Journal
CHEMICAL ENGINEERING JOURNAL
Volume 434, Issue -, Pages -Publisher
ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2022.134673
Keywords
Electron-rich interface; Photocatalytic hydrogen evolution; Cu-Co heterogeneous structure; Cocatalyst; g-C3N4
Categories
Funding
- National Natural Science Foun-dation of China [22078118, 21972048, 21802046]
- Natural Science Foundation of Guangdong Province [2019A1515011138, 2018A0303130018]
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This study investigated the mechanism of interfacial effect on enhanced photocatalytic hydrogen evolution using CuCo@C nanoparticles as cocatalysts. The CuCo@C/g-C3N4 showed a higher rate of visible light-driven photocatalytic hydrogen evolution compared to other control groups. Experimental and theoretical calculations revealed that the enrichment of electrons at the Cu-Co interface promoted the separation of electron-hole pairs and accelerated charge transfer. Additionally, the carbon layer and Cu-Co interface regulated the adsorption free energy of hydrogen on CuCo@C, favoring hydrogen evolution.
Heterogeneous nano-metal structures are widely used in the field of photocatalysis as an efficient cocatalyst, but the structure-activity relationship has not been elucidated clearly. In this work, a classical CuCo@C nanoparticle with a core of bimetallic CuCo and a carbon shell was used as a cocatalyst to explore and reveal the mechanism of interfacial effect for enhanced photocatalytic hydrogen evolution. It was found that the bimetallic CuCo had a heterogeneous structure with abundant Cu-Co interfaces. The desirable visible-light-driven photocatalytic hydrogen evolution rate of CuCo@C/g-C3N4 was much higher than that of Cu@C/g-C3N4, Co@C/g-C3N4, and superior to that of the control group loaded with 1 wt% Pt (Pt/g-C3N4). According to the experimental characterizations and density functional theory calculations, electrons were enriched at the Cu-Co interface, which can promote the electron-hole pairs separation and accelerate charge transfer of the g-C3N4 host photocatalysts. On the other hand, the surface carbon layer and Cu-Co interface modulated the H adsorption free energy on the CuCo@C, which was favorable for hydrogen evolution. It is conceivable that further investigating and tuning different metal interfaces will facilitate the large-scale application of bimetallic cocatalysts.
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