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O. Quinn Carvalho, Rylee Marks, Hoan K. K. Nguyen, Molly E. Vitale-Sullivan, Selena C. Martinez, Líney Árnadóttir, Kelsey A. Stoerzinger
Electrocatalysis is a promising approach to convert waste nitrate to ammonia and help close the nitrogen cycle. This renewably powered ammonia production process sources hydrogen from water (as opposed to methane in the thermal Haber–Bosch process) but requires a delicate balance between a catalyst’s activity for the hydrogen evolution reaction (HER) and the nitrate reduction reaction (NO 3 RR), influencing the Faradaic efficiency (FE) and selectivity to ammonia/ammonium over other nitrogen-containing products. We measure ammonium FEs ranging from 3.6 ± 6.6% (on Ag) to 93.7 ± 0.9% (on Co) across a range of transition metals (TMs; Ti, Fe, Co, Ni, Ni 0.68 Cu 0.32, Cu, and Ag) in buffered neutral media. To better understand these competing reaction kinetics, we develop a microkinetic model that captures the voltage-dependent nitrate rate order and illustrates its origin as competitive adsorption between nitrate and hydrogen adatoms (H*). NO 3 RR FE can be described via competition for electrons with the HER, decreasing sharply for TMs with a high work function and a correspondingly high HER activity (e.g., Ni). Ammonium selectivity nominally increases as the TM d-band center energy ( E d ) approaches and overcomes the Fermi level ( E F ), but is exceptionally high for Co compared to materials with similar E d . Density functional theory (DFT) calculations indicate Co maximizes ammonium selectivity via (1) strong nitrite binding enabling subsequent reduction and (2) promotion of nitric oxide dissociation, leading to selective reduction of the nitrogen adatom (N*) to ammonium.
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Carvalho, O. Q., Marks, R., Nguyen, H. K. K., Vitale-Sullivan, M. E., Martinez, S. C., Árnadóttir, L., & Stoerzinger, K. A. (2022). Role of Electronic Structure on Nitrate Reduction to Ammonium: A Periodic Journey. Journal of the American Chemical Society, 144(32), 14809–14818. https://doi.org/10.1021/jacs.2c05673
Carvalho, O. Quinn, et al. "Role of Electronic Structure on Nitrate Reduction to Ammonium: A Periodic Journey." Journal of the American Chemical Society, vol. 144, no. 32, 2022, pp. 14809–14818, https://doi.org/10.1021/jacs.2c05673.
Carvalho, O. Quinn, Rylee Marks, Hoan K. K. Nguyen, Molly E. Vitale-Sullivan, Selena C. Martinez, Líney Árnadóttir, and Kelsey A. Stoerzinger. "Role of Electronic Structure on Nitrate Reduction to Ammonium: A Periodic Journey." Journal of the American Chemical Society 144, no. 32 (2022): 14809–14818. https://doi.org/10.1021/jacs.2c05673.
Carvalho O. Q., Marks R., Nguyen H. K. K. [и др.] Role of Electronic Structure on Nitrate Reduction to Ammonium: A Periodic Journey // Journal of the American Chemical Society. — 2022. — Vol. 144, № 32. — P. 14809–14818. — URL: https://doi.org/10.1021/jacs.2c05673
@article{carvalho2022role,
title = {{Role of Electronic Structure on Nitrate Reduction to Ammonium: A Periodic Journey}},
author = {O. Quinn Carvalho and Rylee Marks and Hoan K. K. Nguyen and Molly E. Vitale-Sullivan and Selena C. Martinez and Líney Árnadóttir and Kelsey A. Stoerzinger},
journal = {Journal of the American Chemical Society},
year = {2022},
volume = {144},
number = {32},
pages = {14809--14818},
doi = {10.1021/jacs.2c05673},
url = {https://doi.org/10.1021/jacs.2c05673}
}TY - JOUR AU - Carvalho, O. Quinn AU - Marks, Rylee AU - Nguyen, Hoan K. K. AU - Vitale-Sullivan, Molly E. AU - Martinez, Selena C. AU - Árnadóttir, Líney AU - Stoerzinger, Kelsey A. TI - Role of Electronic Structure on Nitrate Reduction to Ammonium: A Periodic Journey JO - Journal of the American Chemical Society VL - 144 IS - 32 SP - 14809 EP - 14818 PY - 2022 DA - 2022/08/04 DO - 10.1021/jacs.2c05673 UR - https://doi.org/10.1021/jacs.2c05673 ER -
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