Selective electrocatalysis imparted by metal–insulator transition for durability enhancement of automotive fuel cells

Jung, Sang‐Mun; Yun, Su-Won; Kim, Jun‐Hyuk; You, Sang‐Hoon; Park, Jinheon; Lee, Seonggyu; Chang, Seo Hyoung; Chae, Seung Chul; Joo, Sang Hoon; Jung, Yousung; Lee, Jun Young; Son, Junwoo; Snyder, Joshua; Stamenković, Vojislav R.; Marković, Nenad M.; Kim, Yong‐Tae

doi:10.1038/s41929-020-0475-4

Cited by 84 publications

(65 citation statements)

References 56 publications

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“…Fuel cells are promising renewable energy devices for advanced portable electronic devices and electrical vehicles. [ 1,2 ] They can convert chemical energy into electrical power via the electrocatalytic processes including the methanol oxidation reaction (MOR), [ 3 ] ethanol oxidation reaction, [ 4 ] oxygen reduction reaction (ORR), [ 5 ] hydrogen oxidation reaction (HOR), [ 6 ] etc. To date, platinum (Pt) is still considered as the most promising and commonly used electrocatalyst in fuel cells.…”

Section: Introductionmentioning

confidence: 99%

“…To date, platinum (Pt) is still considered as the most promising and commonly used electrocatalyst in fuel cells. [ 1–6 ] However, the insufficient activity, inadequate durability, and the high cost and scarcity of Pt hinder the practical large‐scale commercialization of fuel cells.…”

Section: Introductionmentioning

confidence: 99%

“…[ 3–14 ] One strategy is alloying Pt with nonprecious transition metals (e.g., Fe, Co, Ni, and Cu), to improve the intrinsic catalytic activity via ligand and strain effects through modifying the electronic environment of Pt surface atoms. [ 4–8,11 ] Another strategy is maximizing the utilization efficiency of Pt atoms by designing hollow and porous nanostructures or reducing particle size in the Pt‐based nanocatalysts, such as nanoframes, [ 8 ] nanocages, [ 5,12 ] ultrafine nanowire, [ 10,13 ] or even single atom Pt, [ 14 ] etc. Generally, these Pt‐based nanocatalysts are supported on carbon black with high electrical conductivity and high surface area to achieve a uniform dispersion and obtain high activity and high stability.…”

Section: Introductionmentioning

confidence: 99%

“…Generally, these Pt‐based nanocatalysts are supported on carbon black with high electrical conductivity and high surface area to achieve a uniform dispersion and obtain high activity and high stability. [ 4–13 ] Unfortunately, carbon corrosion problems frequently happen in the acidic electrolyte under the high operation potential (>1.0 V RHE ) caused by start‐up/shut‐down (SUSD) sequences of fuel cells, leading to pronounced detachment of the Pt‐based nanocatalysts and low long‐term durability during the practical operation of fuel cells. [ 15,16 ]…”

Section: Introductionmentioning

confidence: 99%

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Boosting Both Electrocatalytic Activity and Durability of Metal Aerogels via Intrinsic Hierarchical Porosity and Continuous Conductive Network Backbone Preservation

Zheng

Yang

et al. 2020

Advanced Energy Materials

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As an emerging class of highly and hierarchically porous materials with continuous conductive metal network backbones, metal aerogels have unleashed tremendous potential in various fields, especially in electrocatalysis. However, it remains a great challenge to maximize the utilization of the intrinsic structural advantages of metal aerogels due to the collapse of their structure during conventional electrode preparation caused by their brittle character. Herein, a general in situ silicone‐confined gelation strategy is developed to integrate metal aerogels (PtPd, PtAg, PdAg, and AuAg) into/onto macroporous skeletons (carbon cloth, carbon fiber foam, and nickel foam). The composite materials have good mechanical flexibility, and can be utilized directly under the condition of well‐preserved intrinsic structure of metal aerogels. This not only results in more efficient electron transfer and faster mass transport, but also eliminates Ostwald ripening and aggregation, leading to both remarkably enhanced activity and durability when compared to that made by conventional ink drop coating with collapsed and compressed structure. This work represents a significant breakthrough for metal aerogels, and provides inspiration for electrocatalyst design with both high activity and durability.

