2D/2D Z-scheme-based α-Fe2O3 @NGr heterojunction implanted with Pt single-atoms for remarkable photocatalytic hydrogen evolution

Vandung Dao; Luis A. Cipriano; Sang Woo Ki; Sunny Yadav; Wenmeng Wang; Giovanni Di Liberto; Kai Chen; Hoki Son; Jin Kyu Yang; Gianfranco Pacchioni; In Hwan Lee

doi:10.1016/j.apcatb.2023.122586

2D/2D Z-scheme-based α-Fe₂O₃ @NGr heterojunction implanted with Pt single-atoms for remarkable photocatalytic hydrogen evolution

Vandung Dao, Luis A. Cipriano, Sang Woo Ki, Sunny Yadav, Wenmeng Wang, Giovanni Di Liberto, Kai Chen, Hoki Son, Jin Kyu Yang, Gianfranco Pacchioni, In Hwan Lee

Department of Materials Science and Engineering

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

6 Citations (Scopus)

Abstract

Direct Z-scheme designs perform well in light-to-fuel conversion. Here, an active and stable ternary Z-scheme core-shell heterojunction for photocatalytic hydrogen evolution (PHE) is fabricated consisting of hexagonal 2D α-Fe₂O₃ (as photocatalyst II) and 2D nitrogen-doped graphene (NGr as photocatalyst I) functionalized with the Pt single-atoms (SAs) cocatalyst. Under visible light, the 2D/2D α-Fe₂O₃ @NGr₃[sbnd]Pt_SAs (NGr shell thickness of 3 nm and Pt loading of 0.5 wt%) achieves a remarkable PHE of 6.4 µmol mg_cat⁻¹ h^–1, which is 16.4- and 3.28-times higher than those of free NGr (0.39 µmol mg_cat⁻¹ h^–1) and binary α-Fe₂O₃ @NGr₃ (1.95 µmol mg_cat⁻¹ h^–1), thus outperforming the currently-advanced PHE catalysts. The outstanding performance is due to the superiority of a direct 2D/2D Z-scheme core-shell fabrication, including a large surface area for light harvesting, facile charge separation and transfer, and the workability of Pt SAs sites. Theoretical investigations provide additional insight into the mechanistic process of the ternary system for PHE reactions.

Original language	English
Article number	122586
Journal	Applied Catalysis B: Environmental
Volume	330
DOIs	https://doi.org/10.1016/j.apcatb.2023.122586
Publication status	Published - 2023 Aug 5

Bibliographical note

Funding Information:
This work was supported by the National Research Foundation of Korea ( NRF ) grant funded by the Korea government ( MSIT ) ( 2021M3H4A1A02051284 , 2022R1A2C1010895 , 2020R1A2C1014498 ), and the Industrial Strategic Technology Development Program ( 20019235 , Deformable and Immersive Volumetric AR Glass) funded by the Ministry of Trade, Industry & Energy ( MOTIE , Korea). LAC, GDL, and GP acknowledge the financial support from the Italian Ministry of University and Research ( MUR ) through the PRIN Project 20179337R7 and the access to the CINECA supercomputing resources via ISCRAB.

Publisher Copyright:
© 2023 Elsevier B.V.

Keywords

2D/2D core-shell
Direct Z-scheme
Hematite
Nitrogen-doped graphene
Photocatalytic hydrogen evolution
Single-atoms

ASJC Scopus subject areas

Catalysis
Environmental Science(all)
Process Chemistry and Technology

Access to Document

10.1016/j.apcatb.2023.122586

Cite this

Dao, V., Cipriano, L. A., Ki, S. W., Yadav, S., Wang, W., Di Liberto, G., Chen, K., Son, H., Yang, J. K., Pacchioni, G., & Lee, I. H. (2023). 2D/2D Z-scheme-based α-Fe₂O₃ @NGr heterojunction implanted with Pt single-atoms for remarkable photocatalytic hydrogen evolution. Applied Catalysis B: Environmental, 330, Article 122586. https://doi.org/10.1016/j.apcatb.2023.122586

@article{ec62c7627ccf4e6d8deceff922961e4b,

title = "2D/2D Z-scheme-based α-Fe2O3 @NGr heterojunction implanted with Pt single-atoms for remarkable photocatalytic hydrogen evolution",

abstract = "Direct Z-scheme designs perform well in light-to-fuel conversion. Here, an active and stable ternary Z-scheme core-shell heterojunction for photocatalytic hydrogen evolution (PHE) is fabricated consisting of hexagonal 2D α-Fe2O3 (as photocatalyst II) and 2D nitrogen-doped graphene (NGr as photocatalyst I) functionalized with the Pt single-atoms (SAs) cocatalyst. Under visible light, the 2D/2D α-Fe2O3 @NGr3[sbnd]PtSAs (NGr shell thickness of 3 nm and Pt loading of 0.5 wt%) achieves a remarkable PHE of 6.4 µmol mgcat−1 h–1, which is 16.4- and 3.28-times higher than those of free NGr (0.39 µmol mgcat−1 h–1) and binary α-Fe2O3 @NGr3 (1.95 µmol mgcat−1 h–1), thus outperforming the currently-advanced PHE catalysts. The outstanding performance is due to the superiority of a direct 2D/2D Z-scheme core-shell fabrication, including a large surface area for light harvesting, facile charge separation and transfer, and the workability of Pt SAs sites. Theoretical investigations provide additional insight into the mechanistic process of the ternary system for PHE reactions.",

