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Identification of FeN4 as an Efficient Active Site for Electrochemical N2 Reduction
Abstract
Electrocatalytic N 2 reduction to NH 3 is an attractive method for artificial N 2 fixation at ambient conditions. Herein, we demonstrate that Fe-NC materials could be efficient for electrochemical N 2 reduction reaction (NRR) using iron phthalocyanine (FePc) with a well-defined FeN 4 configuration as a model catalyst. By uniformly loading FePc molecules on porous carbon, it exhibits a high electrocatalytic activity for NRR with a NH 3 yield rate of 137.95 μg h –1 mg –1 FePc at a low potential of −0.3 V (vs RHE). Importantly, by making comparisons with phthalocyanine without the Fe center and performing control and poisoning experiments together with theoretical calculations, we identify the Fe center in FeN 4 as the most active site for NRR among five possible sites in FePc and discover that the preferred route is the alternating pathway of N 2 on Fe. These results open up opportunities for further exploring metal-nitrogen-carbon materials for highly efficient electrochemical N 2 fixation and NH 3 production.
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Metadata
- Authors
- He, C., Wu, Z.-Y., Zhao, L., Ming, M., Zhang, Y., Yi, Y., & Hu, J.-S.
- Venue
- ACS Catalysis
- Publisher
- American Chemical Society (ACS)
- Published
- 2019-07-03
- Volume
- 9
- Issue
- 8
- Pages
- 7311-7317
- ISSN
- 2155-5435 (ISSN-L)
- OpenAlex
- W2953421237
- Cited by
- 287
- References
- 45
- FWCI
- 8.65
- Type
- journal article
- Language
- en
- Open access
- closed
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