The unexpected activity of Pd nanoparticles prepared using a non-ionic surfactant template

Abass, Nawal Al; Denuault, Guy; Pletcher, Derek

doi:10.1039/c3cp54531h

Cited by 20 publications

(6 citation statements)

References 24 publications

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“…1b). The anodic peaks at around 0.15 and 0.31 V vs. RHE can be assigned to H extraction (H ext ) from the lattice and H desorption (H des ) from the surface, respectively 26 . The oxidation peaks positioned at 0.97 and 0.69 V vs. RHE correspond to the oxidation of adsorbed CO at Pd(111) terrace and stepped sites 27–29 .…”

Section: Resultsmentioning

confidence: 99%

Cyclic two-step electrolysis for stable electrochemical conversion of carbon dioxide to formate

et al. 2019

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Pd metal and Pd-based alloys are ideal catalysts that allow for the electrochemical conversion of CO 2 to HCOO − at almost zero-overpotential with high selectivity, but catalyst degradation caused by concurrent CO poisoning limits their practical implementation. Here, we demonstrate that cyclic two-step electrolysis, by applying the reduction and oxidation potentials alternately, achieves 100% current density stability and 97.8% selectivity toward HCOO − production for at least 45 h. The key idea for achieving the reliability is based on the selective removal of CO by controlling the parameters during the oxidation step, which utilizes the different reversibility of HCOO − and CO production reactions. Furthermore, it is found that potentiostatic electrolysis causes CO adsorption and subsequent dehydridation, which in turn lowers HCOO − selectivity. Our work provides a system-level strategy for solving the poisoning issue that is inevitable in many electrocatalytic reactions.

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Section: Resultsmentioning

confidence: 99%

Cyclic two-step electrolysis for stable electrochemical conversion of carbon dioxide to formate

et al. 2019

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“…These characteristic voltammetric peaks located in the −0.3 V and +0.3 V window potential are mainly attributed to the electroadsorption/electrodesorption of hydrogen atoms preceding the HER reaction, which is overlapped with hydrogen absorption. 93,94 Therefore, after the attachment of PdNDs onto the SAM of 1, electron transfer through the organic monolayer takes place and, subsequently, the applied electrochemical potential is experienced by the outer PdND/electrolyte interface. Oxidative desorption of the SAM of 1 was also carried out ( Fig.…”

Section: Resultsmentioning

confidence: 99%

High surface coverage of a self-assembled monolayer by in situ synthesis of palladium nanodeposits

et al. 2017

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Nascent metal|monolayer|metal devices have been fabricated by depositing palladium, produced through a CO-confined growth method, onto a self-assembled monolayer of an amine-terminated oligo(phenylene ethynylene) derivative on a gold bottom electrode. The high surface area coverage (85%) of the organic monolayer by densely packed palladium particles was confirmed by X-ray photoemission spectroscopy (XPS) and atomic force microscopy (AFM). The electrical properties of these nascent Au|monolayer|Pd assemblies were determined from the I-V curves recorded with a conductive-AFM using the Peak Force Tunneling AFM (PF-TUNA™) mode. The I-V curves together with the electrochemical experiments performed rule out the formation of short-circuits due to palladium penetration through the monolayer, suggesting that the palladium deposition strategy is an effective method for the fabrication of molecular junctions without damaging the organic layer.

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“…Further-more, mesoporous Pd films show enhanced electrocatalytic performance for formic acid oxidation reaction by fully taking advantage of their large surface area. 10 Various synthetic methods, including hard templating from mesoporous silica or alumina, 11−13 dealloying, 14−16 and soft-templating, 6,10,17,18 have been developed to prepare mesoporous/nanoporous metals. Micelle assembly, typically involved in soft-templates, is flexible and convenient for the preparation of mesoporous metals under different conditions and greatly outperforms other methods.…”

Section: ■ Introductionmentioning

confidence: 99%

Continuous Mesoporous Pd Films by Electrochemical Deposition in Nonionic Micellar Solution

Iqbal

Wood

et al. 2017

Chem. Mater.

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Mesoporous metals that combine catalytic activity and high surface area can provide more opportunities for electrochemical applications. Various synthetic methods, including hard and soft templating, have been developed to prepare mesoporous/nanoporous metals. Micelle assembly, typically involved in soft-templates, is flexible and convenient for such purposes. It is, however, difficult to control, and the ordering is significantly destroyed during the metal deposition process, which is detrimental when it comes to designing precisely mesostructured materials. In the present work, mesoporous Pd films were uniformly electrodeposited using a nonionic surfactant, triblock copolymer poly(ethylene oxide)-b-poly(propylene oxide)-b-poly(ethylene oxide), as a pore-directing agent. The interaction between micelles and metal precursors greatly influences the metal growth and determines the final structure. The water-coordinated species interact with the ethylene oxide moiety of the micelles to effectively drive the Pd(II) species toward the working electrode surface. From small-angle neutron scattering data, it is found that spherical P123 micelles, with an average diameter of ∼14 nm, are formed in the electrolyte, and the addition of Pd ions does not significantly modify their structure, which is the essence of the micelle assembly approach. The uniformly sized mesopores are formed over the entire mesoporous Pd film and have an average pore diameter of 10.9 nm. Cross-sectional observation of the film also shows mesopores spanning continuously from the bottom to the top of the film. The crystallinity, crystal phase, and electronic coordination state of the Pd film are also confirmed. Through this study, it is found that the optimized surfactant concentration and applied deposition potential are the key factors to govern the formation of homogeneous and well-distributed pores over the entire film. Interestingly, the as-prepared mesoporous Pd films exhibit superior electrocatalytic activity toward the ethanol oxidation reaction by fully utilizing the accessible active surface area. Our approach combines electrochemistry with colloidal and coordination chemistry and is widely applicable to other promising metals and alloy electrocatalysts.

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The unexpected activity of Pd nanoparticles prepared using a non-ionic surfactant template

Cited by 20 publications

References 24 publications

Cyclic two-step electrolysis for stable electrochemical conversion of carbon dioxide to formate

Cyclic two-step electrolysis for stable electrochemical conversion of carbon dioxide to formate

High surface coverage of a self-assembled monolayer by in situ synthesis of palladium nanodeposits

Continuous Mesoporous Pd Films by Electrochemical Deposition in Nonionic Micellar Solution

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