Highly mixed high-energy d-orbital states enhance oxygen evolution reactions in spinel catalysts

Santhosh Kumar, Ramasamy; Muthu Austeria, P.; Sagaya Selvam Neethinathan, Clament; Ramakrishnan, S.; Sekar, Karthikeyan; Kim, Ae Rhan; Kim, Do Hwan; Yoo, Pil J.; Yoo, Dong Jin

doi:10.1016/j.apsusc.2023.158469

Applied Surface Science

2023

DOI: 10.1016/j.apsusc.2023.158469

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Highly mixed high-energy d-orbital states enhance oxygen evolution reactions in spinel catalysts

Ramasamy Santhosh Kumar,

P. Muthu Austeria,

Clament Sagaya Selvam Neethinathan

et al.

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2024

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Cited by 19 publications

References 73 publications

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Synthesis and Evaluation of Reduced Graphene Oxide (rGO) Supported on Ni₃O₄ as Spinel‐Based Cathode Catalyst for the Effective Anion‐Exchange Membrane Fuel Cell Application

Santhosh Kumar,

Gokulapriyan,

Sakthivel

et al. 2024

ChemCatChem

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Oxygen reduction reaction (ORR) stability and catalytic activity in high‐durability anion exchange membrane fuel cells (AEMFCs) can be improved using graphene‐supported spinel‐based Ni3O4 cathode catalysts. Here, we describe a simple and economical hydrothermal method for synthesizing reduced graphene oxide (rGO) supported on Ni3O4. The atomic‐level contribution of the Ni‐Ni and Ni‐O bonds to the chemical structure of nickel oxide was confirmed by X‐ray photoelectron and absorption spectroscopy analyses. Due to the force of the void for oxygen created by nickel atoms, Ni3O4@rGO for the ORR exhibited enhanced stability and catalytic activity (E1/2 = 0.761 V and over 30,000 CV cycles). A single AEMFC cell achieved the greatest power density and long‐term durability using a Ni3O4@rGO cathode, suggesting superior endurance despite the minimal voltage decrease (power density 29.6 mW cm‐2, endurance for 25h). These findings offer insights and point to opportunities for developing metal oxide–based AEMFCs.

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Synthesis and Evaluation of Reduced Graphene Oxide (rGO) Supported on Ni₃O₄ as Spinel‐Based Cathode Catalyst for the Effective Anion‐Exchange Membrane Fuel Cell Application

Santhosh Kumar,

Gokulapriyan,

Sakthivel

et al. 2024

ChemCatChem

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Boosting the Production of Hydrogen from an Overall Urea Splitting Reaction Using a Tri‐Functional Scandium–Cobalt Electrocatalyst

Tamilarasi,

Kumar,

Kim

et al. 2024

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The creation of highly efficient and economical electrocatalysts is essential to the massive electrolysis of water to produce clean energy. The ability to use urea reaction of oxidation (UOR) in place of the oxygen/hydrogen evolution process (OER/HER) during water splitting is a significant step toward the production of high‐purity hydrogen with less energy usage. Empirical evidence suggests that the UOR process consists of two stages. First, the metal sites undergo an electrochemical pre‐oxidation reaction, and then the urea molecules on the high‐valence metal sites are chemically oxidized. Here, the use of scandium‐doped CoTe supported on carbon nanotubes called Sc@CoTe/CNT is reported and CoTe/CNT as a composite to efficiently promote hydrogen generation from highly durable and active electrocatalysts for the OER/UOR/HER in urea and alkali solutions. Electrochemical impedance spectroscopy indicates that the UOR facilitates charge transfer across the interface. Furthermore, the Sc@CoTe/CNT nanocatalyst has high performance in KOH and KOH‐containing urea solutions as demonstrated by the HER, OER, and UOR (215 mV, 1.59, and 1.31 V, respectively, at 10 mA cm−2 in 1 m KOH) and CoTe/CNT shows 195 mV, 1.61 and 1.3 V, respectively. Consequently, the total urea splitting system achieves 1.29 V, whereas the overall water splitting device obtaines 1.49 V of Sc@CoTe/CNT and CoTe/CNT shows 1.54, 1.48 V, respectively. This work presents a viable method of combining HER with UOR for maximally effective hydrogen production.

