Strong Electronic Orbit Coupling between Cobalt and Single-Atom Praseodymium for Boosted Nitrous Oxide Decomposition on Co3O4 Catalyst

Hao Liu; Shan Yang; Guimin Wang

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Strong Electronic Orbit Coupling between Cobalt and Single-Atom Praseodymium for Boosted Nitrous Oxide Decomposition on Co3O4 Catalyst

机译：Strong Electronic Orbit Coupling between Cobalt and Single-Atom Praseodymium for Boosted Nitrous Oxide Decomposition on Co3O4 Catalyst

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Nitrous oxide (N2O) has gained increasing attention as an important noncarbon dioxide greenhouse gas, and catalytic decomposition is an effective method of reducing its emissions. Here, Co3O4 was synthesized by the sol-gel method and single-atom Pr was confined in its matrix to improve the N2O decomposition performance. It was observed that the reaction rate varied in a volcano-like pattern with the amount of doped Pr. A N2O decomposition reaction rate 5-7.5 times greater than that of pure Co3O4 is achieved on the catalyst with a Pr/Co molar ratio of 0.06:1, and further Pr doping reduced the activity due to PrOx cluster formation. Combined with X-ray photoelectron spectroscopy, X-ray absorption fine structure, density functional theory and in situ near-ambient pressure X-ray photoelectron spectroscopy, it was demonstrated that the single-atom doped Pr in Co3O4 generates the "Pr 4f-O 2p-Co 3d" network, which redistributes the electrons in Co3O4 lattice and increases the t2 electrons at the tetracoordinated Co~(2+) sites. This coupling between the Pr 4f orbit and Co~(2+) 3d orbit triggers the formation of a 4f-3d electronic ladder, which accelerates the electron transfer from Co~(2+) to the 3π* antibonding orbital of N2O, thus contributing to the N-O bond cleavage. Moreover, the energy barrier for each elementary reaction in the decomposition process of N2O is reduced, especially for O2 desorption. Our work provides a theoretical grounding and reference for designing atomically modified catalysts for N2O decomposition.

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来源
《Environmental Science & Technology: ES&T》 |2022年第22期|16325-16335|共11页
作者
Hao Liu; Shan Yang; Guimin Wang;
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作者单位

State Key Joint Laboratory of Environment Simulation and Pollution Control, School of Environment, Tsinghua University, Beijing 100084, P. R China;

- College of Chemistry, Chemical Engineering and Materials Science, Shandong Normal University, Jinan 250014, P. R. China;

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收录信息美国《科学引文索引》(SCI);美国《工程索引》(EI);美国《生物学医学文摘》(MEDLINE);美国《化学文摘》(CA);
原文格式 PDF
正文语种英语
中图分类环境科学、安全科学;
关键词
rare-earth single atom; Pr-doping; Co3O4; N2O decomposition; electronic structure regulation;

Strong Electronic Orbit Coupling between Cobalt and Single-Atom Praseodymium for Boosted Nitrous Oxide Decomposition on Co3O4 Catalyst

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