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

Journal Article · · Advanced Energy Materials
ORCiD logo [1];  [2]; ORCiD logo [1]; ORCiD logo [2]
  1. Univ. of Delaware, Newark, DE (United States)
  2. Columbia Univ., New York, NY (United States)
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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.

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; FG02-13ER16381; SC0009476
OSTI ID:
1712669
Alternate ID(s):
OSTI ID: 1490120
Journal Information:
Advanced Energy Materials, Vol. 9, Issue 9; ISSN 1614-6832
Publisher:
WileyCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 120 works
Citation information provided by
Web of Science

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Cited By (12)

Electrode Materials Engineering in Electrocatalytic CO 2 Reduction: Energy Input and Conversion Efficiency journal October 2019
Engineering Electronic Structure of Stannous Sulfide by Amino‐Functionalized Carbon: Toward Efficient Electrocatalytic Reduction of CO 2 to Formate journal January 2020
Enhancing Activity and Reducing Cost for Electrochemical Reduction of CO 2 by Supporting Palladium on Metal Carbides journal February 2019
Efficient Electrosynthesis of Syngas with Tunable CO/H 2 Ratios over Zn x Cd 1− x S‐Amine Inorganic–Organic Hybrids journal November 2019
In Situ Reconstruction of a Hierarchical Sn‐Cu/SnO x Core/Shell Catalyst for High‐Performance CO 2 Electroreduction journal February 2020
Enhancing Activity and Reducing Cost for Electrochemical Reduction of CO 2 by Supporting Palladium on Metal Carbides journal April 2019
Efficient Electrosynthesis of Syngas with Tunable CO/H 2 Ratios over Zn x Cd 1− x S‐Amine Inorganic–Organic Hybrids journal December 2019
In Situ Reconstruction of a Hierarchical Sn‐Cu/SnO x Core/Shell Catalyst for High‐Performance CO 2 Electroreduction journal February 2020
Effect of Hexadecylpyridinium Bromide (HDPB) on Morphology and Electrocatalytic Performance of Porous Palladium Nanoparticles journal January 2020
Structure-controlled synthesis of palladium concave nanocubes via CTAB-assisted reduction for methanol electro-oxidation journal January 2020
Tuning the activity and selectivity of electroreduction of CO2 to synthesis gas using bimetallic catalysts journal August 2019
Palladium structure engineering induced by electrochemical H intercalation boosts hydrogen evolution catalysis journal January 2019

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Related Subjects

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