4.6 Article

Palladium Hydride on C2N to Boost Formate Oxidation

Journal

ACS SUSTAINABLE CHEMISTRY & ENGINEERING
Volume 11, Issue 31, Pages -

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acssuschemeng.3c00852

Keywords

electrocatalysis; direct formate fuel cell; palladium hydride; C2N; formateoxidationreaction; fuel cell

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PdH0.58@C2N prepared using an in situ growth method exhibits excellent formate oxidation activity and durability. The Pd lattice expands due to hydrogen intercalation, and an electronic redistribution is observed. Both phenomena enhance the activity and stability of the composite catalyst, as confirmed by differential functional theory calculations.
PdH0.58@C2N preparedusing an in situgrowth method demonstrates excellent formate oxidation activity anddurability. Thelack of electrocatalysts for the formate oxidation reaction(FOR) hampers the deployment of direct formate fuel cells (DFFCs).To overcome this limitation, herein, we detail the production of palladiumhydride particles supported on C2N (PdH0.58@C2N) via a facile method. PdH0.58@C(2)Ndisplays excellent FOR performance, reaching current densities upto 5.6 A & BULL;mg(Pd) (-1) and stable cyclingand chronoamperometric operation. The Pd lattice expands due to thehydrogen intercalation. Besides, an electronic redistribution associatedwith the distinct electronegativity of Pd and H is observed. Bothphenomena modify the electron energy levels, enhancing the activityand stability of the composite catalyst. More specifically, differentialfunctional theory calculations show H intercalation to downshift thePd d-band center in Pd-0.58@C2N, weakening adsorbatebinding and accelerating the FOR rate-determining step.

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