Methanol Tolerant Oxygen Reduction Reaction Electrocatalysis using Size‐Specific Triphenylphosphine‐Ligated Gold Nanoclusters

Mousavi, Hanieh; Sharma, Shailendra Kumar; Golovko, Vladimir B.; Shearer, Cameron J.; Metha, Gregory F.

doi:10.1002/cnma.202200122

“…The chronoamperometry experiment clearly suggests that the NCS-rGO catalyst has superior methanol tolerance and stability as compared to the Pt/C electrocatalyst under alkaline conditions. 54 The non-metal composition of NCS-rGO may be fully accountable for its long durability and resistance to methanol crossover effects. The obtained results validate the fascinating ORR activity of NCS-rGO.…”

Section: Electrocatalytic Performance Towards the Oxygen Reduction Re...mentioning

confidence: 99%

“…[51][52][53] The ORR like reactions can occur directly in such a catalytically active region. 54 In NCS-rGO samples, the ORR activity has been studied to better comprehend a correlation between the structure of N-doped species and its catalytic activity.…”

Section: Introductionmentioning

confidence: 99%

Scalable production of reduced graphene oxide via biowaste valorisation: an efficient oxygen reduction reaction towards metal-free electrocatalysis

Shah

¹

,

Singh²,

Prajongtat

³

et al. 2023

View full text Add to dashboard Cite

show abstract

“…26 The catalytic activity of phosphine-protected Au clusters has been tested in many reactions including H2 evolution, CO oxidation, CO2 reduction, benzyl alcohol and photocatalytic amine oxidation. [27][28][29][30][31] In addition to the ease of ligand removal, phosphineprotected Au clusters are free from sulfur poisoning (c.f. thiolate-protected Au clusters).…”

Section: Introductionmentioning

confidence: 99%

Photocatalytic H2O2 Production Over Photocatalysts Prepared By Phosphine-protected Au101 Nanoparticles on WO3

Abd Rahim,

Lee,

Alotabi

et al. 2024

Preprint

0

View full text Add to dashboard Cite

Photocatalytic H2O2 synthesis is an appealing and feasible strategy to replace the energy- intensive, tedious, and waste-generating anthraquinone process. Often, pure metal oxides show low activity in photocatalytic H2O2 production and therefore metal co-catalysts are required to improve the photoactivity. This work investigated photocatalytic H2O2 production using monodisperse gold nanoclusters Au101(PPh3)21Cl5 supported on WO3. From HRTEM imaging, the Au101 size in the uncalcined samples is in the cluster regime (<2 nm) and after calcination at 200 °C the size increases to ca. 4.5 nm. The roles of Au101 have been identified to reduce the charge carrier recombination and provide the active sites for O2 reduction which significantly enhances the photoactivity. Both uncalcined and calcined Au101/WO3 photocatalysts produce over 75 mM g-1 h-1 of H2O2 under UV light irradiation while the pure WO3 is inactive. At early times (up to 30 min), the production rate of H2O2 from calcined Au101/WO3 reaches 173 mM g-1 h-1 and is almost double the rate of the uncalcined catalyst (93 mM g-1 h-1). The higher photoactivity of calcined versus uncalcined Au101/WO3 can be attributed to the aggregated Au101 and removal of phosphine ligands from the Au core as verified by HRTEM and XPS. The reaction rate decreases over time which is attributed to the reverse reaction. Using a simple kinetic model, the rate constant of the H2O2 formation (kf) for uncalcined and calcined Au101/WO3 are 2.07 and 6.31 mM h-1, while the rate constant of the H2O2 decomposition (kd) for uncalcined and calcined Au101/WO3 are 0.49 and 2.93 h-1, respectively. This work highlights a simple preparation of highly active photocatalysts to produce H2O2 derived from Au101 clusters and WO3.

show abstract

“…3,6 However, the production yield of H2O2 is quite unsatisfactory using pure MOX The catalytic activity of phosphine-protected Au clusters has been tested in many reactions including H2 evolution, CO oxidation, CO2 reduction, benzyl alcohol and photocatalytic amine oxidation. [27][28][29][30][31] In addition to the ease of ligand removal, phosphineprotected Au clusters are free from sulfur poisoning (c.f. thiolate-protected Au clusters).…”

Section: Introductionmentioning

confidence: 99%

Photocatalytic H2O2 Production Over Photocatalysts Prepared By Phosphine-protected Au101 Nanoclusters on WO3

Abd Rahim,

Lee,

Alotabi

et al. 2023

Preprint

0

View full text Add to dashboard Cite

Photocatalytic H2O2 synthesis is an appealing and feasible strategy to replace the energy- intensive, tedious, and waste-generating anthraquinone process. Often, pure metal oxides show low activity in photocatalytic H2O2 production and therefore metal co-catalysts are required to improve the photoactivity. This work investigated photocatalytic H2O2 production using monodisperse gold nanoclusters Au101(PPh3)21Cl5 supported on WO3. From HRTEM imaging, the Au101 size in the uncalcined samples is in the cluster regime (<2 nm) and after calcination at 200 °C the size increases to ca. 4.5 nm. The roles of Au101 have been identified to reduce the charge carrier recombination and provide the active sites for O2 reduction which significantly enhances the photoactivity. Both uncalcined and calcined Au101/WO3 photocatalysts produce over 75 mM g-1 h-1 of H2O2 under UV light irradiation while the pure WO3 is inactive. At early times (up to 30 min), the production rate of H2O2 from calcined Au101/WO3 reaches 173 mM g-1 h-1 and is almost double the rate of the uncalcined catalyst (93 mM g-1 h-1). The higher photoactivity of calcined versus uncalcined Au101/WO3 can be attributed to the aggregated Au101 and removal of phosphine ligands from the Au core as verified by HRTEM and XPS. The reaction rate decreases over time which is attributed to the reverse reaction. Using a simple kinetic model, the rate constant of the H2O2 formation (kf) for uncalcined and calcined Au101/WO3 are 2.07 and 6.31 mM h-1, while the rate constant of the H2O2 decomposition (kd) for uncalcined and calcined Au101/WO3 are 0.49 and 2.93 h-1, respectively. This work highlights a simple preparation of highly active photocatalysts to produce H2O2 derived from Au101 clusters and WO3.

show abstract

Methanol Tolerant Oxygen Reduction Reaction Electrocatalysis using Size‐Specific Triphenylphosphine‐Ligated Gold Nanoclusters

Cited by 6 publications

References 50 publications

Scalable production of reduced graphene oxide via biowaste valorisation: an efficient oxygen reduction reaction towards metal-free electrocatalysis

Scalable production of reduced graphene oxide via biowaste valorisation: an efficient oxygen reduction reaction towards metal-free electrocatalysis

Photocatalytic H2O2 Production Over Photocatalysts Prepared By Phosphine-protected Au101 Nanoparticles on WO3

Photocatalytic H2O2 Production Over Photocatalysts Prepared By Phosphine-protected Au101 Nanoclusters on WO3

Contact Info

Product

Resources

About