Insightful understanding of hot-carrier generation and transfer in plasmonic Au@CeO2 core–shell photocatalysts for light-driven hydrogen evolution improvement

Dung Van Dao; Thuy T.D. Nguyen; Periyayya Uthirakumar; Yeong Hoon Cho; Gyu Cheol Kim; Jin Kyu Yang; Duy Thanh Tran; Thanh Duc Le; Hyuk Choi; Hyun You Kim; Yeon Tae Yu; In Hwan Lee

doi:10.1016/j.apcatb.2021.119947

Insightful understanding of hot-carrier generation and transfer in plasmonic Au@CeO₂ core–shell photocatalysts for light-driven hydrogen evolution improvement

Dung Van Dao, Thuy T.D. Nguyen, Periyayya Uthirakumar, Yeong Hoon Cho, Gyu Cheol Kim, Jin Kyu Yang, Duy Thanh Tran, Thanh Duc Le, Hyuk Choi, Hyun You Kim, Yeon Tae Yu, In Hwan Lee

Department of Materials Science and Engineering

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

42 Citations (Scopus)

Abstract

Plasmonic metal@semiconductor core–shell nanoparticles (CSNPs) are considered as promising candidates for artificial photosynthesis. Herein, Au@CeO₂ CSNPs are hydrothermally fabricated for photocatalytic hydrogen evolution reaction (HER). CSNPs deliver superior HER performance compared to free CeO₂. In particular, Au@CeO₂-18 model (shell thickness of 18 nm) produces an HER rate of 4.05 μmol mg^–1 h^–1, which is ∼10 times higher than that of pure CeO₂ (0.40 μmol mg^–1 h^–1) under visible-light. Additionally, Au@CeO₂-18 photocatalyst demonstrates long-term stability after five repetitive runs, at which point it only loses approximately 5% of the activity, while core-free CeO₂ decreases by 37.5 %. Such improvements are attributed to the electronic interactions between Au and CeO₂, which not only enriches Ce³⁺ active sites to narrow bandgap of ceria toward visible, but also increases the affinity for hydrogen ions on the CSNPs surface. Moreover, localized surface plasmon resonance is light-excited and decays to efficiently produce hot-carrier to drive catalytic reactions.

Original language	English
Article number	119947
Journal	Applied Catalysis B: Environmental
Volume	286
DOIs	https://doi.org/10.1016/j.apcatb.2021.119947
Publication status	Published - 2021 Jun 5

Bibliographical note

Funding Information:
This work was supported by the National Research Foundation of Korea (NRF) grant funded by the Korea government (MSIT) ( NRF-2020R1A2B5B03001603 , 2020R1A2C1014498 ), and BK21-FOUR program of the MOE and NRF of Korea . Computing time was provided by the National Institute of Supercomputing and Network/Korea Institute of Science and Technology Information (KSC-2019-CRE-0210).

Funding Information:
This work was supported by the National Research Foundation of Korea (NRF) grant funded by the Korea government (MSIT) (NRF-2020R1A2B5B03001603, 2020R1A2C1014498), and BK21-FOUR program of the MOE and NRF of Korea. Computing time was provided by the National Institute of Supercomputing and Network/Korea Institute of Science and Technology Information (KSC-2019-CRE-0210).

Publisher Copyright:
© 2021 Elsevier B.V.

Keywords

Au@CeOcore–shell
Hot-carrier
Hydrogen production
Photocatalyst
Plasmonic

ASJC Scopus subject areas

Catalysis
Environmental Science(all)
Process Chemistry and Technology

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

Access to Document

10.1016/j.apcatb.2021.119947

Cite this

Dao, D. V., Nguyen, T. T. D., Uthirakumar, P., Cho, Y. H., Kim, G. C., Yang, J. K., Tran, D. T., Le, T. D., Choi, H., Kim, H. Y., Yu, Y. T., & Lee, I. H. (2021). Insightful understanding of hot-carrier generation and transfer in plasmonic Au@CeO₂ core–shell photocatalysts for light-driven hydrogen evolution improvement. Applied Catalysis B: Environmental, 286, Article 119947. https://doi.org/10.1016/j.apcatb.2021.119947

Dao, DV, Nguyen, TTD, Uthirakumar, P, Cho, YH, Kim, GC, Yang, JK, Tran, DT, Le, TD, Choi, H, Kim, HY, Yu, YT & Lee, IH 2021, 'Insightful understanding of hot-carrier generation and transfer in plasmonic Au@CeO₂ core–shell photocatalysts for light-driven hydrogen evolution improvement', Applied Catalysis B: Environmental, vol. 286, 119947. https://doi.org/10.1016/j.apcatb.2021.119947

