期刊
APPLIED CATALYSIS B-ENVIRONMENTAL
卷 306, 期 -, 页码 -出版社
ELSEVIER
DOI: 10.1016/j.apcatb.2022.121092
关键词
Metal cocatalyst; Valence regulation; Surface states; Oxidative active species; Contribution modulating
资金
- Fundamental Research Funds for the Central Universities
- Nankai University [ZB19100141]
- National Natural Science Foundation of China [21872102, 22172080]
- Tianjin Project + Team innovation team, 2020
Nano-structured metal cocatalysts, such as PdO-Pd/CN, have been found to facilitate catalytic performance due to their ability to be easily oxidized and form mixed valences and interfaces. In this study, three different Pd cocatalysts with varying valence distributions were loaded onto g-C3N4 nanosheets. The results showed that the distribution of palladium valence influenced the generation of oxidative active species, with PdO2+ promoting the production of center dot O-2(-) and Pd-0 promoting the production of h(+). The joint action of center dot O-2(-) and h(+) in the PdO50-Pd50/CN cocatalyst resulted in the best performance for degrading ciprofloxacin.
Nano-structured metal cocatalysts are easy to be oxidized and form mixed valences and interfaces which would facilitate the catalytic performance in previous studies. Herein, as an example in photocatalysis, three kinds of Pd cocatalysts with various valence distributions (PdO70-Pd30/CN, PdO50-Pd50/CN and PdO30-Pd70/CN) were loaded on g-C3N4 nanosheets with the close loading amounts (similar to 1 wt%) and uniform sizes (2-3 nm). Then, the results of the photocatalytic degradation of ciprofloxacin showed that the generated oxidative active species are highly related to the distribution of palladium valence. Pd2+ (PdO) benefits the production of center dot O-2(-), while Pd-0 benefits the production of h(+). The theoretical simulations revealed that surface states e.g., electron distribution and the adsorption ability of O-2 on different Pd species determined the production of center dot O-2(-) and h(+). Besides, PdO50-Pd50/CN showed the best performance for degrading ciprofloxacin, due to the joint action of center dot O-2(-) and h(+) in the CIP degradation.
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