期刊
JOURNAL OF THE ENERGY INSTITUTE
卷 111, 期 -, 页码 -出版社
ELSEVIER SCI LTD
DOI: 10.1016/j.joei.2023.101444
关键词
Nitrogen species; Electronic metal-support interactions; D-band center; Work function; 110; Hydrogen evolution reaction
The distribution of nitrogen species in carbon materials can be adjusted by varying the pyrolysis temperature, leading to optimization of the valence band structure and improved catalytic activity.
Nitrogen (N) species in biomass-based carbon can be adjusted through pyrolysis at different temperatures, optimizing the valence band structure of supported metal nanoparticles through electronic metal-support in-teractions (EMSIs). Herein, ginkgo leaves-based carbon supported cobalt phosphide (CoP@NSPC-T, T = 850, 900 and 950 degrees C) was obtained via carbothermal reduction method at different pyrolysis temperature. Pyridinic N and pyrrolic N in carbon lattice were dramatically decreased with pyrolysis temperature raised, whereas the graphitic N showed the opposite trend. The change in N species (pyridinic N, pyrrolic N and graphitic N) reconfigured the valence band structure of CoP@NSPC-T, inducing the enhancement of work function and the upshift of d-band center. A relationship between the ratio of (pyridinic N + pyrrolic N)/graphitic N, work function, d-band center, and HER activity (110) of catalysts was established. CoP@NSPC-900 with a moderate work function value and d -band center tend to achieve a balance for Volmer process and Heyrovsky process, exhibiting the lowest 110 value activity among the resulted catalysts as the ratio of (pyridinic N + pyrrolic N)/graphitic N is 1.33.
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