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Two-dimensional Fe-TPPHZ nanosheets for electrohydrogenation of N2 to NH3 under ambient conditions

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Abstract

The design of high-performance and low-cost catalysts for mild electrocatalytic nitrogen reduction reaction (NRR) is particularly desirable and remains greatly challenging due to the unfavorably low ammonia yield rate and Faradaic efficiency (FE), which comes from the difficulty in making nitrogen activation superior to competitive hydrogen evolution reaction (HER). Herein, we report a well-designed two-dimensional nanosheet-like Fe-tetrapyridophenazine (Fe-TPPHZ) catalyst for ambient NRR process, which was facially prepared by coordinating Fe ions with TPPHZ ligand. The Fe-TPPHZ catalyst shows a remarkable NRR activity at ambient conditions with a high NH3 yield rate of 29.07 µg h−1 mg−1 and an outstanding FE of 11.5% at − 0.3 V vs. RHE. An ammonia yield rate of 21.86 µg h−1 mg−1 is observed after 100 consecutive cycles, with a retention rate of 75.2%. This work will provide a rational design idea to use non-precious metal-based complex as highly effective electrocatalysts for NRR test.

Graphical Abstract

A two-dimensional nanosheet-like Fe-tetrapyridophenazine (Fe-TPPHZ) catalyst was successfully designed and utilized for ambient NRR process, showing a remarkable NRR activity with a high NH3 yield rate of 29.07 μg h−1 mg−1, outstanding FE of 11.5% at − 0.3 V vs. RHE and good retention rate of 75.2% after 100 cycles.

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Acknowledgements

This work was financially supported by the National Natural Science Foundation of China (21773018 and 21975033) and the Analysis and Testing Center, NERC Biomass of Changzhou University.

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Authors and Affiliations

  1. School of Petrochemical Engineering, Jiangsu Key Laboratory of Advanced Catalytic Materials and Technology, Analysis and Testing Center, Changzhou University, 213164, Changzhou, China

    Ying Wang, Hui Luo, Chaoxu Ye, Yanjun Shi, Zhidong Chen, Wenchang Wang, Jianyu Cao & Juan Xu

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Wang, Y., Luo, H., Ye, C. et al. Two-dimensional Fe-TPPHZ nanosheets for electrohydrogenation of N2 to NH3 under ambient conditions. J Appl Electrochem 52, 1295–1304 (2022). https://doi.org/10.1007/s10800-022-01712-y

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