0D ultrafine ruthenium quantum dot decorated 3D porous graphitic carbon nitride with efficient charge separation and appropriate hydrogen adsorption capacity for superior photocatalytic hydrogen evolution
Designing a Pt-alternative cocatalyst capable of dissociating HO-H bonds is of great significance yet challenging for the development of high-efficiency and cost-effective water splitting photocatalytic systems. In this study, we designed and constructed a 0D ultrafine ruthenium (U-Ru) quantum dot d...
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Published in | Dalton transactions : an international journal of inorganic chemistry Vol. 5; no. 7; pp. 2414 - 2425 |
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Main Authors | , , , , , , , |
Format | Journal Article |
Language | English |
Published |
England
Royal Society of Chemistry
21.02.2021
|
Subjects | |
Online Access | Get full text |
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Summary: | Designing a Pt-alternative cocatalyst capable of dissociating HO-H bonds is of great significance yet challenging for the development of high-efficiency and cost-effective water splitting photocatalytic systems. In this study, we designed and constructed a 0D ultrafine ruthenium (U-Ru) quantum dot decorated 3D porous g-C
3
N
4
(3DpCN) nanohybrid (U-Ru/3DpCN) for photocatalytic hydrogen evolution, in which the U-Ru quantum dots act as cocatalysts accelerating the surface proton reduction reaction, and the 3D porous architecture assembled by 2D ultrathin nanosheets inherits a short charge diffusion distance and has a large specific surface area. Owing to these structural and physicochemical merits, the optimal photocatalyst U-1Ru/3DpCN achieves a superior hydrogen evolution performance of 2945.47 μmol g
−1
h
−1
under visible light with a high apparent quantum efficiency (AQE) of 9.5% at 420 nm, which is close to Pt-cocatalyst/3DpCN and better than most reported co-catalysts/g-C
3
N
4
photocatalytic systems. Experimental results indicate that the formed Schottky junction between U-Ru and 3DpCN contributes to efficient charge separation, and DFT calculations show that the Ru-cocatalyst/g-C
3
N
4
system has an appropriate hydrogen adsorption Gibbs free energy (Δ
G
H*
) of 0.24 eV, which are both responsible to improve the photocatalytic performance. This study provides a new way to develop excellent photocatalysts for hydrogen evolution by the integration of cost-effective Ru quantum dot cocatalysts with nanostructured semiconductors.
Ultrafine Ru quantum dot decorated 3D porous g-C
3
N
4
(U-Ru/3DpCN) photocatalysts were prepared. The optimal photocatalyst U-1Ru/3DpCN achieves an excellent H
2
evolution of 2945.47 μmol g
−1
h
−1
under visible light with a high AQE of 9.5% at 420 nm. |
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Bibliography: | 10.1039/d0dt03445b Electronic supplementary information (ESI) available. See DOI ObjectType-Article-1 SourceType-Scholarly Journals-1 ObjectType-Feature-2 content type line 23 |
ISSN: | 1477-9226 1477-9234 |
DOI: | 10.1039/d0dt03445b |