Efficient electrocatalytic urea synthesis from CO2 and nitrate over the scale-up produced FeNi alloy-decorated nanoporous carbon

doi:10.1016/S1872-2067(24)60111-7

Abstract

Abstract:

Electrocatalytic urea synthesis provides a favorable strategy for conventional energy-consuming urea synthesis, but achieving large-scale catalyst synthesis with high catalytic efficiency remains challenging. Herein, we developed a simple method for the preparation of a series of FeNi-alloy-based catalysts, named FeNi@nC-T (n represents the content of nanoporous carbon as 1, 3, 5, 7 or 9 g and T = 900, 950, 1000 or 1100 °C), for highly performed urea synthesis via NO₃^- and CO₂ co-reduction. The FeNi@7C-1000 achieved a high urea yield of 1041.33 mmol h^-1 g_FeNi^-1 with a Faradaic efficiency of 15.56% at -1.2 V vs. RHE. Moreover, the scale-up synthesized FeNi@7C-950-S (over 140 g per batch) was achieved with its high catalytic performance and high stability maintained. Mechanism investigation illuminated that the Ni and Fe sites catalyze and stabilize the key *CO and *N intermediates and minimize the C-N coupling reaction barriers for highly efficient urea synthesis.

Key words: Urea synthesis, Electrocatalysis, FeNi alloy, Scale-up synthesis, C-N coupling

Zuo-Shu Sun, Xue-Yan Xiang, Qiu-Ping Zhao, Zhao Tang, Shi-Yi Jiang, Tong-Bu Lu, Zhi-Ming Zhang, Baifan Wang, Hua-Qing Yin. Efficient electrocatalytic urea synthesis from CO₂ and nitrate over the scale-up produced FeNi alloy-decorated nanoporous carbon[J]. Chinese Journal of Catalysis, 2024, 65: 153-162.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(24)60111-7

https://www.cjcatal.com/EN/Y2024/V65/I10/153

Figures/Tables 4

Fig. 1. (a) HRTEM and (b) enlarged TEM images of FeNi@7C-1000 (inset is a crystal lattice of FeNi@7C-1000). (c) The line scan intensity profile of FeNi@7C-1000. (d) HAADF-STEM images and the corresponding EDX elemental mapping images of FeNi@7C-1000.

Fig. 2. (a) The experimental PXRD patterns of FeNi@nC-1000 (n = 1, 3, 5, 7, 9) and the simulated PXRD signal of FeNi alloy. The high-resolution XPS spectra of Fe 2p (b) and Ni 2p (c) of the FeNi@7C-1000. (d) The nitrogen adsorption-desorption isotherms of the nanoporous carbon before and after FeNi alloy anchoring (inset is the pore size distribution).

Fig. 3. (a) LSV curves of FeNi@7C-1000 in the Ar/KNO3, CO2/KNO3, and CO2/K2SO4 systems. Electrocatalytic performance over FeNi@7C-1000 under different applying potentials (b) and FeNi@nC-1000 under -1.2 V vs. RHE (c). (d) The urea yield over FeNi@7C-1000, FeNi@7C-950 and FeNi@7C-950-S. (e) Recycle experiments and (f) current intensity stability of FeNi@7C-1000.

Fig. 4. DFT calculations. (a) Free-energy diagram for urea production on the FeNi alloy. (b) Corresponding atomic configurations for each step.

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Efficient electrocatalytic urea synthesis from CO₂ and nitrate over the scale-up produced FeNi alloy-decorated nanoporous carbon

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