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Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

See 2 more Smart Citations

Boosting Both Electrocatalytic Activity and Durability of Metal Aerogels via Intrinsic Hierarchical Porosity and Continuous Conductive Network Backbone Preservation

Zheng

Yang

et al. 2020

Advanced Energy Materials

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“…In polymer electrolyte membrane (PEM) fuel cell operation, fuel starvation occurring at the anode side leads to a voltage reversal phenomenon, causing corrosion of carbon components like catalyst support, gas diffusion layer (GDL) and ow eld plate on the anode 8,9 . A recent study proposed to reduce the damage to the electrode by selectively promoting HOR catalysts by suppressing ORR 10 and introducing a water oxidation catalyst to the anode of the PEM fuel cell to induce an OER, as it is a reaction compete with the carbon corrosion reaction 9 . In this regard, multifunctional catalysts can be a promising strategy in environments where the electrochemical reaction changes rapidly, such as the voltage reversal of water electrolysis and PEM fuel cell systems.…”

Section: Introductionmentioning

confidence: 99%

Reversible Ir-based multifunctional electrocatalyst for durable water splitting and fuel cell systems

Lee

Kim

et al. 2020

Preprint

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The voltage reversal of water electrolyzers and fuel cells induces a large positive potential on the hydrogen electrodes, followed by severe system degradation. Applying a reversible multifunctional electrocatalyst to the hydrogen electrode is a practical solution. Ir exhibits excellent catalytic reactivity for hydrogen evolution reactions (HER), and hydrogen oxidation reactions (HOR) around 0 V/RHE, yet irreversibly converts to amorphous IrOx at potentials > 0.8 V/RHE, which is an excellent catalyst for oxygen evolution reactions (OER), yet a poor HER and HOR catalyst. Harnessing these multifunctional catalytic characteristics, we designed a unique Ir-based electrocatalyst for OER, HER, and HOR. Under OER operation, the crystalline nanoparticle catalyst generates an atomically-thin, highly active IrOx layer, which reversibly transforms into a metallic Ir surface at more cathodic electrode potentials, restoring high catalytic activity for HER and HOR. Our analysis reveals that a metallic Ir subsurface to the thin IrOx surface layer can act as a catalytic substrate for the reduction of the dissolved Ir ion, creating reversibility. Our work not only uncovers new fundamental, uniquely reversible catalytic properties of nanoparticle catalysts, but also offers a practical materials-based solution to catalyst layer degradation of electrochemical energy conversion devices.

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Anion Constructor for Atomic‐Scale Engineering of Antiperovskite Crystals for Electrochemical Reactions

Lee

Jung

Jang

et al. 2021

Adv Funct Materials

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Among the Pt group metals, Pd has been considered the most efficient for application in electrocatalysts as an alternative to Pt. Despite the comparable electrochemical activities of Pd and Pd‐metal alloys, they are vulnerable to liquid acidic electrolytes, leading to degradation of catalytic activity. Pd–Ni alloys have been used to enhance catalytic activity because the electronic structure of Pd can be easily changed by adding Ni. In other studies, N atoms have been introduced for more stable M–Ni catalysts by inducing the formation of Ni4N species; however, the structural analysis and the role of nitrogen have not been fully understood yet. Herein, the Pd–Ni alloy nitride with a unique crystal structure shows a promising catalytic activity for oxygen reduction reaction (ORR). The nitride PdNi nanoparticles have a novel monolithic antiperovskite structure of chemical formula (PdxNi1−x)NNi3. The unique antiperovskite crystal (PdxNi1−x)NNi3 possesses superior ORR activity and stability, originating from the downshifted d‐band center of the monolayer Pd/antiperovskite surface and the lower formation energy of the antiperovskite core nanocrystal. Consequently, (PdxNi1−x)NNi3, as a Pt‐free Pd‐based electrocatalyst, overcomes the stability issue of Pd under acidic conditions by achieving 99‐times higher mass activity than commercial Pd/C, as shown by the durability test.

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Selective electrocatalysis imparted by metal–insulator transition for durability enhancement of automotive fuel cells

Cited by 84 publications

References 56 publications

Boosting Both Electrocatalytic Activity and Durability of Metal Aerogels via Intrinsic Hierarchical Porosity and Continuous Conductive Network Backbone Preservation

Boosting Both Electrocatalytic Activity and Durability of Metal Aerogels via Intrinsic Hierarchical Porosity and Continuous Conductive Network Backbone Preservation

Reversible Ir-based multifunctional electrocatalyst for durable water splitting and fuel cell systems

Anion Constructor for Atomic‐Scale Engineering of Antiperovskite Crystals for Electrochemical Reactions

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