2022
DOI: 10.1038/s41467-022-33066-6
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Identifying and tailoring C–N coupling site for efficient urea synthesis over diatomic Fe–Ni catalyst

Abstract: Electrocatalytic urea synthesis emerged as the promising alternative of Haber–Bosch process and industrial urea synthetic protocol. Here, we report that a diatomic catalyst with bonded Fe–Ni pairs can significantly improve the efficiency of electrochemical urea synthesis. Compared with isolated diatomic and single-atom catalysts, the bonded Fe–Ni pairs act as the efficient sites for coordinated adsorption and activation of multiple reactants, enhancing the crucial C–N coupling thermodynamically and kinetically… Show more

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Cited by 247 publications
(193 citation statements)
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“…[16][17][18][19][20][21][22][23][24][25][26][27][28] In comparion with N2 reactant, the superiorities of NO3 − and NO2 − as the reactants are high solubility in aqueous solution, lower dissociation energy of N=O bond (204 KJ mol −1 ), which enable more efficient C−N coupling reaction for urea production. [16][17][18][19][20][21][22][23][24][25][26][27][28] Besides of this, development of high-efficiency electrocatalysts is also critically important for urea synthesis. To date, precious and non-precious metals based electrocatalysts have been fabricated and investigated for electrocatalytic coupling of NO3 − and NO2 − (or NO) and CO2 to efficiently synthesize urea at ambient conditions, exhibiting high electrocatalytic activities.…”
Section: Introductionmentioning
confidence: 99%
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“…[16][17][18][19][20][21][22][23][24][25][26][27][28] In comparion with N2 reactant, the superiorities of NO3 − and NO2 − as the reactants are high solubility in aqueous solution, lower dissociation energy of N=O bond (204 KJ mol −1 ), which enable more efficient C−N coupling reaction for urea production. [16][17][18][19][20][21][22][23][24][25][26][27][28] Besides of this, development of high-efficiency electrocatalysts is also critically important for urea synthesis. To date, precious and non-precious metals based electrocatalysts have been fabricated and investigated for electrocatalytic coupling of NO3 − and NO2 − (or NO) and CO2 to efficiently synthesize urea at ambient conditions, exhibiting high electrocatalytic activities.…”
Section: Introductionmentioning
confidence: 99%
“…To date, precious and non-precious metals based electrocatalysts have been fabricated and investigated for electrocatalytic coupling of NO3 − and NO2 − (or NO) and CO2 to efficiently synthesize urea at ambient conditions, exhibiting high electrocatalytic activities. [16][17][18][19][20][21][22][23][24][25][26][27][28][29] In terms to catalytic mechanism research, Zhang et al reported that the formation of *CO and *NH2 intermediates through the adsorption and activation of CO2 and NO on Zn nanobelts catalyst is critically important for subsequent C−N coupling synthesis of urea with a yield rate of 15.13 mmol h −1 g −1 and a faradaic efficiency of 11.26% at ~40 mA cm −2 . 29 Meanwhile, Zhang et al synthesized urea by coupling CO2 with NO2 − on oxygen vacancy-rich ZnO porous nanosheets with a yield rate of 16.56 μmol h −1 and a faradaic efficiency of 23.26% at −0.79 V (vs. RHE).…”
Section: Introductionmentioning
confidence: 99%
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“…The molar ratio of NO to CO 2 is 3:7, which is comparable to those in the reported publications when using NO 3 − /NO 2 − or N 2 as a nitrogen source. 16,22,24,59 Moreover, in situ ATR-FTIR spectra (Figure 4a), online DEMS measurements (Figure 4b), and DFT calculations (Figure 4c,d) reveal the urea generation goes through a ten-step reduction reaction process. The formation of the C−N bond came from the multistep coupling process of *CO and *NH 2 species (Figure 4e).…”
Section: Urea Synthesis From Electrocatalytic C−n Coupling Nomentioning
confidence: 95%