Cerium-modified Pt/Al2O3 for NH3 synthesis by NO reduction with H2

Min Hye Jeong; Jungseob So; Jinho Oh; Kyung Min Kim; Ji Hoon Park; Young Woo You; Jin Hee Lee; Iljeong Heo; Young Jin Kim

doi:10.1016/j.apsusc.2023.158067

Cerium-modified Pt/Al₂O₃ for NH₃ synthesis by NO reduction with H₂

Min Hye Jeong, Jungseob So, Jinho Oh, Kyung Min Kim, Ji Hoon Park, Young Woo You, Jin Hee Lee, Iljeong Heo, Young Jin Kim

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

5 Scopus citations

Abstract

The Haber–Bosch process is a mature and proven technology for the commercial production of NH₃. However, with the increasing focus on achieving net-zero emissions, alternative technologies have gained interest. This paper proposes an effective catalytic system for synthesizing NH₃ directly from NO and H₂ at atmospheric pressures. Pt/CeO_xAl₂O₃ synthesized via solvent-deficient precipitation (SDP) showed a much higher NH₃ yield compared to conventional Pt/Al₂O₃ and other Pt/Ce-containing catalysts. Various characterization techniques demonstrated that achieving precise control of the electronic metal-support interaction (EMSI) is crucial for attaining the optimal electronic and geometric structure that balances the decisive factors, Pt oxidation state and Pt dispersion, to enable a high rate of NH₃ production from NO and H₂. Pt/CeO_xAl₂O₃ possesses abundant metallic Pt nanoclusters that are well dispersed on CeO_xAl₂O₃ due to the moderate Pt-Ce interactions. These small metallic Pt clusters in contact with CeO_x turned out to play a critical role in the dissociative adsorption of NO and H₂, leading to the formation of the reaction intermediates, the –NH₂ species, which contribute to the improved NH₃ productivity of Pt/CeO_xAl₂O₃.

Original language	English
Article number	158067
Journal	Applied Surface Science
Volume	638
DOIs	https://doi.org/10.1016/j.apsusc.2023.158067
State	Published - 30 Nov 2023

Keywords

Ceria
Hydrogen
NH synthesis
Nitric oxide
Platinum
Solvent-deficient precipitation

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title = "Cerium-modified Pt/Al2O3 for NH3 synthesis by NO reduction with H2",

abstract = "The Haber–Bosch process is a mature and proven technology for the commercial production of NH3. However, with the increasing focus on achieving net-zero emissions, alternative technologies have gained interest. This paper proposes an effective catalytic system for synthesizing NH3 directly from NO and H2 at atmospheric pressures. Pt/CeOxAl2O3 synthesized via solvent-deficient precipitation (SDP) showed a much higher NH3 yield compared to conventional Pt/Al2O3 and other Pt/Ce-containing catalysts. Various characterization techniques demonstrated that achieving precise control of the electronic metal-support interaction (EMSI) is crucial for attaining the optimal electronic and geometric structure that balances the decisive factors, Pt oxidation state and Pt dispersion, to enable a high rate of NH3 production from NO and H2. Pt/CeOxAl2O3 possesses abundant metallic Pt nanoclusters that are well dispersed on CeOxAl2O3 due to the moderate Pt-Ce interactions. These small metallic Pt clusters in contact with CeOx turned out to play a critical role in the dissociative adsorption of NO and H2, leading to the formation of the reaction intermediates, the –NH2 species, which contribute to the improved NH3 productivity of Pt/CeOxAl2O3.",

keywords = "Ceria, Hydrogen, NH synthesis, Nitric oxide, Platinum, Solvent-deficient precipitation",

author = "Jeong, {Min Hye} and Jungseob So and Jinho Oh and Kim, {Kyung Min} and Park, {Ji Hoon} and You, {Young Woo} and Lee, {Jin Hee} and Iljeong Heo and Kim, {Young Jin}",

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doi = "10.1016/j.apsusc.2023.158067",

language = "English",

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T1 - Cerium-modified Pt/Al2O3 for NH3 synthesis by NO reduction with H2

AU - Jeong, Min Hye

AU - So, Jungseob

AU - Oh, Jinho

AU - Kim, Kyung Min

AU - Park, Ji Hoon

AU - You, Young Woo

AU - Lee, Jin Hee

AU - Heo, Iljeong

AU - Kim, Young Jin

PY - 2023/11/30

Y1 - 2023/11/30

N2 - The Haber–Bosch process is a mature and proven technology for the commercial production of NH3. However, with the increasing focus on achieving net-zero emissions, alternative technologies have gained interest. This paper proposes an effective catalytic system for synthesizing NH3 directly from NO and H2 at atmospheric pressures. Pt/CeOxAl2O3 synthesized via solvent-deficient precipitation (SDP) showed a much higher NH3 yield compared to conventional Pt/Al2O3 and other Pt/Ce-containing catalysts. Various characterization techniques demonstrated that achieving precise control of the electronic metal-support interaction (EMSI) is crucial for attaining the optimal electronic and geometric structure that balances the decisive factors, Pt oxidation state and Pt dispersion, to enable a high rate of NH3 production from NO and H2. Pt/CeOxAl2O3 possesses abundant metallic Pt nanoclusters that are well dispersed on CeOxAl2O3 due to the moderate Pt-Ce interactions. These small metallic Pt clusters in contact with CeOx turned out to play a critical role in the dissociative adsorption of NO and H2, leading to the formation of the reaction intermediates, the –NH2 species, which contribute to the improved NH3 productivity of Pt/CeOxAl2O3.

AB - The Haber–Bosch process is a mature and proven technology for the commercial production of NH3. However, with the increasing focus on achieving net-zero emissions, alternative technologies have gained interest. This paper proposes an effective catalytic system for synthesizing NH3 directly from NO and H2 at atmospheric pressures. Pt/CeOxAl2O3 synthesized via solvent-deficient precipitation (SDP) showed a much higher NH3 yield compared to conventional Pt/Al2O3 and other Pt/Ce-containing catalysts. Various characterization techniques demonstrated that achieving precise control of the electronic metal-support interaction (EMSI) is crucial for attaining the optimal electronic and geometric structure that balances the decisive factors, Pt oxidation state and Pt dispersion, to enable a high rate of NH3 production from NO and H2. Pt/CeOxAl2O3 possesses abundant metallic Pt nanoclusters that are well dispersed on CeOxAl2O3 due to the moderate Pt-Ce interactions. These small metallic Pt clusters in contact with CeOx turned out to play a critical role in the dissociative adsorption of NO and H2, leading to the formation of the reaction intermediates, the –NH2 species, which contribute to the improved NH3 productivity of Pt/CeOxAl2O3.

KW - Ceria

KW - Hydrogen

KW - NH synthesis

KW - Nitric oxide

KW - Platinum

KW - Solvent-deficient precipitation

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JO - Applied Surface Science

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Cerium-modified Pt/Al₂O₃ for NH₃ synthesis by NO reduction with H₂

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