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Photocatalytic robust solar energy reduction of dinitrogen to ammonia on ultrathin MoS 2

Sun, Songmei, Li, Xiaoman, Wang, Wenzhong, Zhang, Ling and Sun, Xiang 2017. Photocatalytic robust solar energy reduction of dinitrogen to ammonia on ultrathin MoS 2. Applied Catalysis B: Environmental 200 , p. 323. 10.1016/j.apcatb.2016.07.025

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The crux for solar N2 reduction to ammonia is activating N2 into its high-energy intermediate. Applying a simultaneous multi-electron reduction process could avoid intermediate generation and decrease the thermodynamic barrier. However, this process is extremely difficult from a kinetic view and experiments so far have not shown it is accessible. Here we show the first direct evidence of trion induced multi-electron N2 reduction on ultrathin MoS2. By applying light induced trions, N2 molecular was activated and transformed into ammonia by a simultaneous six-electron reduction process, with a high ammonia synthesis rate of 325 μmol/g h without the assistant of any organic scavengers or co-catalyst. Bulk MoS2 without trions did not exhibit any activity. This demonstrates multi-electron reduction may be realized in electron-rich semiconductors with high concentration of localized electrons such as trions. The methodology of simultaneous multi-electron reduction has wide implications for reactions beyond N2 reduction and for materials beyond MoS2.

Item Type: Article
Date Type: Publication
Status: Published
Schools: Chemistry
Publisher: Elsevier
ISSN: 0926-3373
Date of First Compliant Deposit: 22 May 2019
Date of Acceptance: 16 July 2016
Last Modified: 08 Oct 2021 05:42

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