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Bamboo‐Like Carbon Nanotube‐Encapsulated Fe₂C Nanoparticles Activate Confined Fe₂O₃ Nanoclusters Via d‐p‐d Orbital Coupling for Alkaline Oxygen Evolution Reaction

Chen,

Xu,

Wang

et al. 2024

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The efficient anion exchange membrane water electrolysis is challenging with low cell voltage and long‐term stability at large current density, due to the unstable anodic oxygen evolution reaction (OER). Fe‐based electrocatalysts are potential candidates for the anodic OER. In Fe‐based materials, iron oxides always show better stability in alkaline solution but lower OER activity. However, the catalysts in previous study are difficult to continuously and effectively activate iron oxides supported on carbon during electrocatalysis. Herein, a new class of electrocatalyst: bamboo‐like carbon nanotubes (B‐CNT)‐encapsulated Fe2C nanoparticles (NPs) supported Fe2O3 nanoclusters (NCs), named Fe2O3/B‐CNT@Fe2C is reported. Theoretical calculations and experimental results reveal that B‐CNT‐encapsulate Fe2C NPs activate Fe2O3 NCs by the d‐p‐d orbital coupling, thereby weakening the adsorption of OOH* intermediate during OER process. The electrolyzer based on the electrocatalyst requires only 1.48 V to reach 1.0 A cm−2 and shows a long‐term stability at 1.0 A cm−2 for 1600 h, comparable to the best‐reported values for the anion exchange membrane water electrolyzer (AEMWE).

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Highly mixed high-energy d-orbital states enhance oxygen evolution reactions in spinel catalysts

Cited by 19 publications

References 73 publications

Synthesis and Evaluation of Reduced Graphene Oxide (rGO) Supported on Ni₃O₄ as Spinel‐Based Cathode Catalyst for the Effective Anion‐Exchange Membrane Fuel Cell Application

Synthesis and Evaluation of Reduced Graphene Oxide (rGO) Supported on Ni₃O₄ as Spinel‐Based Cathode Catalyst for the Effective Anion‐Exchange Membrane Fuel Cell Application

Boosting the Production of Hydrogen from an Overall Urea Splitting Reaction Using a Tri‐Functional Scandium–Cobalt Electrocatalyst

Bamboo‐Like Carbon Nanotube‐Encapsulated Fe₂C Nanoparticles Activate Confined Fe₂O₃ Nanoclusters Via d‐p‐d Orbital Coupling for Alkaline Oxygen Evolution Reaction

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Highly mixed high-energy d-orbital states enhance oxygen evolution reactions in spinel catalysts

Cited by 19 publications

References 73 publications

Synthesis and Evaluation of Reduced Graphene Oxide (rGO) Supported on Ni3O4 as Spinel‐Based Cathode Catalyst for the Effective Anion‐Exchange Membrane Fuel Cell Application

Synthesis and Evaluation of Reduced Graphene Oxide (rGO) Supported on Ni3O4 as Spinel‐Based Cathode Catalyst for the Effective Anion‐Exchange Membrane Fuel Cell Application

Boosting the Production of Hydrogen from an Overall Urea Splitting Reaction Using a Tri‐Functional Scandium–Cobalt Electrocatalyst

Bamboo‐Like Carbon Nanotube‐Encapsulated Fe2C Nanoparticles Activate Confined Fe2O3 Nanoclusters Via d‐p‐d Orbital Coupling for Alkaline Oxygen Evolution Reaction

Contact Info

Product

Resources

About

Synthesis and Evaluation of Reduced Graphene Oxide (rGO) Supported on Ni₃O₄ as Spinel‐Based Cathode Catalyst for the Effective Anion‐Exchange Membrane Fuel Cell Application

Synthesis and Evaluation of Reduced Graphene Oxide (rGO) Supported on Ni₃O₄ as Spinel‐Based Cathode Catalyst for the Effective Anion‐Exchange Membrane Fuel Cell Application

Bamboo‐Like Carbon Nanotube‐Encapsulated Fe₂C Nanoparticles Activate Confined Fe₂O₃ Nanoclusters Via d‐p‐d Orbital Coupling for Alkaline Oxygen Evolution Reaction