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title = "Insightful understanding of hot-carrier generation and transfer in plasmonic Au@CeO2 core–shell photocatalysts for light-driven hydrogen evolution improvement",

abstract = "Plasmonic metal@semiconductor core–shell nanoparticles (CSNPs) are considered as promising candidates for artificial photosynthesis. Herein, Au@CeO2 CSNPs are hydrothermally fabricated for photocatalytic hydrogen evolution reaction (HER). CSNPs deliver superior HER performance compared to free CeO2. In particular, Au@CeO2-18 model (shell thickness of 18 nm) produces an HER rate of 4.05 μmol mg–1 h–1, which is ∼10 times higher than that of pure CeO2 (0.40 μmol mg–1 h–1) under visible-light. Additionally, Au@CeO2-18 photocatalyst demonstrates long-term stability after five repetitive runs, at which point it only loses approximately 5% of the activity, while core-free CeO2 decreases by 37.5 %. Such improvements are attributed to the electronic interactions between Au and CeO2, which not only enriches Ce3+ active sites to narrow bandgap of ceria toward visible, but also increases the affinity for hydrogen ions on the CSNPs surface. Moreover, localized surface plasmon resonance is light-excited and decays to efficiently produce hot-carrier to drive catalytic reactions.",

keywords = "Au@CeOcore–shell, Hot-carrier, Hydrogen production, Photocatalyst, Plasmonic",

author = "Dao, {Dung Van} and Nguyen, {Thuy T.D.} and Periyayya Uthirakumar and Cho, {Yeong Hoon} and Kim, {Gyu Cheol} and Yang, {Jin Kyu} and Tran, {Duy Thanh} and Le, {Thanh Duc} and Hyuk Choi and Kim, {Hyun You} and Yu, {Yeon Tae} and Lee, {In Hwan}",

note = "Funding Information: This work was supported by the National Research Foundation of Korea (NRF) grant funded by the Korea government (MSIT) ( NRF-2020R1A2B5B03001603 , 2020R1A2C1014498 ), and BK21-FOUR program of the MOE and NRF of Korea . Computing time was provided by the National Institute of Supercomputing and Network/Korea Institute of Science and Technology Information (KSC-2019-CRE-0210). Funding Information: This work was supported by the National Research Foundation of Korea (NRF) grant funded by the Korea government (MSIT) (NRF-2020R1A2B5B03001603, 2020R1A2C1014498), and BK21-FOUR program of the MOE and NRF of Korea. Computing time was provided by the National Institute of Supercomputing and Network/Korea Institute of Science and Technology Information (KSC-2019-CRE-0210). Publisher Copyright: {\textcopyright} 2021 Elsevier B.V.",

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AU - Dao, Dung Van

AU - Nguyen, Thuy T.D.

AU - Uthirakumar, Periyayya

AU - Cho, Yeong Hoon

AU - Kim, Gyu Cheol

AU - Yang, Jin Kyu

AU - Tran, Duy Thanh

AU - Le, Thanh Duc

AU - Choi, Hyuk

AU - Kim, Hyun You

AU - Yu, Yeon Tae

AU - Lee, In Hwan

N1 - Funding Information: This work was supported by the National Research Foundation of Korea (NRF) grant funded by the Korea government (MSIT) ( NRF-2020R1A2B5B03001603 , 2020R1A2C1014498 ), and BK21-FOUR program of the MOE and NRF of Korea . Computing time was provided by the National Institute of Supercomputing and Network/Korea Institute of Science and Technology Information (KSC-2019-CRE-0210). Funding Information: This work was supported by the National Research Foundation of Korea (NRF) grant funded by the Korea government (MSIT) (NRF-2020R1A2B5B03001603, 2020R1A2C1014498), and BK21-FOUR program of the MOE and NRF of Korea. Computing time was provided by the National Institute of Supercomputing and Network/Korea Institute of Science and Technology Information (KSC-2019-CRE-0210). Publisher Copyright: © 2021 Elsevier B.V.

PY - 2021/6/5

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N2 - Plasmonic metal@semiconductor core–shell nanoparticles (CSNPs) are considered as promising candidates for artificial photosynthesis. Herein, Au@CeO2 CSNPs are hydrothermally fabricated for photocatalytic hydrogen evolution reaction (HER). CSNPs deliver superior HER performance compared to free CeO2. In particular, Au@CeO2-18 model (shell thickness of 18 nm) produces an HER rate of 4.05 μmol mg–1 h–1, which is ∼10 times higher than that of pure CeO2 (0.40 μmol mg–1 h–1) under visible-light. Additionally, Au@CeO2-18 photocatalyst demonstrates long-term stability after five repetitive runs, at which point it only loses approximately 5% of the activity, while core-free CeO2 decreases by 37.5 %. Such improvements are attributed to the electronic interactions between Au and CeO2, which not only enriches Ce3+ active sites to narrow bandgap of ceria toward visible, but also increases the affinity for hydrogen ions on the CSNPs surface. Moreover, localized surface plasmon resonance is light-excited and decays to efficiently produce hot-carrier to drive catalytic reactions.

AB - Plasmonic metal@semiconductor core–shell nanoparticles (CSNPs) are considered as promising candidates for artificial photosynthesis. Herein, Au@CeO2 CSNPs are hydrothermally fabricated for photocatalytic hydrogen evolution reaction (HER). CSNPs deliver superior HER performance compared to free CeO2. In particular, Au@CeO2-18 model (shell thickness of 18 nm) produces an HER rate of 4.05 μmol mg–1 h–1, which is ∼10 times higher than that of pure CeO2 (0.40 μmol mg–1 h–1) under visible-light. Additionally, Au@CeO2-18 photocatalyst demonstrates long-term stability after five repetitive runs, at which point it only loses approximately 5% of the activity, while core-free CeO2 decreases by 37.5 %. Such improvements are attributed to the electronic interactions between Au and CeO2, which not only enriches Ce3+ active sites to narrow bandgap of ceria toward visible, but also increases the affinity for hydrogen ions on the CSNPs surface. Moreover, localized surface plasmon resonance is light-excited and decays to efficiently produce hot-carrier to drive catalytic reactions.

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