mono-NiFe via three oxygen atoms. Furthermore, these SACs prove to be highly active for the hydrazine electrooxidation reaction. Density functional theory calculations demonstrate that the single Ru atoms can stabilize the hydrazine electrooxidation intermediate with one unpaired electron (*N₂H₃ and *N₂H), thus lowering the reaction barrier for the rate-determining step. Moreover, the loading amount of single Ru atoms with a precise location can even go up to 7.0 wt% without any aggregation.

SUBMITTER: Wang Z

PROVIDER: S-EPMC6335951 | biostudies-literature |

REPOSITORIES: biostudies-literature

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Project description:A new electrochemical synthesis route was developed for the fabrication of Fe-containing layered double hydroxide (MFe-LDHs, M = Ni, Co and Li) hierarchical nanoarrays, which exhibit highly-efficient electrocatalytic performances for the oxidation reactions of several small molecules (water, hydrazine, methanol and ethanol). Ultrathin MFe-LDH nanoplatelets (200-300 nm in lateral length; 8-12 nm in thickness) perpendicular to the substrate surface are directly prepared within hundreds of seconds (<300 s) under cathodic potential. The as-obtained NiFe-LDH nanoplatelet arrays display promising behavior in the oxygen evolution reaction (OER), giving rise to a rather low overpotential (0.224 V) at 10.0 mA cm-2 with largely enhanced stability, much superior to previously reported electro-oxidation catalysts as well as the state-of-the-art Ir/C catalyst. Furthermore, the MFe-LDH nanoplatelet arrays can also efficiently catalyze several other fuel molecules' oxidation (e.g., hydrazine, methanol and ethanol), delivering a satisfactory electrocatalytic activity and a high operation stability. In particular, this preparation method of Fe-containing LDHs is amenable to fast, effective and large-scale production, and shows promising applications in water splitting, fuel cells and other clean energy devices.

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Layered double hydroxide-oxidized carbon nanotube hybrids as highly efficient flame retardant nanofillers for polypropylene.

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| S-EPMC5067659 | biostudies-literature

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