Suppressing H<sub>2</sub>O<sub>2</sub> formation in the oxygen reduction reaction using Co-doped copper oxide electrodes

Biswal, Sekhar Kumar; Ranjan, Chinmoy

doi:10.1039/d2ta04349a

Cited by 5 publications

(5 citation statements)

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“…The behavior is not dissimilar to earlier reported Cu[Co]Ox/Au catalyst. 9 The low and steady H2O2 yield from Cu0.8Ni0.2Ox/Au electrode over a large potential range makes it an attractive material for fuel cell ORR electrodes since fluctuations in power are less likely to change H2O2 yields, allowing for predictable device performance. We subjected the Cu0.8Ni0.2Ox/Au electrode to 3000 potential cycles between 0.6 and 1V (a potential range relevant for fuel cells).…”

Section: Methodsmentioning

confidence: 99%

“…Previously, we have seen that in Cu[Co]Ox/Au systems, such steps can be energetically boosted due to higher oxygen binding energy at M* sites due to high amounts of unsaturation present in these doped systems. 9 a chemical rate-limiting step preceded by a fast preequilibrium step. We have previously hypothesized that this could be O-O bond cleavage step preceded by MOOH* formation.…”

Section: S15(a B)mentioning

confidence: 99%

“…We have previously hypothesized that this could be O-O bond cleavage step preceded by MOOH* formation. 9 The combination of Cu and Ni oxides is likely to generate undercoordinated and stressed Ni sites that bind to oxygen more strongly than the pristine counterparts, enabling better O-O cleavage. This study demonstrates that it is feasible to design ORR catalysts based on the idea of mixing metals that have different natural preferences for oxygen coordination.…”

Section: S15(a B)mentioning

confidence: 99%

“…We have previously reported Cu[Co]Ox/Au catalysts, which demonstrated excellent ORR activity and suppressed H2O2 yields. 9 The idea was based on combining two metal ions with differing preferences for oxygen coordination environments within a composite framework, which can lead to substantial structural stress. The outcome of this process can sometimes lead to optimum modulation of the binding of the OOH* intermediate and the preference for four-electron reduction routes.…”

Section: Introductionmentioning

confidence: 99%

“…The outcome of this process can sometimes lead to optimum modulation of the binding of the OOH* intermediate and the preference for four-electron reduction routes. 9 We have now developed a Cu…”

Section: Introductionmentioning

confidence: 99%

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Ni-doped Cu oxide catalysts for ORR: suppressing H2O2 formation by engineering chemical strain

Biswal,

ranjan

2024

Preprint

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Ni-doped copper oxide (Cu[Ni]Ox/Au) has demonstrated considerable promise towards efficient oxygen reduction reaction (ORR) under alkaline conditions. The Cu-rich samples like Cu0.8Ni0.2Ox/Au show better activity and selectivity than benchmarks such as Pt and Au, exhibiting H2O2 yields < 5% throughout a large potential range. The electrode's performance did not degrade even under 3000 potential cycles under ORR conditions. In-situ Raman spectroscopy indicated a Cu-O-Ni type framework where Ni doping into CuOx results in coordinatively unsaturated Ni centers within the Cu-O-Ni framework. These centers are active towards easier cleavage of O-O bonds resulting in an overall preference for the 4e pathway for O2 reduction to H2O.

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Section: Methodsmentioning

confidence: 99%

Section: S15(a B)mentioning

confidence: 99%

Section: S15(a B)mentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Ni-doped Cu oxide catalysts for ORR: suppressing H2O2 formation by engineering chemical strain

Biswal,

ranjan

2024

Preprint

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Cu Embedded in Co–P Nanosheets with Super Wetting Structure for Accelerated Overall Water Splitting under Simulated Industrial Conditions

