Photocatalytic robust solar energy reduction of dinitrogen to ammonia on ultrathin MoS2

Songmei Sun, Xiaoman Li, Wenzhong Wang, Ling Zhang, Xiang Sun

    Research output: Contribution to journalArticlepeer-review

    108 Citations (Scopus)

    Abstract

    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.

    Original languageEnglish
    Pages (from-to)323-329
    Number of pages7
    JournalApplied Catalysis B: Environmental
    Volume200
    DOIs
    Publication statusPublished - Jan 1 2017

    All Science Journal Classification (ASJC) codes

    • Catalysis
    • Environmental Science(all)
    • Process Chemistry and Technology

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