期刊
ADVANCED FUNCTIONAL MATERIALS
卷 32, 期 12, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adfm.202112452
关键词
nitrogen photofixation; ruthenium; second coordination sphere; single-atom catalysts
类别
资金
- National Key R&D Program of China [2017YFA0206703, 2017YFA0700104]
- National Natural Science Foundation of China [11875258, U1932213, U1932148]
- Fundamental Research Funds for the Central Universities [WK2060000016]
- Collaborative Innovation Program of Hefei Science Center, CAS [2019HSC-CIP009]
- Users with Excellence Program of Hefei Science Center CAS [2019HSC-UE004]
- Youth Innovation Promotion Association CAS [2020454]
- National Science Fund for Distinguished Young Scholars [22025205]
This study demonstrates that the strong interaction between Ru single atoms and the second coordination sphere can enrich photogenerated electrons at Ru active sites and enhance N-2 photofixation activity. Mechanistic studies reveal that Ru-Co coordination serves as an additional photoelectron transfer channel, facilitating the photoreduction of N-2 into NH3.
Orienting the migration of photogenerated electrons to the target active single atoms instead of dissipation at inert sites is crucial to improve the photocatalytic activity of single-atom catalysts, but remains a challenge. Herein, it is demonstrated that the strong interaction between Ru single atoms and the second coordination sphere significantly enriches photogenerated electrons at Ru active sites and boosted N-2 photofixation activity. The extra Ru-Co coordination from the strong interaction with the second coordination sphere is observed over CoO-supported Ru single atoms (RuO+Co/CoO) relative to the weakly interacting ones (Ru-O/CoO). For N-2 photofixation, RuO+Co/CoO exhibits an ammonia production rate of 306 mu mol g(cat.)(-1) h(-1) without any sacrificial agents at room temperature, which is 4.6 times that of Ru-O/CoO. Mechanistic studies reveal that Ru-Co coordination in RuO+Co/CoO serves as an additional photoelectron transfer channel. Such channel promotes the accumulation of photoelectrons that excite from O to Co atoms on Ru active sites, facilitating the photoreduction of N-2 into NH3 process. The concept of the second coordination sphere modulation offers a powerful platform toward rational design of highly efficient single-atom catalysts for N-2 fixation and beyond.
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