Insights in the Oxygen Reduction Reaction: From Metallic Electrocatalysts to Diporphyrins

Wan, Hao; Jensen, Annie Aarup; Escudero-Escribano, Marı́a; Rossmeisl, Jan

doi:10.1021/acscatal.0c01085

Cited by 64 publications

(75 citation statements)

References 106 publications

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“…11,13 A promising strategy towards this goal is the confinement of *OOH within a 3-D active site environment, which has been demonstrated for a few model systems and homogenous molecular catalysts. For instance, Rossmeisl et al 14,15 have shown that diporphyrin motifs are capable of facilitating *OOH dissociation via two closely-spaced binding sites. This approach bypasses the limitations imposed by *OOH scaling in favor of the less restrictive dissociated *O + *OH pathway.…”

mentioning

confidence: 99%

Circumventing Scaling Relations in Oxygen Electrochemistry Using Metal–Organic Frameworks

Sours

Patel

Nørskov

et al. 2020

J. Phys. Chem. Lett.

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It has been well-established that unfavorable scaling relationships between *OOH, *OH, and *O are responsible for the high overpotentials associated with oxygen electrochemistry. A number of strategies have been proposed for breaking these linear constraints for traditional electrocatalysts (e.g., metals, alloys, metal-doped carbons); such approaches have not yet been validated experimentally for heterogeneous catalysts. Development of a new class of catalysts capable of circumventing such scaling relations remains an ongoing challenge in the field. In this work, we use density functional theory (DFT) calculations to demonstrate that bimetallic porphyrin-based MOFs (PMOFs) are an ideal materials platform for rationally designing the 3-D active site environments for oxygen reduction reaction (ORR). Specifically, we show that the *OOH binding energy and the theoretical limiting potential can be optimized by appropriately tuning the transition metal active site, the oxophilic spectator, and the MOF topology. Our calculations predict theoretical limiting potentials as high as 1.07 V for Fe/Cr-PMOF-Al, which exceeds the Pt/C benchmark for 4e ORR. More broadly, by highlighting their unique characteristics, this work aims to establish bimetallic porphyrin-based MOFs as a viable materials platform for future experimental and theoretical ORR studies.

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mentioning

confidence: 99%

Circumventing Scaling Relations in Oxygen Electrochemistry Using Metal–Organic Frameworks

Sours

Patel

Nørskov

et al. 2020

J. Phys. Chem. Lett.

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Δ {normalG}_{HO*}

, in light blue) and HOO* intermediates (

Δ {normalG}_{HOO*}

, in blue), as a function of

Δ {normalG}_{O*}

for metal (100) surfaces.…”

Section: Fundamentals Of Orr Electrocatalysismentioning

confidence: 99%

Engineering the Electrochemical Interface of Oxygen Reduction Electrocatalysts with Ionic Liquids: A Review

Favero

Stephens

Titirici

2020

Adv Energy and Sustain Res

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Hydrogen fuel cells are a promising technology for the environmentally sustainable production of electricity. However, their commercialization is hindered by the sluggish kinetics of the oxygen reduction reaction and by the high cost of the state‐of‐the‐art platinum catalysts. To address these challenges, research has focused on the enhancement of the activity of platinum and platinum group metal (PGM)‐free electrocatalysts, by modifying their composition and topology. Recently, a new approach has emerged to boost the activity of ORR catalysts, based on engineering the electrochemical interface. Herein, the recent developments in the use of ionic liquids (ILs) to modify the triple‐point interface of ORR catalysts are summarized. In this review, the current understanding in the literature of the effect of IL layers is presented, along with the open questions and remaining challenges. A short perspective on the applicability of this simple and effective modification to other electrochemical reactions is discussed.

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“…[ 1,2 ] However, the sluggish kinetics of the cathodic oxygen reduction reaction (ORR) is a key factor, determining the energy conversion efficiency of these devices. [ 3,4 ] Although platinum (Pt) and its alloy nanoparticles have proved to be the most effective and viable catalysts for ORR, its high price, low stability, and scarcity extremely hamper the commercial application. [ 5,6 ] Therefore, the exploration of non‐noble metal catalysts with excellent electrocatalytic activity, high durability, and wide‐available resources for ORR is highly desirable.…”

Section: Introductionmentioning

confidence: 99%

Design of Co Nanoparticles‐Encapsulated by Boron and Nitrogen Co‐Doped Carbon Nanosheets as Highly Efficient Electrocatalyst for Oxygen Reduction Reaction

Niu

Sun

Wang

et al. 2021

Adv Materials Inter

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In this paper, for the first time, a rationally designed strategy for synthesis of Co nanoparticles encapsulated by boron and nitrogen co‐doped carbon nanosheets (CNs), namely B, N‐Co/CNs, as highly efficient electrocatalyst for oxygen reduction reaction (ORR) is demonstrated. The generated Co nanoparticles not only create well‐defined heterointerfaces with high conductivity to overcome the poor ORR activity but also promote the formation of robust graphitic carbon. The co‐existence of boron and nitrogen atoms can increase the highest occupied molecular orbital energy of sp2 hybridization, activating π electrons in graphitic CNs, thereby enhancing the activity of the catalyst. The B, N‐Co/CNs exhibit a comparable half‐wave potential (E1/2 = 0.83 V) to that of commercial Pt/C catalyst (E1/2 = 0.85 V) with a larger current density for ORR. Importantly, the homemade disposable Zn‐air battery (ZAB) is able to deliver excellent performance, including a peak power density of 93.93 mW cm−2 and a specific capacity of 727.5 mAh g−1, outperforming the Pt/C catalyst. The findings highlight a new guideline for constructing B, N‐Co/CNs catalyst with a rationally designed structure toward superior property for advanced metal‐air cathode materials.

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Insights in the Oxygen Reduction Reaction: From Metallic Electrocatalysts to Diporphyrins

Cited by 64 publications

References 106 publications

Circumventing Scaling Relations in Oxygen Electrochemistry Using Metal–Organic Frameworks

Circumventing Scaling Relations in Oxygen Electrochemistry Using Metal–Organic Frameworks

Engineering the Electrochemical Interface of Oxygen Reduction Electrocatalysts with Ionic Liquids: A Review

Design of Co Nanoparticles‐Encapsulated by Boron and Nitrogen Co‐Doped Carbon Nanosheets as Highly Efficient Electrocatalyst for Oxygen Reduction Reaction

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