Pd–Ir alloy as an anode material for borohydride oxidation

Merino-Jiménez, Irene; Janik, Michael J.; León, Carlos Ponce de; Walsh, Frank C.

doi:10.1016/j.jpowsour.2014.06.140

Cited by 47 publications

(26 citation statements)

References 35 publications

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“…stepwise reaction on platinum and compete with the electrooxidation. Such a CE mechanism (chemical reaction followed by electrochemical reaction) is reported by Gyenge (Reactions 5 and 6) while the product can further undergo electrooxidation yielding 6 electrons (7), hydrolysis reaction (8) or a combination of both (see Reactions 9 and 10) [1,7,10]:…”

Section: Introductionmentioning

confidence: 87%

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The electrooxidation of borohydride: A mechanistic study on palladium (Pd/C) applying RRDE, 11B-NMR and FTIR

Grimmer

Grandi

Zacharias

et al. 2016

Applied Catalysis B: Environmental

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Section: Introductionmentioning

confidence: 87%

“…There is little literature concerning the reaction mechanism on palladium but several authors assume similar reaction steps to platinum catalysts [7][8][9]. The hydrolysis is reported to undergo a http://dx.doi.org/10.1016/j.apcatb.2015.07.028 0926-3373/© 2015 Elsevier B.V. All rights reserved.…”

Section: Introductionmentioning

confidence: 99%

The electrooxidation of borohydride: A mechanistic study on palladium (Pd/C) applying RRDE, 11B-NMR and FTIR

Grimmer

Grandi

Zacharias

et al. 2016

Applied Catalysis B: Environmental

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“…13 Our mechanistic studies [10][11] of the BOR over the Au(111) surface concluded that the unfavorable borohydride adsorption and low activity for breaking B-H bonds causes low activity and large overpotentials. Alternatively, very exothermic, dissociative adsorption of BH 4 -ions over the platinum surface produces a large surface coverage of hydrogen.…”

Section: Introductionmentioning

confidence: 87%

“…Carbon supported palladium and copper nanoparticles were also considered for BOR and show better performance than pure palladium nanoparticles. 21 DFT studies were also performed on Pd-Ir alloys for BOR, 13 suggesting that the presence of Ir favored borohydride oxidation rather than the hydrogen evolution and increased the number of electrons released from the BOR when the concentration of Ir was increased.…”

Section: Introductionmentioning

confidence: 99%

Electrocatalyst Design for Direct Borohydride Oxidation Guided by First Principles

Rostamikia¹,

Patel²,

Merino-Jiménez

et al. 2017

J. Phys. Chem. C

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Density functional theory (DFT) calculations are used to propose a Au–Cu binary metal catalyst for the electrochemical borohydride oxidation reaction (BOR), which is evaluated experimentally and observed to show enhanced oxidation activity relative to a pure Au electrode. Our previous work has applied DFT methods to determine the BOR mechanism and elucidate the key reaction steps that dictate catalyst activity and selectivity to complete oxidation. A balanced initial adsorption strength of the borohydride anion is essential for an active and selective catalyst. Adsorption must be strong enough to provide a reasonable coverage of surface species and promote B–H bond dissociation but not so strong as to promote easy dissociation and provide a high coverage of surface H atoms that result in H2 evolution. Borohydride adsorption energetics were evaluated for a series of close-packed pure metal surfaces. Copper catalysts appear encouraging but are not electrochemically stable under reaction conditions. Gold–copper alloys are predicted to show increased activity compared to a pure gold electrode while maintaining the selectivity to direct oxidation and increasing the stability compared to pure Cu. DFT results suggest an approximately 0.2 V decrease in the overpotential for borohydride oxidation on a Au2Cu(111) electrode compared to that on a Au(111) electrode. This DFT-predicted reduction in overpotential is realized experimentally. Electrodeposition was used to prepare AuCu electrodes, and their borohydride oxidation electrokinetics were examined by linear sweep voltammetry. An 88.5% gold and 11.5% copper sample demonstrated an overpotential reduction of 0.17 V compared to a pure Au electrode. The binding energy and adsorption free energy of BH4 – over other surface alloys are also examined to further identify promising BOR electrodes.

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“…Consequently, iridium has been successfully used to improve the durability of Pd-Co, Pd-Cu and Pd-Ce catalysts [15][16][17]. Though palladium-iridium bimetallic nanocrystals have been used as electro-catalysts for formic acid/borohydride/CO oxidation, little work has been focused on their electro-catalytic activities towards ORR [18][19][20]. In addition, previously reported Pd-Ir bimetallic nanoparticles were universally spherical in shape with very small size.…”

Section: Accepted Manuscriptmentioning

confidence: 99%

Palladium–iridium nanowires for enhancement of electro-catalytic activity towards oxygen reduction reaction

Yang

Huang

et al. 2015

Electrochemistry Communications

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Pd–Ir alloy as an anode material for borohydride oxidation

Cited by 47 publications

References 35 publications

The electrooxidation of borohydride: A mechanistic study on palladium (Pd/C) applying RRDE, 11B-NMR and FTIR

The electrooxidation of borohydride: A mechanistic study on palladium (Pd/C) applying RRDE, 11B-NMR and FTIR

Electrocatalyst Design for Direct Borohydride Oxidation Guided by First Principles

Palladium–iridium nanowires for enhancement of electro-catalytic activity towards oxygen reduction reaction

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