期刊
CHEMICAL ENGINEERING JOURNAL
卷 442, 期 -, 页码 -出版社
ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2022.136156
关键词
Heterojunction engineering; Cuprous oxide@cupric oxide core-shell nano-particles; Cupric oxide; Photocatalytic nitrogen fixation; Carbon nitride nanotubes
资金
- National Natural Science Foundation of China [52002186]
- Scientific Research Founda-tion from Nanjing Forestry University
Tunable CuxO (core-shell structured Cu2O@CuO and CuO) nanoparticles are loaded on carbon nitride nanotubes using a simple method involving annealing under different atmospheres. The resulting core-shell nanostructures exhibit enhanced photocatalytic nitrogen fixation and quantum efficiency. Compared to other structures, these nanoparticles also show accelerated charge carrier transfer and increased photoreduction capability.
Tunable CuxO (core-shell structured Cu2O@CuO and CuO) nanoparticles (NPs) are finely loaded on carbon nitride nanotubes (CNNTs) using a facile one-pot method but annealing under different atmospheres. Calcining under H-2/Ar (5% H-2) ensured a Z-scheme heterojunction of Cu2O@CuO/CNNTs, and core-shell nanostructured Cu2O@CuO NPs in particle size of 20-80 nm are firmly anchored along the nanochannels of CNNTs. Calcining under static air conditions led to a Type II heterojunction of CuO/CNNTs, and larger CuO NPs of ca. 200 nm are on the surface of CNNTs. The effect of the calcination temperature and loading content on the photocatalytic ammonia yield was studied. With the annealing temperature at 400 C and 9 wt% copper percentage, the resulting Z-scheme Cu2O@CuO/CNNTs exhibit a nitrogen photofixation rate of 1.38 mM gcat-1h- 1 with an apparent quantum efficiency of 6.28% at 420 nm, which is about 1.4 and 4.4 times higher than that of CuO/ CNNTs and the bare CNNTs, respectively. Introducing Cu2O cores upshifts the band positions of the CuxO NPs, resulting in the formation of a Z-scheme band structure. Comprehensive characterizations reveal that compared to Type II CuO/CNNTs, Z-scheme Cu2O@CuO/CNNTs offer higher N-2 chemisorption energy, accelerated charge carrier transfer and increased photoreduction capability. This study provides a reliable and promising route to engineer core-shell structured Z-scheme heterojunctions for enhanced photocatalytic nitrogen fixation.
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