Electrochemical N2 reduction to ammonia using single Au/Fe atoms supported on nitrogen-doped porous carbon

Sahoo SK, Heske J, Antonietti M, Qin Q, Oschatz M, Kühne TD (2020)

Publication Type: Journal article

Publication year: 2020

Journal

ACS Applied Energy Materials American Chemical Society

Book Volume: 3

Pages Range: 10061-10069

Journal Issue: 10

DOI: 10.1021/acsaem.0c01740

Abstract

The electrochemical nitrogen reduction reaction (NRR) to ammonia (NH3) is a promising alternative route for an NH3 synthesis at ambient conditions to the conventional high temperature and pressure Haber−Bosch process without the need for hydrogen gas. Single metal ions or atoms are attractive candidates for the catalytic activation of non-reactive nitrogen (N2), and for future targeted improvement of NRR catalysts, it is of utmost importance to get detailed insights into structure-performance relationships and mechanisms of N2 activation in such structures. Here, we report density functional theory studies on the NRR catalyzed by single Au and Fe atoms supported in graphitic C2N materials. Our results show that the metal atoms present in the structure of C2N are the reactive sites, which catalyze the aforesaid reaction by strong adsorption and activation of N2. We further demonstrate that a lower onset electrode potential is required for Fe−C2N than for Au−C2N. Thus, Fe−C2N is theoretically predicted to be a potentially better NRR catalyst at ambient conditions than Au−C2N owing to the larger adsorption energy of N2 molecules. Furthermore, we have experimentally shown that single sites of Au and Fe supported on nitrogen-doped porous carbon are indeed active NRR catalysts. However, in contrast to our theoretical results, the Au-based catalyst performed slightly better with a Faradaic efficiency (FE) of 10.1% than the Fe-based catalyst with an FE of 8.4% at −0.2 V vs. RHE. The DFT calculations suggest that this difference is due to the competitive hydrogen evolution reaction and higher desorption energy of ammonia.

Involved external institutions

Universität Paderborn

Germany (DE) Max-Planck-Institut für Kolloid- und Grenzflächenforschung / Max Planck Institute of Colloids and Interfaces

Germany (DE)

How to cite

APA:

Sahoo, S.K., Heske, J., Antonietti, M., Qin, Q., Oschatz, M., & Kühne, T.D. (2020). Electrochemical N2 reduction to ammonia using single Au/Fe atoms supported on nitrogen-doped porous carbon. ACS Applied Energy Materials, 3(10), 10061-10069. https://doi.org/10.1021/acsaem.0c01740

MLA:

Sahoo, Sudhir K., et al. "Electrochemical N2 reduction to ammonia using single Au/Fe atoms supported on nitrogen-doped porous carbon." ACS Applied Energy Materials 3.10 (2020): 10061-10069.

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