In:
Angewandte Chemie, Wiley, Vol. 135, No. 26 ( 2023-06-26)
Abstract:
The ambient ammonia synthesis coupled with distributed green hydrogen production technology can provide promising solutions for low‐carbon NH 3 production and H 2 storage. Herein, we reported Ru‐loaded defective pyrochlore K 2 Ta 2 O 6− x with remarkable visible‐light absorption and a very low work function, enabling effective visible‐light‐driven ammonia synthesis from N 2 and H 2 at low pressure down to 0.2 atm. The photocatalytic rate was 2.8 times higher than that of the best previously reported photocatalyst and the photo‐thermal rate at 425 K was similar to that of Ru‐loaded black TiO 2 at 633 K. Compared to perovskite‐type KTaO 3− x with the same composition, the pyrochlore exhibited a 3.7‐fold increase in intrinsic activity due to a higher photoexcited charge separation efficiency and a higher conduction band position. The interfacial Schottky barrier and spontaneous electron transfer between K 2 Ta 2 O 6− x and Ru further improve photoexcited charge separation and accumulate energetic electrons to facilitate N 2 activation.
Type of Medium:
Online Resource
ISSN:
0044-8249
,
1521-3757
DOI:
10.1002/ange.v135.26
DOI:
10.1002/ange.202303629
Language:
English
Publisher:
Wiley
Publication Date:
2023
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