Contrasting Capability of Single Atom Palladium for Thermocatalytic versus Electrocatalytic Nitrate Reduction Reaction

Xuanhao Wu, Mohammadreza Nazemi, Srishti Gupta, Adam Chismar, Kiheon Hong, Hunter Jacobs, Wenqing Zhang, Kali Rigby, Tayler Hedtke, Qingxiao Wang, Eli Stavitski, Michael S. Wong, Christopher Muhich, Jae-Hong Kim

    Research output: Contribution to journalArticlepeer-review

    21 Scopus citations

    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(1:100) SAA exhibited the greatest activity (TOFPd = 2 min–1) and highest N2 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 N2 selectivity of Pd/Cu(1:100) in E-NRR compared to T-NRR originate from the higher stability of NO3* in electrocatalysis and a lower N2 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.
    Original languageEnglish (US)
    Pages (from-to)6804-6812
    Number of pages9
    JournalACS Catalysis
    DOIs
    StatePublished - May 3 2023

    ASJC Scopus subject areas

    • Catalysis

    Fingerprint

    Dive into the research topics of 'Contrasting Capability of Single Atom Palladium for Thermocatalytic versus Electrocatalytic Nitrate Reduction Reaction'. Together they form a unique fingerprint.

    Cite this