Shape-Controlled CO2 Electrochemical Reduction on Nanosized Pd Hydride Cubes and Octahedra

Zhu, Wenlei; Kattel, Shyam; Jiao, Feng; Chen, Jingguang G.

doi:10.1002/aenm.201802840

Shape-Controlled CO₂ Electrochemical Reduction on Nanosized Pd Hydride Cubes and Octahedra

Journal Article · Tue Jan 08 23:00:00 EST 2019 · Advanced Energy Materials

DOI:https://doi.org/10.1002/aenm.201802840· OSTI ID:1712669

^[1]; Kattel, Shyam ^[2]; ^[3]; ^[2]

Univ. of Delaware, Newark, DE (United States); University of Delaware
Columbia Univ., New York, NY (United States)
Univ. of Delaware, Newark, DE (United States)

Electrochemical CO₂ reduction reaction (CO₂RR) provides a potential pathway to mitigate challenges related to CO₂ emissions. Pd nanoparticles have shown interesting properties as CO₂RR electrocatalysts, while how different facets of Pd affect its performance in CO₂ reduction to synthesis gas with controlled H₂ to CO ratios has not been studied. Herein, we synthesized nano-sized Pd cubes and octahedra particles dominated by Pd(100) and Pd(111) facets, respectively. Here, the Pd octahedra particles show higher CO selectivity (up to 95%) and better activity than Pd cubes and commercial particles. For both Pd octahedra and cubes, the ratio of H₂/CO products was tunable between 1 and 2, a desirable ratio for methanol production and the Fischer-Tropsch processes. Further studies of Pd octahedra in a 25-cm² flow cell showed a total CO current of 5.47 A was achieved at a potential of 3.4 V, corresponding to a CO partial current density of 220 mA/cm^-2. In situ X-ray absorption spectroscopy studies showed that regardless of facet Pd transformed into Pd hydride (PdH) under reaction conditions. DFT calculations show that the reduced binding energies of CO and HOCO intermediates on PdH(111) are key parameters to the high current density and Faradaic efficiency in CO₂ to CO conversion.

View Accepted Manuscript (DOE)

Research Organization:: Univ. of Delaware, Newark, DE (United States); Columbia Univ., New York, NY (United States)

Sponsoring Organization:: USDOE Office of Fossil Energy (FE); USDOE Office of Science (SC)

Grant/Contract Number:: FE0029868; AC02-06CH11357; SC0009476; SC0009476

OSTI ID:: 1712669

Alternate ID(s):: OSTI ID: 1614350
OSTI ID: 1490120

Journal Information:: Advanced Energy Materials, Journal Name: Advanced Energy Materials Journal Issue: 9 Vol. 9; ISSN 1614-6832

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
CO2 reduction
Pd nanocrystals
carbon dioxide
density functional theory
electrocatalysts
electrochemical reduction
free energy
syngas ratio