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Selective electroreduction of dinitrogen to ammonia on a molecular iron phthalocyanine/O-MWCNT catalyst under ambient conditions

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Abstract

Effective catalysts with sufficient activity and selectivity are essential for the nitrogen reduction reaction (NRR). Many fruitful NRR electrocatalysts have been investigated with regard to NH3 production under ambient conditions in recent years. However, well-defined and modifiable molecular catalysts have rarely been reported for the NRR to date. Here, molecular FePc was grafted on an O-MWCNT surface as a NRR electrocatalyst to improve its recyclability. This catalyst displayed high electrocatalytic ability and selectivity, giving a large NH3 yield of 36 μg h−1 mg−1 cat., a FE of 9.73% and a turnover number (TON) of 12.56 after 2 h of electrocatalytic reaction in an acidic electrolyte, superior to most of the reported materials. DFT calculations indicated that the NRR preferentially proceeded along the alternate pathway, the activation of N2 to produce N2H* is the rate-limiting step with a ΔG value of 1.79 eV. Conclusively, we report FePc/O-MWCNT as a low-cost, high-efficiency NRR catalyst that also offers a valuable reference for molecular electrocatalyst research in electrochemical nitrogen reduction.

Graphical abstract: Selective electroreduction of dinitrogen to ammonia on a molecular iron phthalocyanine/O-MWCNT catalyst under ambient conditions

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Publication details

The article was received on 24 Aug 2019, accepted on 09 Oct 2019 and first published on 10 Oct 2019


Article type: Communication
DOI: 10.1039/C9CC06574A
Chem. Commun., 2019, Advance Article

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    Selective electroreduction of dinitrogen to ammonia on a molecular iron phthalocyanine/O-MWCNT catalyst under ambient conditions

    F. Xu, L. Zhang, X. Ding, M. Cong, Y. Jin, L. Chen and Y. Gao, Chem. Commun., 2019, Advance Article , DOI: 10.1039/C9CC06574A

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