keywords = "2D/2D core-shell, Direct Z-scheme, Hematite, Nitrogen-doped graphene, Photocatalytic hydrogen evolution, Single-atoms",

author = "Vandung Dao and Cipriano, {Luis A.} and Ki, {Sang Woo} and Sunny Yadav and Wenmeng Wang and {Di Liberto}, Giovanni and Kai Chen and Hoki Son and Yang, {Jin Kyu} and Gianfranco Pacchioni 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 ) ( 2021M3H4A1A02051284 , 2022R1A2C1010895 , 2020R1A2C1014498 ), and the Industrial Strategic Technology Development Program ( 20019235 , Deformable and Immersive Volumetric AR Glass) funded by the Ministry of Trade, Industry & Energy ( MOTIE , Korea). LAC, GDL, and GP acknowledge the financial support from the Italian Ministry of University and Research ( MUR ) through the PRIN Project 20179337R7 and the access to the CINECA supercomputing resources via ISCRAB. Publisher Copyright: {\textcopyright} 2023 Elsevier B.V.",

year = "2023",

month = aug,

day = "5",

doi = "10.1016/j.apcatb.2023.122586",

language = "English",

volume = "330",

journal = "Applied Catalysis B: Environmental",

issn = "0926-3373",

publisher = "Elsevier",

}

TY - JOUR

T1 - 2D/2D Z-scheme-based α-Fe2O3 @NGr heterojunction implanted with Pt single-atoms for remarkable photocatalytic hydrogen evolution

AU - Dao, Vandung

AU - Cipriano, Luis A.

AU - Ki, Sang Woo

AU - Yadav, Sunny

AU - Wang, Wenmeng

AU - Di Liberto, Giovanni

AU - Chen, Kai

AU - Son, Hoki

AU - Yang, Jin Kyu

AU - Pacchioni, Gianfranco

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 ) ( 2021M3H4A1A02051284 , 2022R1A2C1010895 , 2020R1A2C1014498 ), and the Industrial Strategic Technology Development Program ( 20019235 , Deformable and Immersive Volumetric AR Glass) funded by the Ministry of Trade, Industry & Energy ( MOTIE , Korea). LAC, GDL, and GP acknowledge the financial support from the Italian Ministry of University and Research ( MUR ) through the PRIN Project 20179337R7 and the access to the CINECA supercomputing resources via ISCRAB. Publisher Copyright: © 2023 Elsevier B.V.

PY - 2023/8/5

Y1 - 2023/8/5

N2 - Direct Z-scheme designs perform well in light-to-fuel conversion. Here, an active and stable ternary Z-scheme core-shell heterojunction for photocatalytic hydrogen evolution (PHE) is fabricated consisting of hexagonal 2D α-Fe2O3 (as photocatalyst II) and 2D nitrogen-doped graphene (NGr as photocatalyst I) functionalized with the Pt single-atoms (SAs) cocatalyst. Under visible light, the 2D/2D α-Fe2O3 @NGr3[sbnd]PtSAs (NGr shell thickness of 3 nm and Pt loading of 0.5 wt%) achieves a remarkable PHE of 6.4 µmol mgcat−1 h–1, which is 16.4- and 3.28-times higher than those of free NGr (0.39 µmol mgcat−1 h–1) and binary α-Fe2O3 @NGr3 (1.95 µmol mgcat−1 h–1), thus outperforming the currently-advanced PHE catalysts. The outstanding performance is due to the superiority of a direct 2D/2D Z-scheme core-shell fabrication, including a large surface area for light harvesting, facile charge separation and transfer, and the workability of Pt SAs sites. Theoretical investigations provide additional insight into the mechanistic process of the ternary system for PHE reactions.

AB - Direct Z-scheme designs perform well in light-to-fuel conversion. Here, an active and stable ternary Z-scheme core-shell heterojunction for photocatalytic hydrogen evolution (PHE) is fabricated consisting of hexagonal 2D α-Fe2O3 (as photocatalyst II) and 2D nitrogen-doped graphene (NGr as photocatalyst I) functionalized with the Pt single-atoms (SAs) cocatalyst. Under visible light, the 2D/2D α-Fe2O3 @NGr3[sbnd]PtSAs (NGr shell thickness of 3 nm and Pt loading of 0.5 wt%) achieves a remarkable PHE of 6.4 µmol mgcat−1 h–1, which is 16.4- and 3.28-times higher than those of free NGr (0.39 µmol mgcat−1 h–1) and binary α-Fe2O3 @NGr3 (1.95 µmol mgcat−1 h–1), thus outperforming the currently-advanced PHE catalysts. The outstanding performance is due to the superiority of a direct 2D/2D Z-scheme core-shell fabrication, including a large surface area for light harvesting, facile charge separation and transfer, and the workability of Pt SAs sites. Theoretical investigations provide additional insight into the mechanistic process of the ternary system for PHE reactions.

KW - 2D/2D core-shell

KW - Direct Z-scheme

KW - Hematite

KW - Nitrogen-doped graphene

KW - Photocatalytic hydrogen evolution

KW - Single-atoms

UR - http://www.scopus.com/inward/record.url?scp=85149883946&partnerID=8YFLogxK

U2 - 10.1016/j.apcatb.2023.122586

DO - 10.1016/j.apcatb.2023.122586

M3 - Article

AN - SCOPUS:85149883946

SN - 0926-3373

VL - 330

JO - Applied Catalysis B: Environmental

JF - Applied Catalysis B: Environmental

M1 - 122586

ER -