Deng,

Zhang

2024

Advanced Energy Materials

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The development of advanced electrocatalysts with exceptional performance at high current densities is pivotal for reducing electric energy consumption in industrial water splitting for hydrogen production. Herein, a flexible one‐step electrodeposition approach is developed to synthesize superhydrophilic 3D flower‐like clusters of Cu–Co–P nanosheets grown in situ on nickel foam (NF). Introducing Cu into Co–P causes strong electron interactions, forming an electronic configuration favorable for the adsorption and desorption of intermediates, which significantly improves the intrinsic catalytic activity. The as‐deposited Cu–Co–P/NF display notable bifunctional catalytic activity with low overpotentials of 259 and 65 mV for the oxygen and hydrogen evolution reactions, respectively, at 10 mA cm−2. Superwetting 3D flower‐like nanostructures are conducive to the penetration of electrolytes and the rapid release of bubbles, enabling the efficient utilization of active sites and the timely release of bubble stress under high current densities. An assembled Cu–Co–P/NF(+, −) electrolyzer achieves an impressive voltage of 1.85 V at 500 mA cm−2 for water splitting and appreciable stability for over 220 h under simulated industrial conditions. This work offers an attractive strategy for regulating superaerophobic Co–P electrocatalysts for industrial water splitting, which can contribute to practical applications.

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Ligand‐Driven Electron‐Deficient Cobalt Pentlandite Nanocrystals for Efficient Hydrogen Peroxide Electrosynthesis

Kim,

Lee,

Kim

et al. 2024

Energy & Environ Materials

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Cobalt pentlandite (Co9S8) is a promising non‐precious catalyst due to its superior oxygen reduction reaction activity and excellent stability. However, its oxygen reduction reaction catalytic activity has traditionally been limited to the four‐electron pathway because of strong *OOH intermediate adsorption. In this study, we synthesized electron‐deficient Co9S8 nanocrystals with an increased number of Co3+ states compared to conventional Co9S8. This was achieved by incorporating a high density of surface ligands in small‐sized Co9S8 nanocrystals, which enabled the transition of the electrochemical reduction pathway from four‐electron oxygen reduction reaction to two‐electron oxygen reduction reaction by decreasing *OOH adsorption strength. As a result, the Co3+‐enriched Co9S8 nanocrystals exhibited a high onset potential of 0.64 V (vs RHE) for two‐electron oxygen reduction reaction, achieving H2O2 selectivity of 70–80% over the potential range from 0.05 to 0.6 V. Additionally, these nanocrystals demonstrated a stable H2O2 electrosynthesis at a rate of 459.12 mmol g−1 h−1 with a H2O2 Faradaic efficiency over 90% under alkaline conditions. This study provides insights into nanoscale catalyst design for modulating electrochemical reactions.

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Suppressing H₂O₂ formation in the oxygen reduction reaction using Co-doped copper oxide electrodes

Abstract: Transition metal oxides form the basis of promising oxygen reduction electrocatalysts due to their low cost, high activity, and abundance on the planet. A new class of Co-doped CuOx (Cu[Co]Ox/Au)...

Cited by 5 publications

References 63 publications

Ni-doped Cu oxide catalysts for ORR: suppressing H2O2 formation by engineering chemical strain

Ni-doped Cu oxide catalysts for ORR: suppressing H2O2 formation by engineering chemical strain

Cu Embedded in Co–P Nanosheets with Super Wetting Structure for Accelerated Overall Water Splitting under Simulated Industrial Conditions

Ligand‐Driven Electron‐Deficient Cobalt Pentlandite Nanocrystals for Efficient Hydrogen Peroxide Electrosynthesis

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Suppressing H2O2 formation in the oxygen reduction reaction using Co-doped copper oxide electrodes

Abstract: Transition metal oxides form the basis of promising oxygen reduction electrocatalysts due to their low cost, high activity, and abundance on the planet. A new class of Co-doped CuOx (Cu[Co]Ox/Au)...

Cited by 5 publications

References 63 publications

Ni-doped Cu oxide catalysts for ORR: suppressing H2O2 formation by engineering chemical strain

Ni-doped Cu oxide catalysts for ORR: suppressing H2O2 formation by engineering chemical strain

Cu Embedded in Co–P Nanosheets with Super Wetting Structure for Accelerated Overall Water Splitting under Simulated Industrial Conditions

Ligand‐Driven Electron‐Deficient Cobalt Pentlandite Nanocrystals for Efficient Hydrogen Peroxide Electrosynthesis

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Suppressing H₂O₂ formation in the oxygen reduction reaction using Co-doped copper oxide electrodes