Tailored Ni(OH)2/CuCo/Ni(OH)2 Composite Interfaces for Efficient and Durable Urea Oxidation Reaction

Sahanaz Parvin; Emmanuel Aransiola; Mohamed Ammar; Seunghoon Lee; Lihua Zhang; Juliane Weber; Jonas Baltrusaitis

doi:10.1021/acsami.4c14041

Tailored Ni(OH)₂/CuCo/Ni(OH)₂ Composite Interfaces for Efficient and Durable Urea Oxidation Reaction

Sahanaz Parvin, Emmanuel Aransiola, Mohamed Ammar, Seunghoon Lee, Lihua Zhang, Juliane Weber, Jonas Baltrusaitis

Geochemistry & Interfacial Science

Research output: Contribution to journal › Article › peer-review

3 Scopus citations

Abstract

Electrocatalytic urea oxidation reaction is a promising alternative to water oxidation for more efficient hydrogen production due to its significantly lower thermodynamic potential. However, achieving efficient electrochemical urea oxidation remains a formidable challenge, and development of an improved electrocatalyst with an optimal physicochemical and electronic structure toward urea oxidation is desired. This can be accomplished by designing a tailored two-dimensional composite with an abundance of active sites in a favorable electronic environment. In this study, we demonstrate the fabrication of a self-supported, electrochemically grown metal/mixed metal hydroxide composite interface via a two-step electrodeposition method. Specifically, Ni(OH)₂ was electrodeposited on the top of the CuCo layer (Ni(OH)₂/CuCo/Ni(OH)₂), and the resultant 2D composite structure required 1.333 ± 0.006 V to oxidize urea electrochemically to achieve a current density of 10 mA cm^-2, which outperformed the potential required for individual components, Ni(OH)₂ and CuCo. The high density of Ni³⁺ active sites in the composite structure facilitated high electrocatalyst activity and stability. Ni(OH)₂/CuCo/Ni(OH)₂ was stable for at least 50 h without any noticeable degradation in the activity or alteration of the morphology. As a bifunctional electrocatalyst, the material also exhibited excellent performance for water oxidation with 260 mV overpotential and 50 h stability. In a two-electrode configuration coupled with a NiMo cathode catalyst, the electrolyzer required 1.42 V cell voltage for overall urea splitting. Overall, the engineered Ni(OH)₂/CuCo/Ni(OH)₂ composite demonstrated exceptional potential as an efficient and stable electrocatalyst for both urea and water oxidation reactions, paving the way for more effective hydrogen production technologies.

Original language	English
Pages (from-to)	67715-67729
Number of pages	15
Journal	ACS Applied Materials and Interfaces
Volume	16
Issue number	49
DOIs	https://doi.org/10.1021/acsami.4c14041
State	Published - Dec 11 2024

Funding

This work was supported as part of Understanding, and Controlling Accelerated and Gradual Evolution of Materials for Energy (UNCAGE-ME), an Energy Frontier Research Center Funded by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, under Award No. SC-0012577. FESEM characterization was conducted as part of a user project at the Center for Nanophase Materials Sciences (CNMS), which is a US Department of Energy, Office of Science User Facility at Oak Ridge National Laboratory.

Keywords

active site
electrocatalysis
hydrogen
interface
stability
synergism
urea

Access to Document

10.1021/acsami.4c14041

Cite this

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title = "Tailored Ni(OH)2/CuCo/Ni(OH)2 Composite Interfaces for Efficient and Durable Urea Oxidation Reaction",

abstract = "Electrocatalytic urea oxidation reaction is a promising alternative to water oxidation for more efficient hydrogen production due to its significantly lower thermodynamic potential. However, achieving efficient electrochemical urea oxidation remains a formidable challenge, and development of an improved electrocatalyst with an optimal physicochemical and electronic structure toward urea oxidation is desired. This can be accomplished by designing a tailored two-dimensional composite with an abundance of active sites in a favorable electronic environment. In this study, we demonstrate the fabrication of a self-supported, electrochemically grown metal/mixed metal hydroxide composite interface via a two-step electrodeposition method. Specifically, Ni(OH)2 was electrodeposited on the top of the CuCo layer (Ni(OH)2/CuCo/Ni(OH)2), and the resultant 2D composite structure required 1.333 ± 0.006 V to oxidize urea electrochemically to achieve a current density of 10 mA cm-2, which outperformed the potential required for individual components, Ni(OH)2 and CuCo. The high density of Ni3+ active sites in the composite structure facilitated high electrocatalyst activity and stability. Ni(OH)2/CuCo/Ni(OH)2 was stable for at least 50 h without any noticeable degradation in the activity or alteration of the morphology. As a bifunctional electrocatalyst, the material also exhibited excellent performance for water oxidation with 260 mV overpotential and 50 h stability. In a two-electrode configuration coupled with a NiMo cathode catalyst, the electrolyzer required 1.42 V cell voltage for overall urea splitting. Overall, the engineered Ni(OH)2/CuCo/Ni(OH)2 composite demonstrated exceptional potential as an efficient and stable electrocatalyst for both urea and water oxidation reactions, paving the way for more effective hydrogen production technologies.",

