In:
Advanced Functional Materials, Wiley, Vol. 32, No. 12 ( 2022-03)
Abstract:
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 RuCo coordination from the strong interaction with the second coordination sphere is observed over CoO‐supported Ru single atoms (Ru O+Co /CoO) relative to the weakly interacting ones (Ru O /CoO). For N 2 photofixation, Ru O+Co /CoO exhibits an ammonia production rate of 306 µ 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 RuCo coordination in Ru O+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 NH 3 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.
Type of Medium:
Online Resource
ISSN:
1616-301X
,
1616-3028
DOI:
10.1002/adfm.202112452
Language:
English
Publisher:
Wiley
Publication Date:
2022
detail.hit.zdb_id:
2029061-5
detail.hit.zdb_id:
2039420-2
SSG:
11
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