Robust palladium hydride catalyst for electrocatalytic formate formation with high CO tolerance

Guo, Shengyuan; Liu, Yuanchao; Murphy, Eamonn; Ly, Alvin; Xu, Mingjie; Matanovic, Ivana; Pan, Xiaoqing; Atanassov, Plamen

doi:10.1016/j.apcatb.2022.121659

Robust palladium hydride catalyst for electrocatalytic formate formation with high CO tolerance

Journal Article · Wed Jun 22 00:00:00 EDT 2022 · Applied Catalysis. B, Environmental

DOI:https://doi.org/10.1016/j.apcatb.2022.121659· OSTI ID:1998117

Guo, Shengyuan ^[1]; Liu, Yuanchao ^[1]; Murphy, Eamonn ^[1]; Ly, Alvin ^[1]; Xu, Mingjie ^[1]; ^[2]; Pan, Xiaoqing ^[1]; Atanassov, Plamen ^[1]

Univ. of California, Irvine, CA (United States)
Univ. of New Mexico, Albuquerque, NM (United States); Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)

Palladium is unique in the electrocatalytic reduction of CO₂ to formate because of its low or even near-equilibrium onset potential. However, the inevitably produced CO molecules poison and deactivate the catalyst surface, resulting in an insufficient operating lifetime (<30 min) for conventional and optimized Pd catalysts. In this work, we present a hydrogen-rich Palladium hydride catalyst (PdH0.5/C) derived from a one-step solvothermal synthesis. This catalyst showed a 93.1 % faradaic efficiency towards formate at – 0.4 V (vs RHE). The working lifetime reached a record of 4 h, which was ~15 times longer than a commercial Pd catalyst and outperformed all previous Pd-based electrocatalysts for CO₂-HCOO^– conversion. The high CO tolerance was attributed to the selectivity improvement induced by lattice hydrogen and the weak CO adsorption strength on diverse active sites (i.e. kink, step, and terrace). Isotopic analysis revealed a direct participation of the lattice hydrogen in the protonation of CO₂ molecules in formate formation.

View Accepted Manuscript (DOE)

Research Organization:: Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Bioenergy Technologies Office (BETO)

Grant/Contract Number:: 89233218CNA000001; EE0008923

OSTI ID:: 1998117

Report Number(s):: LA-UR--22-24339

Journal Information:: Applied Catalysis. B, Environmental, Journal Name: Applied Catalysis. B, Environmental Vol. 316; ISSN 0926-3373

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
CO tolerance
Electrochemical CO2 reduction
Formate
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Robust palladium hydride catalyst for electrocatalytic formate formation with high CO tolerance

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