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Contrasting Capability of Single Atom Palladium for Thermocatalytic versus Electrocatalytic Nitrate Reduction Reaction.
- Source :
-
ACS catalysis [ACS Catal] 2023 May 03; Vol. 13 (10), pp. 6804-6812. Date of Electronic Publication: 2023 May 03 (Print Publication: 2023). - Publication Year :
- 2023
-
Abstract
- The occurrence of high concentrations of nitrate in various water resources is a significant environmental and human health threat, demanding effective removal technologies. Single atom alloys (SAAs) have emerged as a promising bimetallic material architecture in various thermocatalytic and electrocatalytic schemes including nitrate reduction reaction (NRR). This study suggests that there exists a stark contrast between thermocatalytic (T-NRR) and electrocatalytic (E-NRR) pathways that resulted in dramatic differences in SAA performances. Among Pd/Cu nanoalloys with varying Pd-Cu ratios from 1:100 to 100:1, Pd/Cu <subscript>(1:100)</subscript> SAA exhibited the greatest activity (TOF <subscript>Pd</subscript> = 2 min <superscript>-1</superscript> ) and highest N <subscript>2</subscript> selectivity (94%) for E-NRR, while the same SAA performed poorly for T-NRR as compared to other nanoalloy counterparts. DFT calculations demonstrate that the improved performance and N <subscript>2</subscript> selectivity of Pd/Cu <subscript>(1:100)</subscript> in E-NRR compared to T-NRR originate from the higher stability of NO <subscript>3</subscript> * in electrocatalysis and a lower N <subscript>2</subscript> formation barrier than NH due to localized pH effects and the ability to extract protons from water. This study establishes the performance and mechanistic differences of SAA and nanoalloys for T-NRR versus E-NRR.<br />Competing Interests: The authors declare no competing financial interest.<br /> (© 2023 The Authors. Published by American Chemical Society.)
Details
- Language :
- English
- ISSN :
- 2155-5435
- Volume :
- 13
- Issue :
- 10
- Database :
- MEDLINE
- Journal :
- ACS catalysis
- Publication Type :
- Academic Journal
- Accession number :
- 37234352
- Full Text :
- https://doi.org/10.1021/acscatal.3c01285