Using the site-knockout strategy to understand the low activity of the nitrate electro-reduction reaction on Pt(111)

Silva, Kaline Nascimento da; Soffiati, Gabriela Volpini; Silva, E. Z. da; San-Miguel, Miguel A.; Sitta, Elton

doi:10.1039/d2nj01773c

“…We next focused on the application of these ultra‐low loading antenna‐reactor catalysts for the electrocatalytic conversion of NO 2 − to NH 3 (NO 2 RR). The cyclic voltammograms for Au 99.4 Pt 0.6 and Au 94 Pt 6 NPs in the presence of NO 2 − are characteristic of the reduction of NO x compounds (Figure 4A and Figure S20, red and blue traces, respectively) [40] . Voltammograms in the absence of NO 2 − are shown in Figure S21.…”

Section: Resultsmentioning

confidence: 97%

“…À are characteristic of the reduction of NO x compounds (Figure 4A and Figure S20, red and blue traces, respectively). [40] Voltammograms in the absence of NO 2 À are shown in Figure S21. Figure 4A is normalized by the mass of Pt, and since Au 99.4 Pt 0.6 contains a smaller amount of Pt, its mass-normalized CV presents a significantly higher capacitive current compared to Au 94 Pt 6 .…”

Section: Resultsmentioning

confidence: 99%

Ultralow Catalytic Loading for Optimised Electrocatalytic Performance of AuPt Nanoparticles to Produce Hydrogen and Ammonia

Bezerra,

Brasseur,

Sullivan‐Allsop

et al. 2024

Angewandte Chemie

Self Cite

0

View full text Add to dashboard Cite

The hydrogen evolution and nitrite reduction reactions are key to producing green hydrogen and ammonia. Antenna–reactor nanoparticles hold promise to improve the performances of these transformations under visible‐light excitation, by combining plasmonic and catalytic materials. However, current materials involve compromising either on the catalytic activity or the plasmonic enhancement and also lack control of reaction selectivity. Here, we demonstrate that ultralow loadings and non‐uniform surface segregation of the catalytic component optimize catalytic activity and selectivity under visible‐light irradiation. Taking Pt‐Au as an example we find that fine‐tuning the Pt content produces a 6‐fold increase in the hydrogen evolution compared to commercial Pt/C as well as a 6.5‐fold increase in the nitrite reduction and a 2.5‐fold increase in the selectivity for producing ammonia under visible light excitation relative to dark conditions. Density functional theory suggests that the catalytic reactions are accelerated by the intimate contact between nanoscale Pt‐rich and Au‐rich regions at the surface, which facilitates the formation of electron‐rich hot‐carrier puddles associated with the Pt‐based active sites. The results provide exciting opportunities to design new materials with improved photocatalytic performance for demanding sustainable energy applications.

show abstract

Ultralow Catalytic Loading for Optimised Electrocatalytic Performance of AuPt Nanoparticles to Produce Hydrogen and Ammonia

Bezerra,

Brasseur,

Sullivan‐Allsop

et al. 2024

Angew Chem Int Ed

Self Cite

3

0

View full text Add to dashboard Cite

The hydrogen evolution and nitrite reduction reactions are key to producing green hydrogen and ammonia. Antenna–reactor nanoparticles hold promise to improve the performances of these transformations under visible‐light excitation, by combining plasmonic and catalytic materials. However, current materials involve compromising either on the catalytic activity or the plasmonic enhancement and also lack control of reaction selectivity. Here, we demonstrate that ultralow loadings and non‐uniform surface segregation of the catalytic component optimize catalytic activity and selectivity under visible‐light irradiation. Taking Pt‐Au as an example we find that fine‐tuning the Pt content produces a 6‐fold increase in the hydrogen evolution compared to commercial Pt/C as well as a 6.5‐fold increase in the nitrite reduction and a 2.5‐fold increase in the selectivity for producing ammonia under visible light excitation relative to dark conditions. Density functional theory suggests that the catalytic reactions are accelerated by the intimate contact between nanoscale Pt‐rich and Au‐rich regions at the surface, which facilitates the formation of electron‐rich hot‐carrier puddles associated with the Pt‐based active sites. The results provide exciting opportunities to design new materials with improved photocatalytic performance for demanding sustainable energy applications.

show abstract

Enhanced electrocatalytic nitrate reduction and energy conversion through Zn-Nitrate battery by Cu3P@Co(OH)2/CF heterostructure catalyst

Yue,

Liping,

Yuechen

et al. 2024

International Journal of Hydrogen Energy

4

0

View full text Add to dashboard Cite

Using the site-knockout strategy to understand the low activity of the nitrate electro-reduction reaction on Pt(111)

Abstract: Nitrate and nitrite reduction reactions (NO3RR and NO2RR, respectively) are important processes in water treatment as well as model processes in surface science. The sluggish kinetics observed for the NO3RR...

Cited by 4 publications

References 57 publications

Ultralow Catalytic Loading for Optimised Electrocatalytic Performance of AuPt Nanoparticles to Produce Hydrogen and Ammonia

Ultralow Catalytic Loading for Optimised Electrocatalytic Performance of AuPt Nanoparticles to Produce Hydrogen and Ammonia

Ultralow Catalytic Loading for Optimised Electrocatalytic Performance of AuPt Nanoparticles to Produce Hydrogen and Ammonia

Enhanced electrocatalytic nitrate reduction and energy conversion through Zn-Nitrate battery by Cu3P@Co(OH)2/CF heterostructure catalyst

Contact Info

Product

Resources

About