keywords = "active site, electrocatalysis, hydrogen, interface, stability, synergism, urea",

author = "Sahanaz Parvin and Emmanuel Aransiola and Mohamed Ammar and Seunghoon Lee and Lihua Zhang and Juliane Weber and Jonas Baltrusaitis",

note = "Publisher Copyright: {\textcopyright} 2024 The Authors. Published by American Chemical Society.",

year = "2024",

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T1 - Tailored Ni(OH)2/CuCo/Ni(OH)2 Composite Interfaces for Efficient and Durable Urea Oxidation Reaction

AU - Parvin, Sahanaz

AU - Aransiola, Emmanuel

AU - Ammar, Mohamed

AU - Lee, Seunghoon

AU - Zhang, Lihua

AU - Weber, Juliane

AU - Baltrusaitis, Jonas

PY - 2024/12/11

Y1 - 2024/12/11

N2 - Electrocatalytic urea oxidation reaction is a promising alternative to water oxidation for more efficient hydrogen production due to its significantly lower thermodynamic potential. However, achieving efficient electrochemical urea oxidation remains a formidable challenge, and development of an improved electrocatalyst with an optimal physicochemical and electronic structure toward urea oxidation is desired. This can be accomplished by designing a tailored two-dimensional composite with an abundance of active sites in a favorable electronic environment. In this study, we demonstrate the fabrication of a self-supported, electrochemically grown metal/mixed metal hydroxide composite interface via a two-step electrodeposition method. Specifically, Ni(OH)2 was electrodeposited on the top of the CuCo layer (Ni(OH)2/CuCo/Ni(OH)2), and the resultant 2D composite structure required 1.333 ± 0.006 V to oxidize urea electrochemically to achieve a current density of 10 mA cm-2, which outperformed the potential required for individual components, Ni(OH)2 and CuCo. The high density of Ni3+ active sites in the composite structure facilitated high electrocatalyst activity and stability. Ni(OH)2/CuCo/Ni(OH)2 was stable for at least 50 h without any noticeable degradation in the activity or alteration of the morphology. As a bifunctional electrocatalyst, the material also exhibited excellent performance for water oxidation with 260 mV overpotential and 50 h stability. In a two-electrode configuration coupled with a NiMo cathode catalyst, the electrolyzer required 1.42 V cell voltage for overall urea splitting. Overall, the engineered Ni(OH)2/CuCo/Ni(OH)2 composite demonstrated exceptional potential as an efficient and stable electrocatalyst for both urea and water oxidation reactions, paving the way for more effective hydrogen production technologies.

AB - Electrocatalytic urea oxidation reaction is a promising alternative to water oxidation for more efficient hydrogen production due to its significantly lower thermodynamic potential. However, achieving efficient electrochemical urea oxidation remains a formidable challenge, and development of an improved electrocatalyst with an optimal physicochemical and electronic structure toward urea oxidation is desired. This can be accomplished by designing a tailored two-dimensional composite with an abundance of active sites in a favorable electronic environment. In this study, we demonstrate the fabrication of a self-supported, electrochemically grown metal/mixed metal hydroxide composite interface via a two-step electrodeposition method. Specifically, Ni(OH)2 was electrodeposited on the top of the CuCo layer (Ni(OH)2/CuCo/Ni(OH)2), and the resultant 2D composite structure required 1.333 ± 0.006 V to oxidize urea electrochemically to achieve a current density of 10 mA cm-2, which outperformed the potential required for individual components, Ni(OH)2 and CuCo. The high density of Ni3+ active sites in the composite structure facilitated high electrocatalyst activity and stability. Ni(OH)2/CuCo/Ni(OH)2 was stable for at least 50 h without any noticeable degradation in the activity or alteration of the morphology. As a bifunctional electrocatalyst, the material also exhibited excellent performance for water oxidation with 260 mV overpotential and 50 h stability. In a two-electrode configuration coupled with a NiMo cathode catalyst, the electrolyzer required 1.42 V cell voltage for overall urea splitting. Overall, the engineered Ni(OH)2/CuCo/Ni(OH)2 composite demonstrated exceptional potential as an efficient and stable electrocatalyst for both urea and water oxidation reactions, paving the way for more effective hydrogen production technologies.

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KW - hydrogen

KW - interface

KW - stability

KW - synergism

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